WorldWideScience

Sample records for saline aerosol emissions

  1. Attenuation of pancreatitis-induced pulmonary injury by aerosolized hypertonic saline.

    LENUS (Irish Health Repository)

    Shields, C J

    2012-02-03

    BACKGROUND: The immunomodulatory effects of hypertonic saline (HTS) provide potential strategies to attenuate inappropriate inflammatory reactions. This study tested the hypothesis that administration of intratracheal aerosolized HTS modulates the development of lung injury in pancreatitis. METHODS: Pancreatitis was induced in 24 male Sprague-Dawley rats by intraperitoneal injection of 20% L-arginine (500 mg\\/100 g body weight). At 24 and 48 h, intratracheal aerosolized HTS (7.5% NaCl, 0.5 mL) was administered to 8 rats, while a further 8 received 0.5 mL of aerosolized normal saline (NS). At 72 hours, pulmonary neutrophil infiltration (myeloperoxidase activity) and endothelial permeability (bronchoalveolar lavage and wet:dry weight ratios) were assessed. In addition, histological assessment of representative lung tissue was performed by a blinded assessor. In a separate experiment, polymorphonucleocytes (PMN) were isolated from human donors, and exposed to increments of HTS. Neutrophil transmigration across an endothelial cell layer, VEGF release, and apoptosis at 1, 6, 12, 18, and 24 h were assessed. RESULTS: Histopathological lung injury scores were significantly reduced in the HTS group (4.78 +\\/- 1.43 vs. 8.64 +\\/- 0.86); p < 0.001). Pulmonary neutrophil sequestration (1.40 +\\/- 0.2) and increased endothelial permeability (6.77 +\\/- 1.14) were evident in the animals resuscitated with normal saline when compared with HTS (0.70 +\\/- 0.1 and 3.57 +\\/- 1.32), respectively; p < 0.04). HTS significantly reduced PMN transmigration (by 97.1, p = 0.002, and induced PMN apoptosis (p < 0.03). HTS did not impact significantly upon neutrophil VEGF release (p > 0.05). CONCLUSIONS: Intratracheal aerosolized HTS attenuates the neutrophil-mediated pulmonary insult subsequent to pancreatitis. This may represent a novel therapeutic strategy.

  2. Climate Impacts From a Removal of Anthropogenic Aerosol Emissions

    Science.gov (United States)

    Samset, B. H.; Sand, M.; Smith, C. J.; Bauer, S. E.; Forster, P. M.; Fuglestvedt, J. S.; Osprey, S.; Schleussner, C.-F.

    2018-01-01

    Limiting global warming to 1.5 or 2.0°C requires strong mitigation of anthropogenic greenhouse gas (GHG) emissions. Concurrently, emissions of anthropogenic aerosols will decline, due to coemission with GHG, and measures to improve air quality. However, the combined climate effect of GHG and aerosol emissions over the industrial era is poorly constrained. Here we show the climate impacts from removing present-day anthropogenic aerosol emissions and compare them to the impacts from moderate GHG-dominated global warming. Removing aerosols induces a global mean surface heating of 0.5-1.1°C, and precipitation increase of 2.0-4.6%. Extreme weather indices also increase. We find a higher sensitivity of extreme events to aerosol reductions, per degree of surface warming, in particular over the major aerosol emission regions. Under near-term warming, we find that regional climate change will depend strongly on the balance between aerosol and GHG forcing.

  3. Regional aerosol emissions and temperature response: Local and remote climate impacts of regional aerosol forcing

    Science.gov (United States)

    Lewinschal, Anna; Ekman, Annica; Hansson, Hans-Christen

    2017-04-01

    Emissions of anthropogenic aerosols vary substantially over the globe and the short atmospheric residence time of aerosols leads to a highly uneven radiative forcing distribution, both spatially and temporally. Regional aerosol radiative forcing can, nevertheless, exert a large influence on the temperature field away from the forcing region through changes in heat transport or the atmospheric or ocean circulation. Moreover, the global temperature response distribution to aerosol forcing may vary depending on the geographical location of the forcing. In other words, the climate sensitivity in one region can vary depending on the location of the forcing. The surface temperature distribution response to changes in sulphate aerosol forcing caused by sulphur dioxide (SO2) emission perturbations in four different regions is investigated using the Norwegian Earth System Model (NorESM). The four regions, Europe, North America, East and South Asia, are all regions with historically high aerosol emissions and are relevant from both an air-quality and climate policy perspective. All emission perturbations are defined relative to the year 2000 emissions provided for the Coupled Model Intercomparison Project phase 5. The global mean temperature change per unit SO2 emission change is similar for all four regions for similar magnitudes of emissions changes. However, the global temperature change per unit SO2 emission in simulations where regional SO2 emission were removed is substantially higher than that obtained in simulations where regional SO2 emissions were increased. Thus, the climate sensitivity to regional SO2 emissions perturbations depends on the magnitude of the emission perturbation in NorESM. On regional scale, on the other hand, the emission perturbations in different geographical locations lead to different regional temperature responses, both locally and in remote regions. The results from the model simulations are used to construct regional temperature potential

  4. Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

    Energy Technology Data Exchange (ETDEWEB)

    Mills, Michael J. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Schmidt, Anja [School of Earth and Environment, University of Leeds, Leeds UK; Easter, Richard [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Solomon, Susan [Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge Massachusetts USA; Kinnison, Douglas E. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Ghan, Steven J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Neely, Ryan R. [School of Earth and Environment, University of Leeds, Leeds UK; National Centre for Atmospheric Science, University of Leeds, Leeds UK; Marsh, Daniel R. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Conley, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Bardeen, Charles G. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Gettelman, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA

    2016-03-06

    Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptions between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.

  5. Climate and health implications of future aerosol emission scenarios

    Science.gov (United States)

    Partanen, Antti-Ilari; Landry, Jean-Sébastien; Damon Matthews, H.

    2018-02-01

    Anthropogenic aerosols have a net cooling effect on climate and also cause adverse health effects by degrading air quality. In this global-scale sensitivity study, we used a combination of the aerosol-climate model ECHAM-HAMMOZ and the University of Victoria Earth System Climate Model to assess the climate and health effects of aerosols emissions from three Representative Concentration Pathways (RCP2.6, RCP4.5, and RCP8.5) and two new (LOW and HIGH) aerosol emission scenarios derived from RCP4.5, but that span a wider spectrum of possible future aerosol emissions. All simulations had CO2 emissions and greenhouse gas forcings from RCP4.5. Aerosol forcing declined similarly in the standard RCP aerosol emission scenarios: the aerosol effective radiative forcing (ERF) decreased from -1.3 W m-2 in 2005 to between -0.1 W m-2 and -0.4 W m-2 in 2100. The differences in ERF were substantially larger between LOW (-0.02 W m-2 in 2100) and HIGH (-0.8 W m-2) scenarios. The global mean temperature difference between the simulations with standard RCP aerosol emissions was less than 0.18 °C, whereas the difference between LOW and HIGH reached 0.86 °C in 2061. In LOW, the rate of warming peaked at 0.48 °C per decade in the 2030s, whereas in HIGH it was the lowest of all simulations and never exceeded 0.23 °C per decade. Using present-day population density and baseline mortality rates for all scenarios, PM2.5-induced premature mortality was 2 371 800 deaths per year in 2010 and 525 700 in 2100 with RCP4.5 aerosol emissions; in HIGH, the premature mortality reached its maximum value of 2 780 800 deaths per year in 2030, whereas in LOW the premature mortality at 2030 was below 299 900 deaths per year. Our results show potential trade-offs in aerosol mitigation with respect to climate change and public health as ambitious reduction of aerosol emissions considerably increased warming while decreasing mortality.

  6. The role of reduced aerosol precursor emissions in driving near-term warming

    International Nuclear Information System (INIS)

    Gillett, Nathan P; Von Salzen, Knut

    2013-01-01

    The representative concentration pathway (RCP) scenarios all assume stringent emissions controls on aerosols and their precursors, and hence include progressive decreases in aerosol and aerosol precursor emissions through the 21st century. Recent studies have suggested that the resultant decrease in aerosols could drive rapid near-term warming, which could dominate the effects of greenhouse gas (GHG) increases in the coming decades. In CanESM2 simulations, we find that under the RCP 2.6 scenario, which includes the fastest decrease in aerosol and aerosol precursor emissions, the contribution of aerosol reductions to warming between 2000 and 2040 is around 30%. Moreover, the rate of warming in the RCP 2.6 simulations declines gradually from its present-day value as GHG emissions decrease. Thus, while aerosol emission reductions contribute to gradual warming through the 21st century, we find no evidence that aerosol emission reductions drive particularly rapid near-term warming in this scenario. In the near-term, as in the long-term, GHG increases are the dominant driver of warming. (letter)

  7. Effects of aerosol emission pathways on future warming and human health

    Science.gov (United States)

    Partanen, Antti-Ilari; Matthews, Damon

    2016-04-01

    The peak global temperature is largely determined by cumulative emissions of long-lived greenhouse gases. However, anthropogenic emissions include also so-called short-lived climate forcers (SLCFs), which include aerosol particles and methane. Previous studies with simple models indicate that the timing of SLCF emission reductions has only a small effect on the rate of global warming and even less of an effect on global peak temperatures. However, these simple model analyses do not capture the spatial dynamics of aerosol-climate interactions, nor do they consider the additional effects of aerosol emissions on human health. There is therefore merit in assessing how the timing of aerosol emission reductions affects global temperature and premature mortality caused by elevated aerosol concentrations, using more comprehensive climate models. Here, we used an aerosol-climate model ECHAM-HAMMOZ to simulate the direct and indirect radiative forcing resulting from aerosol emissions. We simulated Representative Concentration Pathway (RCP) scenarios, and we also designed idealized low and high aerosol emission pathways based on RCP4.5 scenario (LOW and HIGH, respectively). From these simulations, we calculated the Effective Radiative Forcing (ERF) from aerosol emissions between 1850 and 2100, as well as aerosol concentrations used to estimate the premature mortality caused by particulate pollution. We then use the University of Victoria Earth System Climate Model to simulate the spatial and temporal pattern of climate response to these aerosol-forcing scenarios, in combination with prescribed emissions of both short and long-lived greenhouse gases according to the RCP4.5 scenario. In the RCP scenarios, global mean ERF declined during the 21st century from -1.3 W m-2 to -0.4 W m-2 (RCP8.5) and -0.2 W m-2 (RCP2.6). In the sensitivity scenarios, the forcing at the end of the 21st century was -1.6 W m-2 (HIGH) and practically zero (LOW). The difference in global mean temperature

  8. Significance of Future Biogenic and Fire Emissions on Regional Aerosol Burden

    Science.gov (United States)

    Lim, A.; Tai, A. P. K.; Val Martin, M.

    2017-12-01

    Land-use and land cover changes have been found to substantially affect atmospheric aerosols and climate worldwide1,2, but the complex mechanisms and pathways involved in the interactions between terrestrial processes and aerosols are not well understood. Here we use a global coupled aerosol chemistry-climate-land model (CESM with CAM5 using Modal Aerosol Module 3 and CLM4.5 in Satellite Phenology mode) to investigate how aerosols respond to future climate and land-use changes, and in turn, affects cloud cover and other hydrometeorological variables in the long term. Time-sliced simulations are conducted for a base year (2000) as a base case; then three future projected scenarios for year 2050 driven by land-use and climate projections following the Representative Concentration Pathways RCP8.53 are conducted. The first scenario considers future projected biogenic emissions, allowing us to investigate the effect of increased plant activity and enhanced biogenic emissions due to future land-use and climate on aerosol burden. The second scenario considers future biomass burning emissions, allowing us to investigate the effect of increased biomass burning emissions due to future land-use and climate on aerosol burden. The third scenario combines the projected changes in the two emissions. We find that both biogenic and biomass burning emissions contribute significantly to local aerosol and cloud condensation nuclei (CCN) concentrations. The contribution from biogenic emissions to local aerosol burden is smaller in magnitude (10% to 20%), but the effects are ubiquitous in many places globally. Meanwhile, the contribution from biomass burning emissions can be much higher in magnitude (63%)4, but concentrated in heavily burned regions and occurs only during burning season. Effects of both emissions are not additive since a larger flux of emissions causes greater deposition. The resulting further impacts of land-use change on regional hydrometeorology are also explored

  9. A simple parameterization of aerosol emissions in RAMS

    Science.gov (United States)

    Letcher, Theodore

    Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical

  10. An Investigation of the Radiative Effects and Climate Feedbacks of Sea Ice Sources of Sea Salt Aerosol

    Science.gov (United States)

    Horowitz, H. M.; Alexander, B.; Bitz, C. M.; Jaegle, L.; Burrows, S. M.

    2017-12-01

    In polar regions, sea ice is a major source of sea salt aerosol through lofting of saline frost flowers or blowing saline snow from the sea ice surface. Under continued climate warming, an ice-free Arctic in summer with only first-year, more saline sea ice in winter is likely. Previous work has focused on climate impacts in summer from increasing open ocean sea salt aerosol emissions following complete sea ice loss in the Arctic, with conflicting results suggesting no net radiative effect or a negative climate feedback resulting from a strong first aerosol indirect effect. However, the radiative forcing from changes to the sea ice sources of sea salt aerosol in a future, warmer climate has not previously been explored. Understanding how sea ice loss affects the Arctic climate system requires investigating both open-ocean and sea ice sources of sea-salt aerosol and their potential interactions. Here, we implement a blowing snow source of sea salt aerosol into the Community Earth System Model (CESM) dynamically coupled to the latest version of the Los Alamos sea ice model (CICE5). Snow salinity is a key parameter affecting blowing snow sea salt emissions and previous work has assumed constant regional snow salinity over sea ice. We develop a parameterization for dynamic snow salinity in the sea ice model and examine how its spatial and temporal variability impacts the production of sea salt from blowing snow. We evaluate and constrain the snow salinity parameterization using available observations. Present-day coupled CESM-CICE5 simulations of sea salt aerosol concentrations including sea ice sources are evaluated against in situ and satellite (CALIOP) observations in polar regions. We then quantify the present-day radiative forcing from the addition of blowing snow sea salt aerosol with respect to aerosol-radiation and aerosol-cloud interactions. The relative contributions of sea ice vs. open ocean sources of sea salt aerosol to radiative forcing in polar regions is

  11. Dissecting Future Aerosol Emissions. Warming Tendencies and Mitigation Opportunities

    Energy Technology Data Exchange (ETDEWEB)

    Streets, D.G. [Decision and Information Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL, 60439 (United States)

    2007-04-15

    Future global emissions of aerosols will play an important role in governing the nature and magnitude of future anthropogenic climate change. We present in this paper a number of future scenarios of emissions of black carbon (BC) and organic carbon (OC) by world region, which we combine with sulfate (SO4) assessed in terms of the emissions of its precursor, SO2. We find that aerosol emissions from the household and industrial sectors are likely to decline along almost all future pathways. Transportation emissions, however, are subject to complex interacting forces that can lead to either increases or decreases. Biomass burning declines in many scenarios, but the Amazon rainforests remain vulnerable if unsustainable economic growth persists. East Asia is the key region for primary aerosols, and trends in China will have a major bearing on the direction and magnitude of releases of BC (expected reductions in the range of 640-1290 Gg), OC (reductions of 520-1900 Gg), and SO2 (ranging from an increase of 21 Tg to a reduction of 30 Tg). Analysis of joint BC, OC, and SO2 emission changes identifies a number of key world regions and economic sectors that could be effectively targeted for aerosol reductions.

  12. Aerosol emission during human speech

    Science.gov (United States)

    Asadi, Sima; Wexler, Anthony S.; Cappa, Christopher D.; Bouvier, Nicole M.; Barreda-Castanon, Santiago; Ristenpart, William D.

    2017-11-01

    We show that the rate of aerosol particle emission during healthy human speech is strongly correlated with the loudness (amplitude) of vocalization. Emission rates range from approximately 1 to 50 particles per second for quiet to loud amplitudes, regardless of language spoken (English, Spanish, Mandarin, or Arabic). Intriguingly, a small fraction of individuals behave as ``super emitters,'' consistently emitting an order of magnitude more aerosol particles than their peers. We interpret the results in terms of the eggressive flowrate during vocalization, which is known to vary significantly for different types of vocalization and for different individuals. The results suggest that individual speech patterns could affect the probability of airborne disease transmission. The results also provide a possible explanation for the existence of ``super spreaders'' who transmit pathogens much more readily than average and who play a key role in the spread of epidemics.

  13. Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion

    Science.gov (United States)

    Haslett, Sophie; Thomas, J. Chris; Morgan, William; Hadden, Rory; Liu, Dantong; Allan, James; Williams, Paul; Sekou, Keïta; Liousse, Catherine; Coe, Hugh

    2017-04-01

    Particulate emissions from biomass burning can alter the atmosphere's radiative balance and cause significant harm to human health. However, the relationship between these emissions and fundamental combustion processes is, to date, poorly characterised. In atmospheric models, aerosol emissions are represented by emission factors based on mass loss, which are averaged over an entire combustion event for each particulate species. This approach, however, masks huge variability in emissions during different phases of the combustion period. Laboratory tests have shown that even small changes to the burning environment can lead to huge variation in observed aerosol emission factors (Akagi et al., 2011). In order to address this gap in understanding, in this study, small wood samples sourced from Côte D'Ivoire were burned in a highly-controlled laboratory environment. The shape and mass of samples, available airflow and surrounding heat were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real-time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. Both of these instruments are used regularly to measure aerosol concentrations in the field. This methodology produced remarkably repeatable results, allowing three different phases of combustion to be identified by their emissions. Black carbon was emitted predominantly during flaming combustion; organic aerosols were emitted during pyrolysis before ignition and from smouldering-dominated behaviour near the end of combustion. During the flaming period, there was a strong correlation between the emission of black carbon and the rate of mass loss, which suggests there is value in employing a mass-based emission factor for this species. However, very little correlation was seen between organic aerosol and mass loss throughout the tests. As such, results here suggest that emission factors averaged over an entire combustion event are unlikely to be

  14. Radiative effects of interannually varying vs. interannually invariant aerosol emissions from fires

    Directory of Open Access Journals (Sweden)

    B. S. Grandey

    2016-11-01

    Full Text Available Open-burning fires play an important role in the earth's climate system. In addition to contributing a substantial fraction of global emissions of carbon dioxide, they are a major source of atmospheric aerosols containing organic carbon, black carbon, and sulfate. These “fire aerosols” can influence the climate via direct and indirect radiative effects. In this study, we investigate these radiative effects and the hydrological fast response using the Community Atmosphere Model version 5 (CAM5. Emissions of fire aerosols exert a global mean net radiative effect of −1.0 W m−2, dominated by the cloud shortwave response to organic carbon aerosol. The net radiative effect is particularly strong over boreal regions. Conventionally, many climate modelling studies have used an interannually invariant monthly climatology of emissions of fire aerosols. However, by comparing simulations using interannually varying emissions vs. interannually invariant emissions, we find that ignoring the interannual variability of the emissions can lead to systematic overestimation of the strength of the net radiative effect of the fire aerosols. Globally, the overestimation is +23 % (−0.2 W m−2. Regionally, the overestimation can be substantially larger. For example, over Australia and New Zealand the overestimation is +58 % (−1.2 W m−2, while over Boreal Asia the overestimation is +43 % (−1.9 W m−2. The systematic overestimation of the net radiative effect of the fire aerosols is likely due to the non-linear influence of aerosols on clouds. However, ignoring interannual variability in the emissions does not appear to significantly impact the hydrological fast response. In order to improve understanding of the climate system, we need to take into account the interannual variability of aerosol emissions.

  15. The impact of aerosol emissions on the 1.5 °C pathways

    Science.gov (United States)

    Hienola, Anca; Partanen, Antti-Ilari; Pietikäinen, Joni-Pekka; O’Donnell, Declan; Korhonen, Hannele; Damon Matthews, H.; Laaksonen, Ari

    2018-04-01

    To assess the impact of anthropogenic aerosol emission reduction on limiting global temperature increase to 1.5 °C or 2 °C above pre-industrial levels, two climate modeling approaches have been used (MAGICC6, and a combination of ECHAM-HAMMOZ and the UVic ESCM), with two aerosol control pathways under two greenhouse gas (GHG) reduction scenarios. We found that aerosol emission reductions associated with CO2 co-emissions had a significant warming effect during the first half of the century and that the near-term warming is dependent on the pace of aerosol emission reduction. The modeling results show that these aerosol emission reductions account for about 0.5 °C warming relative to 2015, on top of the 1 °C above pre-industrial levels that were already reached in 2015. We found also that the decreases in aerosol emissions lead to different decreases in the magnitude of the aerosol radiative forcing in the two models. By 2100, the aerosol forcing is projected by ECHAM–UVic to diminish in magnitude by 0.96 W m‑2 and by MAGICC6 by 0.76 W m‑2 relative to 2000. Despite this discrepancy, the climate responses in terms of temperature are similar. Aggressive aerosol control due to air quality legislation affects the peak temperature, which is 0.2 °C–0.3 °C above the 1.5 °C limit even within the most ambitious CO2/GHG reduction scenario. At the end of the century, the temperature differences between aerosol reduction scenarios in the context of ambitious CO2 mitigation are negligible.

  16. Regional deposition of saline aerosols of different tonicities in normal and asthmatic subjects

    International Nuclear Information System (INIS)

    Phipps, P.R.; Gonda, I.; Anderson, S.D.; Bailey, D.; Bautovich, G.

    1994-01-01

    Nonisotonic aerosols are frequently used in the diagnosis and therapy of lung disease. The purpose of this work was to study the difference in the pattern of deposition of aerosols containing aqueous solutions of different tonicities. 99m Technetium-diethyltriaminepentaacetic acid ( 99m Tc-DTPA)-labelled saline aerosols, with mass median aerodynamic diameter 3.7-3.8 μm and geometric standard deviation 1.4, were inhaled under reproducible breathing conditions on two occasions. Hypotonic and hypertonic solutions were used in 11 normals subjects, isotonic and hypertonic solutions in 9 asthmatics. The regional deposition was quantified by a penetration index measured with the help of a tomographic technique. There was a small but significant increase (6.7%) in the penetration index of the hypotonic as compared to the hypertonic aerosols in the normal subjects. The region that was markedly affected was the trachea. The differences in the penetration of the isotonic and hypertonic aerosols in the asthmatics appeared to be strongly dependent on the state of the airways at the time of the study. These findings can be interpreted in terms of effects of growth or shrinkage of nonisotonic aerosols, as well as of airway narrowing, on regional deposition of aerosols. Tonicity of aerosols appears to affect their deposition both through physical and physiological mechanisms. This should be taken into account when interpreting the effects of inhaled aqueous solutions of various tonicities in patients in vivo. (au) (44 refs.)

  17. The Influence of Emission Location on the Magnitude and Spatial Distribution of Aerosols' Climate Effects

    Science.gov (United States)

    Persad, G.; Caldeira, K.

    2017-12-01

    The global distribution of anthropogenic aerosol emissions has evolved continuously since the preindustrial era - from 20th century North American and Western European emissions hotspots to present-day South and East Asian ones. With this comes a relocation of the regional radiative, dynamical, and hydrological impacts of aerosol emissions, which may influence global climate differently depending on where they occur. A lack of understanding of this relationship between aerosol emissions' location and their global climate effects, however, obscures the potential influence that aerosols' evolving geographic distribution may have on global and regional climate change—a gap which we address in this work. Using a novel suite of experiments in the CESM CAM5 atmospheric general circulation model coupled to a slab ocean, we systematically test and analyze mechanisms behind the relative climate impact of identical black carbon and sulfate aerosol emissions located in each of 8 past, present, or projected future major emissions regions. Results indicate that historically high emissions regions, such as North America and Western Europe, produce a stronger cooling effect than current and projected future high emissions regions. Aerosol emissions located in Western Europe produce 3 times the global mean cooling (-0.34 °C) as those located in East Africa or India (-0.11 °C). The aerosols' in-situ radiative effects remain relatively confined near the emissions region, but large distal cooling results from remote feedback processes - such as ice albedo and cloud changes - that are excited more strongly by emissions from certain regions than others. Results suggest that aerosol emissions from different countries should not be considered equal in the context of climate mitigation accounting, and that the evolving geographic distribution of aerosol emissions may have a substantial impact on the magnitude and spatial distribution of global climate change.

  18. Influence of gypsum amendment on methane emission from paddy rice soil affected by saline irrigation water

    Directory of Open Access Journals (Sweden)

    Ei Ei eTheint

    2016-01-01

    Full Text Available To investigate the influence of gypsum application on methane (CH4 emission from paddy rice soil affected by saline irrigation water, two pot experiments with the rice cultivation were conducted. In pot experiment (I, salinity levels 30 mMNaCl (S30 and 90 mMNaCl (S90, that showed maximum and minimum CH4 production in an incubation experiment, respectively, were selected and studied without and with application of 1 Mg gypsum ha-1(G1. In pot experiment (II, CH4 emission was investigated under different rates of gypsum application: 1 (G1, 2.5 (G2.5 and 5 (G5 Mg gypsum ha-1 under a non-saline and saline condition of 25 mMNaCl (S25. In experiment (I, the smallest CH4 emission was observed in S90. Methane emission in S30 was not significantly different with the non-saline control. The addition of gypsum showed significant lower CH4 emission in saline and non-saline treatments compared with non-saline control. In experiment (II, the CH4 emissions in the saline treatments were not significantly different to the non-saline treatments except S25-G5. However, our work has shown that gypsum can lower CH4 emissions under saline and non-saline conditions. Thus, gypsum can be used as a CH4 mitigation option in non-saline as well as in saline conditions.

  19. Smoke aerosol chemistry and aging of Siberian biomass burning emissions in a large aerosol chamber

    Science.gov (United States)

    Kalogridis, A.-C.; Popovicheva, O. B.; Engling, G.; Diapouli, E.; Kawamura, K.; Tachibana, E.; Ono, K.; Kozlov, V. S.; Eleftheriadis, K.

    2018-07-01

    Vegetation open fires constitute a significant source of particulate pollutants on a global scale and play an important role in both atmospheric chemistry and climate change. To better understand the emission and aging characteristics of smoke aerosols, we performed small-scale fire experiments using the Large Aerosol Chamber (LAC, 1800 m3) with a focus on biomass burning from Siberian boreal coniferous forests. A series of burn experiments were conducted with typical Siberian biomass (pine and debris), simulating separately different combustion conditions, namely, flaming, smoldering and mixed phase. Following smoke emission and dispersion in the combustion chamber, we investigated aging of aerosols under dark conditions. Here, we present experimental data on emission factors of total, elemental and organic carbon, as well as individual organic compounds, such as anhydrosugars, phenolic and dicarboxylic acids. We found that total carbon accounts for up to 80% of the fine mode (PM2.5) smoke aerosol. Higher PM2.5 emission factors were observed in the smoldering compared to flaming phase and in pine compared to debris smoldering phase. For low-temperature combustion, organic carbon (OC) contributed to more than 90% of total carbon, whereas elemental carbon (EC) dominated the aerosol composition in flaming burns with a 60-70% contribution to the total carbon mass. For all smoldering burns, levoglucosan (LG), a cellulose decomposition product, was the most abundant organic species (average LG/OC = 0.26 for pine smoldering), followed by its isomer mannosan or dehydroabietic acid (DA), an important constituent of conifer resin (DA/OC = 0.033). A levoglucosan-to-mannosan ratio of about 3 was observed, which is consistent with ratios reported for coniferous biomass and more generally softwood. The rates of aerosol removal for OC and individual organic compounds were investigated during aging in the chamber in terms of mass concentration loss rates over time under dark

  20. Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

    Science.gov (United States)

    Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

    2014-10-07

    Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

  1. Physico-Chemical Evolution of Organic Aerosol from Wildfire Emissions

    Science.gov (United States)

    Croteau, P.; Jathar, S.; Akherati, A.; Galang, A.; Tarun, S.; Onasch, T. B.; Lewane, L.; Herndon, S. C.; Roscioli, J. R.; Yacovitch, T. I.; Fortner, E.; Xu, W.; Daube, C.; Knighton, W. B.; Werden, B.; Wood, E.

    2017-12-01

    Wildfires are the largest combustion-related source of carbonaceous emissions to the atmosphere; these include direct emissions of black carbon (BC), primary organic aerosol (POA) and semi-volatile, intermediate-volatility, and volatile organic compounds (SVOCs, IVOCs, and VOCs). However, there are large uncertainties surrounding the evolution of these carbonaceous emissions as they are physically and chemically transformed in the atmosphere. To understand these transformations, we performed sixteen experiments using an environmental chamber to simulate day- and night-time chemistry of gas- and aerosol-phase emissions from 6 different fuels at the Fire Laboratory in Missoula, MT. Across the test matrix, the experiments simulated 2 to 8 hours of equivalent day-time aging (with the hydroxyl radical and ozone) or several hours of night-time aging (with the nitrate radical). Aging resulted in an average organic aerosol (OA) mass enhancement of 28% although the full range of OA mass enhancements varied between -10% and 254%. These enhancement findings were consistent with chamber and flow reactor experiments performed at the Fire Laboratory in 2010 and 2012 but, similar to previous studies, offered no evidence to link the OA mass enhancement to fuel type or oxidant exposure. Experiments simulating night-time aging resulted in an average OA mass enhancement of 10% and subsequent day-time aging resulted in a decrease in OA mass of 8%. While small, for the first time, these experiments highlighted the continuous nature of the OA evolution as the wildfire smoke cycled through night- and day-time processes. Ongoing work is focussed on (i) quantifying bulk compositional changes in OA, (ii) comparing the near-field aging simulated in this work with far-field aging simulated during the same campaign (via a mini chamber and flow tube) and (iii) integrating wildfire smoke aging datasets over the past decade to examine the relationship between OA mass enhancement ratios, modified

  2. Transient Climate Impacts for Scenarios of Aerosol Emissions from Asia: A Story of Coal versus Gas

    Science.gov (United States)

    Grandey, B. S.; Cheng, H.; Wang, C.

    2014-12-01

    Projections of anthropogenic aerosol emissions are uncertain. In Asia, it is possible that emissions may increase if business continues as usual, with economic growth driving an increase in coal burning. But it is also possible that emissions may decrease rapidly due to the widespread adoption of cleaner technology or a shift towards non-coal fuels, such as natural gas. In this study, the transient climate impacts of three aerosol emissions scenarios are investigated: an RCP4.5 (Representative Concentration Pathway 4.5) control; a scenario with reduced Asian anthropogenic aerosol emissions; and a scenario with enhanced Asian anthropogenic aerosol emissions. A coupled atmosphere-ocean configuration of CESM (Community Earth System Model), including CAM5 (Community Atmosphere Model version 5), is used. Enhanced Asian aerosol emissions are found to delay global mean warming by one decade at the end of the century. Aerosol-induced suppression of the East Asian and South Asian summer monsoon precipitation occurs. The enhanced Asian aerosol emissions also remotely impact precipitation in other parts of the world: over the Sahel, West African monsoon precipitation is suppressed; and over Australia, austral summer monsoon precipitation is enhanced. These remote impacts on precipitation are associated with a southward shift of the ITCZ. The aerosol-induced sea surface temperature (SST) response appears to play an important role in the precipitation changes over South Asia and Australia, but not over East Asia. These results indicate that energy production in Asia, through the consequent aerosol emissions and associated radiative effects, might significantly influence future climate both locally and globally.

  3. Characterization of selenium in ambient aerosols and primary emission sources.

    Science.gov (United States)

    De Santiago, Arlette; Longo, Amelia F; Ingall, Ellery D; Diaz, Julia M; King, Laura E; Lai, Barry; Weber, Rodney J; Russell, Armistead G; Oakes, Michelle

    2014-08-19

    Atmospheric selenium (Se) in aerosols was investigated using X-ray absorption near-edge structure (XANES) spectroscopy and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the oxidation state and elemental associations of Se in common primary emission sources and ambient aerosols collected from the greater Atlanta area. In the majority of ambient aerosol and primary emission source samples, the spectroscopic patterns as well as the absence of elemental correlations suggest Se is in an elemental, organic, or oxide form. XRF microscopy revealed numerous Se-rich particles, or hotspots, accounting on average for ∼16% of the total Se in ambient aerosols. Hotspots contained primarily Se(0)/Se(-II). However, larger, bulk spectroscopic characterizations revealed Se(IV) as the dominant oxidation state in ambient aerosol, followed by Se(0)/Se(-II) and Se(VI). Se(IV) was the only observed oxidation state in gasoline, diesel, and coal fly ash, while biomass burning contained a combination of Se(0)/Se(-II) and Se(IV). Although the majority of Se in aerosols was in the most toxic form, the Se concentration is well below the California Environmental Protection Agency chronic exposure limit (∼20000 ng/m(3)).

  4. Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source

    Science.gov (United States)

    Haslett, Sophie L.; Thomas, J. Chris; Morgan, William T.; Hadden, Rory; Liu, Dantong; Allan, James D.; Williams, Paul I.; Keita, Sekou; Liousse, Cathy; Coe, Hugh

    2018-01-01

    Particulate emissions from biomass burning can both alter the atmosphere's radiative balance and cause significant harm to human health. However, due to the large effect on emissions caused by even small alterations to the way in which a fuel burns, it is difficult to study particulate production of biomass combustion mechanistically and in a repeatable manner. In order to address this gap, in this study, small wood samples sourced from Côte D'Ivoire in West Africa were burned in a highly controlled laboratory environment. The shape and mass of samples, available airflow and surrounding thermal environment were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. This methodology produced remarkably repeatable results, allowing aerosol emissions to be mapped directly onto different phases of combustion. Emissions from pyrolysis were visible as a distinct phase before flaming was established. After flaming combustion was initiated, a black-carbon-dominant flame was observed during which very little organic aerosol was produced, followed by a period that was dominated by organic-carbon-producing smouldering combustion, despite the presence of residual flaming. During pyrolysis and smouldering, the two phases producing organic aerosol, distinct mass spectral signatures that correspond to previously reported variations in biofuel emissions measured in the atmosphere are found. Organic aerosol emission factors averaged over an entire combustion event were found to be representative of the time spent in the pyrolysis and smouldering phases, rather than reflecting a coupling between emissions and the mass loss of the sample. Further exploration of aerosol yields from similarly carefully controlled fires and a careful comparison with data from macroscopic fires and real-world emissions will help to deliver greater constraints on the

  5. Aerosol exposure versus aerosol cooling of climate: what is the optimal emission reduction strategy for human health?

    Directory of Open Access Journals (Sweden)

    J. Löndahl

    2010-10-01

    Full Text Available Particles, climate change, and health have thought-provoking interactions. Air pollution is one of the largest environmental problems concerning human health. On the other hand, aerosol particles can have a cooling effect on climate and a reduction of those emissions may result in an increased temperature globally, which in turn may have negative health effects. The objective of this work was to investigate the "total health effects" of aerosol emissions, which include both exposure to particles and consequences for climate change initiated by particles. As a case study the "total health effect" from ship emissions was derived by subtracting the number of deaths caused by exposure with the estimated number of lives saved from the cooling effect of the emissions. The analysis showed that, with current level of scientific understanding, it could not be determined whether ship emissions are negative or positive for human health on a short time scale. This first attempt to approximate the combined effect of particle emissions on health shows that reductions of particulate air pollution will in some cases (black carbon have win-win effects on health and climate, but sometimes also cause a shift from particle exposure-related health effects towards an increasing risk of health consequences from climate change. Thus, measures to reduce aerosol emissions have to be coupled with climate change mitigation actions to achieve a full health benefit on a global level.

  6. Atmospheric Aerosol Emissions Related to the Mediterranean Seawater Biogeochemistry

    Science.gov (United States)

    Sellegri, K.; Schwier, A.; Rose, C.; Gazeau, F. P. H.; Guieu, C.; D'anna, B.; Ebling, A. M.; Pey, J.; Marchand, N.; Charriere, B.; Sempéré, R.; Mas, S.

    2016-02-01

    Marine aerosols contribute significantly to the global aerosol load and consequently has an important impact on the Earth's climate. Different factors influence the way they are produced at the air/seawater interface. The sea state (whitecap coverage, temperature, etc. ) influence the size and concentration of primarily produced particles but also biogeochemical characteristics of the seawater influence both the physical and chemical primary fluxes to the atmosphere. An additional aerosol source of marine aerosol to the atmosphere is the formation of new particles by gaz-to-particle conversion, i.e. nucleation. How the seawater and surface microlayer biogeochemical compositions influences the aerosol emissions is still a large debate. In order to study marine emissions, one approach is to use semi-controlled environments such as mesocosms. Within the MedSea and SAM projects, we characterize the primary Sea Spray Aerosol (SSA) during mesocosms experiments performed during different seasons in the Mediteranean Sea. Mesocosms were either left unchanged as control or enriched by addition of nutriments in order to create different levels of phytoplanctonic activities. The mesocosms waters were daily analyzed for their chemical and biological composition (DOC, CDOM, TEP, Chl-a, virus, bacteria, phytoplankton and zooplankton concentrations). SSA production by bubble bursting was daily simulated in a dedicated set-up. The size segregated SSA number fluxes, cloud condensation nuclei (CCN) properties, and chemical composition were determined as a function of the seawater characteristics. We show that the SSA organic content was clearly correlated to the seawater Chl-a level, provided that the mesocosm was not enriched to create an artificial phytoplanctonic bloom. In our experiments, the enrichment of the seawater with natural surface microlayer did not impact the SSA organic content nor its CCN properties. At last, nucleation of secondary particles were observed to occur in

  7. Gas phase emissions from cooking processes and their secondary aerosol production potential

    Science.gov (United States)

    Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

    2014-05-01

    Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR

  8. Global radiative effects of solid fuel cookstove aerosol emissions

    Science.gov (United States)

    Huang, Yaoxian; Unger, Nadine; Storelvmo, Trude; Harper, Kandice; Zheng, Yiqi; Heyes, Chris

    2018-04-01

    We apply the NCAR CAM5-Chem global aerosol-climate model to quantify the net global radiative effects of black and organic carbon aerosols from global and Indian solid fuel cookstove emissions for the year 2010. Our assessment accounts for the direct radiative effects, changes to cloud albedo and lifetime (aerosol indirect effect, AIE), impacts on clouds via the vertical temperature profile (semi-direct effect, SDE) and changes in the surface albedo of snow and ice (surface albedo effect). In addition, we provide the first estimate of household solid fuel black carbon emission effects on ice clouds. Anthropogenic emissions are from the IIASA GAINS ECLIPSE V5a inventory. A global dataset of black carbon (BC) and organic aerosol (OA) measurements from surface sites and aerosol optical depth (AOD) from AERONET is used to evaluate the model skill. Compared with observations, the model successfully reproduces the spatial patterns of atmospheric BC and OA concentrations, and agrees with measurements to within a factor of 2. Globally, the simulated AOD agrees well with observations, with a normalized mean bias close to zero. However, the model tends to underestimate AOD over India and China by ˜ 19 ± 4 % but overestimate it over Africa by ˜ 25 ± 11 % (± represents modeled temporal standard deviations for n = 5 run years). Without BC serving as ice nuclei (IN), global and Indian solid fuel cookstove aerosol emissions have net global cooling radiative effects of -141 ± 4 mW m-2 and -12 ± 4 mW m-2, respectively (± represents modeled temporal standard deviations for n = 5 run years). The net radiative impacts are dominated by the AIE and SDE mechanisms, which originate from enhanced cloud condensation nuclei concentrations for the formation of liquid and mixed-phase clouds, and a suppression of convective transport of water vapor from the lower troposphere to the upper troposphere/lower stratosphere that in turn leads to reduced ice cloud formation. When BC is allowed

  9. The impact of residential combustion emissions on atmospheric aerosol, human health, and climate

    Directory of Open Access Journals (Sweden)

    E. W. Butt

    2016-01-01

    Full Text Available Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC and organic carbon (OC mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5 concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (>  30 years of age premature mortality (due to both cardiopulmonary disease and lung cancer to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range for monthly varying residential emissions and 517 000 (192 000–827 000 when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the

  10. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    International Nuclear Information System (INIS)

    Lacey, Forrest; Henze, Daven

    2015-01-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  11. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    Science.gov (United States)

    Lacey, Forrest; Henze, Daven

    2015-11-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  12. Aerosol Emissions from Fuse-Deposition Modeling 3D Printers in a Chamber and in Real Indoor Environments.

    Science.gov (United States)

    Vance, Marina E; Pegues, Valerie; Van Montfrans, Schuyler; Leng, Weinan; Marr, Linsey C

    2017-09-05

    Three-dimensional (3D) printers are known to emit aerosols, but questions remain about their composition and the fundamental processes driving emissions. The objective of this work was to characterize the aerosol emissions from the operation of a fuse-deposition modeling 3D printer. We modeled the time- and size-resolved emissions of submicrometer aerosols from the printer in a chamber study, gained insight into the chemical composition of emitted aerosols using Raman spectroscopy, and measured the potential for exposure to the aerosols generated by 3D printers under real-use conditions in a variety of indoor environments. The average aerosol emission rates ranged from ∼10 8 to ∼10 11 particles min -1 , and the rates varied over the course of a print job. Acrylonitrile butadiene styrene (ABS) filaments generated the largest number of aerosols, and wood-infused polylactic acid (PLA) filaments generated the smallest amount. The emission factors ranged from 6 × 10 8 to 6 × 10 11 per gram of printed part, depending on the type of filament used. For ABS, the Raman spectra of the filament and the printed part were indistinguishable, while the aerosol spectra lacked important peaks corresponding to styrene and acrylonitrile, which are both present in ABS. This observation suggests that aerosols are not a result of volatilization and subsequent nucleation of ABS or direct release of ABS aerosols.

  13. A new oxidation flow reactor for measuring secondary aerosol formation of rapidly changing emission sources

    Science.gov (United States)

    Simonen, Pauli; Saukko, Erkka; Karjalainen, Panu; Timonen, Hilkka; Bloss, Matthew; Aakko-Saksa, Päivi; Rönkkö, Topi; Keskinen, Jorma; Dal Maso, Miikka

    2017-04-01

    Oxidation flow reactors (OFRs) or environmental chambers can be used to estimate secondary aerosol formation potential of different emission sources. Emissions from anthropogenic sources, such as vehicles, often vary on short timescales. For example, to identify the vehicle driving conditions that lead to high potential secondary aerosol emissions, rapid oxidation of exhaust is needed. However, the residence times in environmental chambers and in most oxidation flow reactors are too long to study these transient effects ( ˜ 100 s in flow reactors and several hours in environmental chambers). Here, we present a new oxidation flow reactor, TSAR (TUT Secondary Aerosol Reactor), which has a short residence time ( ˜ 40 s) and near-laminar flow conditions. These improvements are achieved by reducing the reactor radius and volume. This allows studying, for example, the effect of vehicle driving conditions on the secondary aerosol formation potential of the exhaust. We show that the flow pattern in TSAR is nearly laminar and particle losses are negligible. The secondary organic aerosol (SOA) produced in TSAR has a similar mass spectrum to the SOA produced in the state-of-the-art reactor, PAM (potential aerosol mass). Both reactors produce the same amount of mass, but TSAR has a higher time resolution. We also show that TSAR is capable of measuring the secondary aerosol formation potential of a vehicle during a transient driving cycle and that the fast response of TSAR reveals how different driving conditions affect the amount of formed secondary aerosol. Thus, TSAR can be used to study rapidly changing emission sources, especially the vehicular emissions during transient driving.

  14. Characterization of fresh and aged organic aerosol emissions from meat charbroiling

    Directory of Open Access Journals (Sweden)

    C. Kaltsonoudis

    2017-06-01

    Full Text Available Cooking emissions can be a significant source of fine particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. Greek souvlakia with pork were cooked using a commercial charbroiler and a fraction of the emissions were introduced into a smog chamber where after a characterization phase they were exposed to UV illumination and oxidants. The particulate and gas phases were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS and a proton-transfer-reaction mass spectrometer (PTR-MS correspondingly. More than 99 % of the aerosol emitted was composed of organic compounds, while black carbon (BC contributed 0.3 % and the inorganic species less than 0.5 % of the total aerosol mass. The initial O  :  C ratio was approximately 0.09 and increased up to 0.30 after a few hours of chemical aging (exposures of 1010 molecules cm−3 s for OH and 100 ppb h for ozone. The initial and aged AMS spectra differed considerably (θ =  27°. Ambient measurements were also conducted during Fat Thursday in Patras, Greece, when traditionally meat is charbroiled everywhere in the city. Positive matrix factorization (PMF revealed that cooking organic aerosol (COA reached up to 85 % of the total OA from 10:00 to 12:00 LST that day. The ambient COA factor in two major Greek cities had a mass spectrum during spring and summer similar to the aged meat charbroiling emissions. In contrast, the ambient COA factor during winter resembled strongly the fresh laboratory meat charbroiling emissions.

  15. Modeling regional aerosol and aerosol precursor variability over California and its sensitivity to emissions and long-range transport during the 2010 CalNex and CARES campaigns

    Science.gov (United States)

    Fast, J. D.; Allan, J.; Bahreini, R.; Craven, J.; Emmons, L.; Ferrare, R.; Hayes, P. L.; Hodzic, A.; Holloway, J.; Hostetler, C.; Jimenez, J. L.; Jonsson, H.; Liu, S.; Liu, Y.; Metcalf, A.; Middlebrook, A.; Nowak, J.; Pekour, M.; Perring, A.; Russell, L.; Sedlacek, A.; Seinfeld, J.; Setyan, A.; Shilling, J.; Shrivastava, M.; Springston, S.; Song, C.; Subramanian, R.; Taylor, J. W.; Vinoj, V.; Yang, Q.; Zaveri, R. A.; Zhang, Q.

    2014-09-01

    The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using the extensive meteorological, trace gas, and aerosol measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The overall objective of the field campaigns was to obtain data needed to better understand processes that affect both climate and air quality, including emission assessments, transport and chemical aging of aerosols, aerosol radiative effects. Simulations were performed that examined the sensitivity of aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. We found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics quantifying the differences between observed and simulated quantities. Comparisons with lidar and in situ measurements indicate

  16. Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source

    Directory of Open Access Journals (Sweden)

    S. L. Haslett

    2018-01-01

    Full Text Available Particulate emissions from biomass burning can both alter the atmosphere's radiative balance and cause significant harm to human health. However, due to the large effect on emissions caused by even small alterations to the way in which a fuel burns, it is difficult to study particulate production of biomass combustion mechanistically and in a repeatable manner. In order to address this gap, in this study, small wood samples sourced from Côte D'Ivoire in West Africa were burned in a highly controlled laboratory environment. The shape and mass of samples, available airflow and surrounding thermal environment were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. This methodology produced remarkably repeatable results, allowing aerosol emissions to be mapped directly onto different phases of combustion. Emissions from pyrolysis were visible as a distinct phase before flaming was established. After flaming combustion was initiated, a black-carbon-dominant flame was observed during which very little organic aerosol was produced, followed by a period that was dominated by organic-carbon-producing smouldering combustion, despite the presence of residual flaming. During pyrolysis and smouldering, the two phases producing organic aerosol, distinct mass spectral signatures that correspond to previously reported variations in biofuel emissions measured in the atmosphere are found. Organic aerosol emission factors averaged over an entire combustion event were found to be representative of the time spent in the pyrolysis and smouldering phases, rather than reflecting a coupling between emissions and the mass loss of the sample. Further exploration of aerosol yields from similarly carefully controlled fires and a careful comparison with data from macroscopic fires and real-world emissions will help to deliver

  17. Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

    Science.gov (United States)

    Strada, Susanna; Unger, Nadine

    2016-04-01

    A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP) and isoprene emission. The impacts of different pollution aerosol sources (anthropogenic, biomass burning, and non-biomass burning) are investigated by performing sensitivity experiments. The model framework includes all known light and meteorological responses of photosynthesis, but uses fixed canopy structures and phenology. On a global scale, our results show that global land carbon fluxes (GPP and isoprene emission) are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse) by ˜ 9 %. At a regional scale, GPP and isoprene emission show a robust but opposite sensitivity to pollution aerosols in regions where forested canopies dominate. In eastern North America and Eurasia, anthropogenic pollution aerosols (mainly from non-biomass burning sources) enhance GPP by +5-8 % on an annual average. In the northwestern Amazon Basin and central Africa, biomass burning aerosols increase GPP by +2-5 % on an annual average, with a peak in the northwestern Amazon Basin during the dry-fire season (+5-8 %). The prevailing mechanism varies across regions: light scattering dominates in eastern North America, while a reduction in direct radiation dominates in Europe and China. Aerosol-induced GPP productivity increases in the Amazon and central Africa include an additional positive feedback from reduced canopy temperatures in response to increases in canopy conductance. In Eurasia and northeastern China, anthropogenic pollution aerosols drive a decrease in isoprene emission of -2 to -12 % on an annual average. Future research needs to incorporate the indirect effects of aerosols and possible feedbacks from dynamic carbon allocation and phenology.

  18. Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

    Science.gov (United States)

    Jathar, Shantanu Hemant

    Atmospheric aerosols exert a large influence on the Earth's climate and cause adverse public health effects, reduced visibility and material degradation. Secondary organic aerosol (SOA), defined as the aerosol mass arising from the oxidation products of gas-phase organic species, accounts for a significant fraction of the submicron atmospheric aerosol mass. Yet, there are large uncertainties surrounding the sources, atmospheric evolution and properties of SOA. This thesis combines laboratory experiments, extensive data analysis and global modeling to investigate the contribution of semi-volatile and intermediate volatility organic compounds (SVOC and IVOC) from combustion sources to SOA formation. The goals are to quantify the contribution of these emissions to ambient PM and to evaluate and improve models to simulate its formation. To create a database for model development and evaluation, a series of smog chamber experiments were conducted on evaporated fuel, which served as surrogates for real-world combustion emissions. Diesel formed the most SOA followed by conventional jet fuel / jet fuel derived from natural gas, gasoline and jet fuel derived from coal. The variability in SOA formation from actual combustion emissions can be partially explained by the composition of the fuel. Several models were developed and tested along with existing models using SOA data from smog chamber experiments conducted using evaporated fuel (this work, gasoline, fischertropschs, jet fuel, diesels) and published data on dilute combustion emissions (aircraft, on- and off-road gasoline, on- and off-road diesel, wood burning, biomass burning). For all of the SOA data, existing models under-predicted SOA formation if SVOC/IVOC were not included. For the evaporated fuel experiments, when SVOC/IVOC were included predictions using the existing SOA model were brought to within a factor of two of measurements with minor adjustments to model parameterizations. Further, a volatility

  19. Effect of aircraft exhaust sulfur emissions on near field plume aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

    1997-12-31

    Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

  20. Effect of aircraft exhaust sulfur emissions on near field plume aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Brown, R C; Miake-Lye, R C; Anderson, M R; Kolb, C E [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

    1998-12-31

    Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

  1. Impacts of controlling biomass burning emissions on wintertime carbonaceous aerosol in Europe

    NARCIS (Netherlands)

    Fountoukis, C.; Butler, T.; Lawrence, M.G.; Denier van der Gon, H.A.C.; Visschedijk, A.J.H.; Charalampidis, P.; Pilinis, C.; Pandis, S.N.

    2014-01-01

    We use a 3-D regional chemical transport model, with the latest advancements in the organic aerosol (OA) treatment, and an updated emission inventory for wood combustion to study the organic aerosol change in response to the replacement of current residential wood combustion technologies with pellet

  2. Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

    Directory of Open Access Journals (Sweden)

    S. Strada

    2016-04-01

    Full Text Available A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP and isoprene emission. The impacts of different pollution aerosol sources (anthropogenic, biomass burning, and non-biomass burning are investigated by performing sensitivity experiments. The model framework includes all known light and meteorological responses of photosynthesis, but uses fixed canopy structures and phenology. On a global scale, our results show that global land carbon fluxes (GPP and isoprene emission are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse by  ∼ 9 %. At a regional scale, GPP and isoprene emission show a robust but opposite sensitivity to pollution aerosols in regions where forested canopies dominate. In eastern North America and Eurasia, anthropogenic pollution aerosols (mainly from non-biomass burning sources enhance GPP by +5–8 % on an annual average. In the northwestern Amazon Basin and central Africa, biomass burning aerosols increase GPP by +2–5 % on an annual average, with a peak in the northwestern Amazon Basin during the dry-fire season (+5–8 %. The prevailing mechanism varies across regions: light scattering dominates in eastern North America, while a reduction in direct radiation dominates in Europe and China. Aerosol-induced GPP productivity increases in the Amazon and central Africa include an additional positive feedback from reduced canopy temperatures in response to increases in canopy conductance. In Eurasia and northeastern China, anthropogenic pollution aerosols drive a decrease in isoprene emission of −2 to −12 % on an annual average. Future research needs to incorporate the indirect effects of aerosols and possible feedbacks from dynamic carbon allocation and phenology.

  3. Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

    Science.gov (United States)

    Bahreini, R.; Middlebrook, A. M.; de Gouw, J. A.; Warneke, C.; Trainer, M.; Brock, C. A.; Stark, H.; Brown, S. S.; Dube, W. P.; Gilman, J. B.; Hall, K.; Holloway, J. S.; Kuster, W. C.; Perring, A. E.; Prevot, A. S. H.; Schwarz, J. P.; Spackman, J. R.; Szidat, S.; Wagner, N. L.; Weber, R. J.; Zotter, P.; Parrish, D. D.

    2012-03-01

    Although laboratory experiments have shown that organic compounds in both gasoline fuel and diesel engine exhaust can form secondary organic aerosol (SOA), the fractional contribution from gasoline and diesel exhaust emissions to ambient SOA in urban environments is poorly known. Here we use airborne and ground-based measurements of organic aerosol (OA) in the Los Angeles (LA) Basin, California made during May and June 2010 to assess the amount of SOA formed from diesel emissions. Diesel emissions in the LA Basin vary between weekdays and weekends, with 54% lower diesel emissions on weekends. Despite this difference in source contributions, in air masses with similar degrees of photochemical processing, formation of OA is the same on weekends and weekdays, within the measurement uncertainties. This result indicates that the contribution from diesel emissions to SOA formation is zero within our uncertainties. Therefore, substantial reductions of SOA mass on local to global scales will be achieved by reducing gasoline vehicle emissions.

  4. Could aerosol emissions be used for regional heat wave mitigation?

    Directory of Open Access Journals (Sweden)

    D. N. Bernstein

    2013-07-01

    Full Text Available Geoengineering applications by injection of sulfate aerosols into the stratosphere are under consideration as a measure of last resort to counter global warming. Here a potential regional-scale application to offset the impacts of heat waves is critically examined. Using the Weather Research and Forecasting model with fully coupled chemistry (WRF-Chem, the effect of regional-scale sulfate aerosol emission over California in each of two days of the July 2006 heat wave is used to quantify potential reductions in surface temperature as a function of emission rates in a layer at 12 km altitude. Local meteorological factors yield geographical differences in surface air temperature sensitivity. For emission rates of approximately 30 μg m−2 s−1 of sulfate aerosols (with standard WRF-Chem size distribution over the region, temperature decreases of around 7 °C result during the middle part of the day over the Central Valley, one of the areas hardest hit by the heat wave. Regions more ventilated with oceanic air such as Los Angeles have slightly smaller reductions. The length of the hottest part of the day is also reduced. Advection effects on the aerosol cloud must be more carefully forecast for smaller injection regions. Verification of the impacts could be done via measurements of differences in reflected and surface downward shortwave. Such regional geoengineering applications with specific near-term target effects but smaller cost and side effects could potentially provide a means of testing larger scale applications. However, design considerations for regional applications, such as a preference for injection at a level of relatively low wind speed, differ from those for global applications. The size of the required injections and the necessity of injection close to the target region raise substantial concerns. The evaluation of this regional-scale application is thus consistent with global model evaluations, emphasizing that mitigation via

  5. Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

    Directory of Open Access Journals (Sweden)

    Th. F. Mentel

    2013-09-01

    Full Text Available Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Biogenic secondary organic aerosols (BSOAs comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOCs emitted by vegetation are the source of BSOAs. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed BSOAs, and possibly their climatic effects. This raises questions of whether stress-induced changes in BSOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on BSOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical BSOA formation for plants infested by aphids in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify BSOA formation and yield. Stress-induced emissions of sesquiterpenes, methyl salicylate, and C17-BVOCs increase BSOA yields. Mixtures including these compounds exhibit BSOA yields between 17 and 33%, significantly higher than mixtures containing mainly monoterpenes (4–6% yield. Green leaf volatiles suppress SOA formation, presumably by scavenging OH, similar to isoprene. By classifying emission types, stressors and BSOA formation potential, we discuss possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate–vegetation feedback mechanisms.

  6. The role of anthropogenic aerosol emission reduction in achieving the Paris Agreement's objective

    Science.gov (United States)

    Hienola, Anca; Pietikäinen, Joni-Pekka; O'Donnell, Declan; Partanen, Antti-Ilari; Korhonen, Hannele; Laaksonen, Ari

    2017-04-01

    The Paris agreement reached in December 2015 under the auspices of the United Nation Framework Convention on Climate Change (UNFCCC) aims at holding the global temperature increase to well below 2◦C above preindustrial levels and "to pursue efforts to limit the temperature increase to 1.5◦C above preindustrial levels". Limiting warming to any level implies that the total amount of carbon dioxide (CO2) - the dominant driver of long-term temperatures - that can ever be emitted into the atmosphere is finite. Essentially, this means that global CO2 emissions need to become net zero. CO2 is not the only pollutant causing warming, although it is the most persistent. Short-lived, non-CO2 climate forcers also must also be considered. Whereas much effort has been put into defining a threshold for temperature increase and zero net carbon emissions, surprisingly little attention has been paid to the non-CO2 climate forcers, including not just the non-CO2 greenhouse gases (methane (CH4), nitrous oxide (N2O), halocarbons etc.) but also the anthropogenic aerosols like black carbon (BC), organic carbon (OC) and sulfate. This study investigates the possibility of limiting the temperature increase to 1.5◦C by the end of the century under different future scenarios of anthropogenic aerosol emissions simulated with the very simplistic MAGICC climate carbon cycle model as well as with ECHAM6.1-HAM2.2-SALSA + UVic ESCM. The simulations include two different CO2 scenarios- RCP3PD as control and a CO2 reduction leading to 1.5◦C (which translates into reaching the net zero CO2 emissions by mid 2040s followed by negative emissions by the end of the century); each CO2 scenario includes also two aerosol pollution control cases denoted with CLE (current legislation) and MFR (maximum feasible reduction). The main result of the above scenarios is that the stronger the anthropogenic aerosol emission reduction is, the more significant the temperature increase by 2100 relative to pre

  7. Semi-quantitative characterisation of ambient ultrafine aerosols resulting from emissions of coal fired power stations

    International Nuclear Information System (INIS)

    Hinkley, J.T.; Bridgman, H.A.; Buhre, B.J.P.; Gupta, R.P.; Nelson, P.F.; Wall, T.F.

    2008-01-01

    Emissions from coal fired power stations are known to be a significant anthropogenic source of fine atmospheric particles, both through direct primary emissions and secondary formation of sulfate and nitrate from emissions of gaseous precursors. However, there is relatively little information available in the literature regarding the contribution emissions make to the ambient aerosol, particularly in the ultrafine size range. In this study, the contribution of emissions to particles smaller than 0.3 μm in the ambient aerosol was examined at a sampling site 7 km from two large Australian coal fired power stations equipped with fabric filters. A novel approach was employed using conditional sampling based on sulfur dioxide (SO 2 ) as an indicator species, and a relatively new sampler, the TSI Nanometer Aerosol Sampler. Samples were collected on transmission electron microscope (TEM) grids and examined using a combination of TEM imaging and energy dispersive X-ray (EDX) analysis for qualitative chemical analysis. The ultrafine aerosol in low SO 2 conditions was dominated by diesel soot from vehicle emissions, while significant quantities of particles, which were unstable under the electron beam, were observed in the high SO 2 samples. The behaviour of these particles was consistent with literature accounts of sulfate and nitrate species, believed to have been derived from precursor emissions from the power stations. A significant carbon peak was noted in the residues from the evaporated particles, suggesting that some secondary organic aerosol formation may also have been catalysed by these acid seed particles. No primary particulate material was observed in the minus 0.3 μm fraction. The results of this study indicate the contribution of species more commonly associated with gas to particle conversion may be more significant than expected, even close to source

  8. Exchanges in boundary layer and low troposphere and consequences on pollution of Fos-Berre-Marseille area (ESCOMPTE experiment); Les aerosols: emissions, formation d'aerosols organiques secondaires, transport longue distance. Zoom sur les aerosols carbones en Europe

    Energy Technology Data Exchange (ETDEWEB)

    Guillaume, B

    2006-01-15

    There are two types of 'carbonaceous aerosols': 'black carbon' (BC) and 'organic carbon'(OC). BC is directly emitted in the atmosphere while OC is either directly emitted (primary OC, OCp) or secondarily formed through oxidation processes in the atmosphere (secondary organic aerosols, SOA). Complexity of carbonaceous aerosols is still poorly represented in existing aerosol models and uncertainties appear mainly both in their emission inventories and in their complex atmospheric evolution (transport, gas-particle interactions, dry/wet deposition), making difficult the estimation of their radiative impact. In this framework, I developed during my PhD at Laboratoire d'Aerologie, a new approach to deal with this complexity, with implementation of both a new carbonaceous aerosol emission inventory and a new aerosol modelling tool at global scale. My work is divided in 5 different tasks: - better characterisation of BC and OCp emissions, achieved through the development of a new emission inventory from fossil fuel and biofuel combustion sources (industrial, domestic and mobile sources). This inventory provides BC and OCp emissions for Europe at 25 km * 25 km resolution for the years 1990, 1995, 2000, 2005 and 2010, with two additional regional zooms: on France, at 10 km * 10 km resolution for the years 2000 and 2010 with improved road traffic, and in Marseille region (Escompte campaign, 1999,-2001) at 1 km * 1 km resolution for the year 1999; - better modelling of carbonaceous aerosol complex atmospheric evolution, through coupling of a global scale gas transport/chemistry model (TM4) with an aerosol module (ORISAM) featuring size-distributed aerosols (on 8 diameter sections from 40 nm to 10 {mu}m) organic/inorganic chemical composition and explicit treatment of SOA formation; - simulations with this new aerosol model ORISAM-TM4 and model/measurements comparisons to study BC and OC long-range transport; - sensitivity tests on SOA

  9. Updating Sea Spray Aerosol Emissions in the Community Multiscale Air Quality Model

    Science.gov (United States)

    Gantt, B.; Bash, J. O.; Kelly, J.

    2014-12-01

    Sea spray aerosols (SSA) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. In this study, the Community Multiscale Air Quality (CMAQ) model is updated to enhance fine mode SSA emissions, include sea surface temperature (SST) dependency, and revise surf zone emissions. Based on evaluation with several regional and national observational datasets in the continental U.S., the updated emissions generally improve surface concentrations predictions of primary aerosols composed of sea-salt and secondary aerosols affected by sea-salt chemistry in coastal and near-coastal sites. Specifically, the updated emissions lead to better predictions of the magnitude and coastal-to-inland gradient of sodium, chloride, and nitrate concentrations at Bay Regional Atmospheric Chemistry Experiment (BRACE) sites near Tampa, FL. Including SST-dependency to the SSA emission parameterization leads to increased sodium concentrations in the southeast U.S. and decreased concentrations along the Pacific coast and northeastern U.S., bringing predictions into closer agreement with observations at most Interagency Monitoring of Protected Visual Environments (IMPROVE) and Chemical Speciation Network (CSN) sites. Model comparison with California Research at the Nexus of Air Quality and Climate Change (CalNex) observations will also be discussed, with particular focus on the South Coast Air Basin where clean marine air mixes with anthropogenic pollution in a complex environment. These SSA emission updates enable more realistic simulation of chemical processes in coastal environments, both in clean marine air masses and mixtures of clean marine and polluted conditions.

  10. Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

    Directory of Open Access Journals (Sweden)

    T. Liu

    2017-06-01

    Full Text Available Cooking emissions can potentially contribute to secondary organic aerosol (SOA but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils was investigated in a potential aerosol mass (PAM chamber. Experiments were conducted at 19–20 °C and 65–70 % relative humidity (RH. The characterization instruments included a scanning mobility particle sizer (SMPS and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS. The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm−3 s, was 1. 35 ± 0. 30 µg min−1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5 from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc of SOA was −1.51 to −0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA and semi-volatile oxygenated organic aerosol (SV-OOA, indicating that SOA in these experiments was lightly oxidized.

  11. The global impact of the transport sectors on atmospheric aerosol: simulations for year 2000 emissions

    Directory of Open Access Journals (Sweden)

    M. Righi

    2013-10-01

    Full Text Available We use the EMAC (ECHAM/MESSy Atmospheric Chemistry global model with the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications to quantify the impact of transport emissions (land transport, shipping and aviation on the global aerosol. We consider a present-day (2000 scenario according to the CMIP5 (Climate Model Intercomparison Project Phase 5 emission data set developed in support of the IPCC (Intergovernmental Panel on Climate Change Fifth Assessment Report. The model takes into account particle mass and number emissions: The latter are derived from mass emissions under different assumptions on the size distribution of particles emitted by the three transport sectors. Additional sensitivity experiments are performed to quantify the effects of the uncertainties behind such assumptions. The model simulations show that the impact of the transport sectors closely matches the emission patterns. Land transport is the most important source of black carbon (BC pollution in the USA, Europe and the Arabian Peninsula, contributing up to 60–70% of the total surface-level BC concentration in these regions. Shipping contributes about 40–60% of the total aerosol sulfate surface-level concentration along the most-traveled routes of the northern Atlantic and northern Pacific oceans, with a significant impact (~ 10–20% along the coastlines. Aviation mostly affects aerosol number, contributing about 30–40% of the particle number concentration in the northern midlatitudes' upper troposphere (7–12 km, although significant effects are also simulated at the ground, due to the emissions from landing and take-off cycles. The transport-induced perturbations to the particle number concentrations are very sensitive to the assumptions on the size distribution of emitted particles, with the largest uncertainties (about one order of magnitude obtained for the land transport sector. The simulated climate impacts, due to

  12. Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

    Science.gov (United States)

    Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

    2014-12-01

    Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

  13. The effect of harmonized emissions on aerosol properties in global models – an AeroCom experiment

    Directory of Open Access Journals (Sweden)

    C. Textor

    2007-08-01

    Full Text Available The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA and one with unified emissions, injection heights, and particle sizes at the source (ExpB. Surprisingly, harmonization of aerosol sources has only a small impact on the simulated inter-model diversity of the global aerosol burden, and consequently global optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols and parameterizations of aerosol microphysics (e.g., the split between deposition pathways and to a lesser extent by the spatial and temporal distributions of the (precursor emissions.

    The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversities for these two species were caused by a few outliers. The experiment also showed that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences.

    These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.

  14. Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

    Science.gov (United States)

    Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

    2012-04-01

    New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

  15. Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

    Science.gov (United States)

    Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

    2018-03-01

    Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

  16. Photochemical production of aerosols from real plant emissions

    Directory of Open Access Journals (Sweden)

    Th. F. Mentel

    2009-07-01

    Full Text Available Emission of biogenic volatile organic compounds (VOC which on oxidation form secondary organic aerosols (SOA can couple the vegetation with the atmosphere and climate. Particle formation from tree emissions was investigated in a new setup: a plant chamber coupled to a reaction chamber for oxidizing the plant emissions and for forming SOA. Emissions from the boreal tree species birch, pine, and spruce were studied. In addition, α-pinene was used as reference compound. Under the employed experimental conditions, OH radicals were essential for inducing new particle formation, although O3 (≤80 ppb was always present and a fraction of the monoterpenes and the sesquiterpenes reacted with ozone before OH was generated. Formation rates of 3 nm particles were linearly related to the VOC carbon mixing ratios, as were the maximum observed volume and the condensational growth rates. For all trees, the threshold of new particle formation was lower than for α-pinene. It was lowest for birch which emitted the largest fraction of oxygenated VOC (OVOC, suggesting that OVOC may play a role in the nucleation process. Incremental mass yields were ≈5% for pine, spruce and α-pinene, and ≈10% for birch. α-Pinene was a good model compound to describe the yield and the growth of SOA particles from coniferous emissions. The mass fractional yields agreed well with observations for boreal forests. Despite the somewhat enhanced VOC and OH concentrations our results may be up-scaled to eco-system level. Using the mass fractional yields observed for the tree emissions and weighting them with the abundance of the respective trees in boreal forests SOA mass concentration calculations agree within 6% with field observations. For a future VOC increase of 50% we predict a particle mass increase due to SOA of 19% assuming today's mass contribution of pre-existing aerosol and oxidant levels.

  17. Primary anthropogenic aerosol emission trends for China, 1990–2005

    Directory of Open Access Journals (Sweden)

    Y. Lei

    2011-02-01

    Full Text Available An inventory of anthropogenic primary aerosol emissions in China was developed for 1990–2005 using a technology-based approach. Taking into account changes in the technology penetration within industry sectors and improvements in emission controls driven by stricter emission standards, a dynamic methodology was derived and implemented to estimate inter-annual emission factors. Emission factors of PM2.5 decreased by 7%–69% from 1990 to 2005 in different industry sectors of China, and emission factors of TSP decreased by 18%–80% as well, with the measures of controlling PM emissions implemented. As a result, emissions of PM2.5 and TSP in 2005 were 11.0 Tg and 29.7 Tg, respectively, less than what they would have been without the adoption of these measures. Emissions of PM2.5, PM10 and TSP presented similar trends: they increased in the first six years of 1990s and decreased until 2000, then increased again in the following years. Emissions of TSP peaked (35.5 Tg in 1996, while the peak of PM10 (18.8 Tg and PM2.5 (12.7 Tg emissions occurred in 2005. Although various emission trends were identified across sectors, the cement industry and biofuel combustion in the residential sector were consistently the largest sources of PM2.5 emissions, accounting for 53%–62% of emissions over the study period. The non-metallic mineral product industry, including the cement, lime and brick industries, accounted for 54%–63% of national TSP emissions. There were no significant trends of BC and OC emissions until 2000, but the increase after 2000 brought the peaks of BC (1.51 Tg and OC (3.19 Tg emissions in 2005. Although significant improvements in the estimation of primary aerosols are presented here, there still exist large uncertainties. More accurate and detailed activity information and emission factors based on local tests are essential to further improve emission estimates

  18. A new physically-based quantification of marine isoprene and primary organic aerosol emissions

    Directory of Open Access Journals (Sweden)

    N. Meskhidze

    2009-07-01

    Full Text Available The global marine sources of organic carbon (OC are estimated here using a physically-based parameterization for the emission of marine isoprene and primary organic matter. The marine isoprene emission model incorporates new physical parameters such as light sensitivity of phytoplankton isoprene production and dynamic euphotic depth to simulate hourly marine isoprene emissions totaling 0.92 Tg C yr−1. Sensitivity studies using different schemes for the euphotic zone depth and ocean phytoplankton speciation produce the upper and the lower range of marine-isoprene emissions of 0.31 to 1.09 Tg C yr−1, respectively. Established relationships between sea spray fractionation of water-insoluble organic carbon (WIOC and chlorophyll-a concentration are used to estimate the total primary sources of marine sub- and super-micron OC of 2.9 and 19.4 Tg C yr−1, respectively. The consistent spatial and temporal resolution of the two emission types allow us, for the first time, to explore the relative contributions of sub- and super-micron organic matter and marine isoprene-derived secondary organic aerosol (SOA to the total OC fraction of marine aerosol. Using a fixed 3% mass yield for the conversion of isoprene to SOA, our emission simulations show minor (<0.2% contribution of marine isoprene to the total marine source of OC on a global scale. However, our model calculations also indicate that over the tropical oceanic regions (30° S to 30° N, marine isoprene SOA may contribute over 30% of the total monthly-averaged sub-micron OC fraction of marine aerosol. The estimated contribution of marine isoprene SOA to hourly-averaged sub-micron marine OC emission is even higher, approaching 50% over the vast regions of the oceans during the midday hours when isoprene emissions are highest. As it is widely believed that sub-micron OC has the potential to influence the cloud droplet activation of marine aerosols, our

  19. Ocean Surface Emissivity at L-band (1.4 GHz): The Dependence on Salinity and Roughness

    Science.gov (United States)

    LeVine, D. M.; Lang, R.; Wentz, F.; Messiner, T.

    2012-01-01

    A characterization of the emissivity of sea water at L-band is important for the remote sensing of sea surface salinity. Measurements of salinity are currently being made in the radio astronomy band at 1.413 GHz by ESA's Soil Moisture and Ocean Salinity (SMOS) mission and NASA's Aquarius instrument aboard the Aquarius/SAC-D observatory. The goal of both missions is accuracy on the order of 0.1 psu. This requires accurate knowledge of the dielectric constant of sea water as a function of salinity and temperature and also the effect of waves (roughness). The former determines the emissivity of an ideal (i.e. flat) surface and the later is the major source of error from predictions based on a flat surface. These two aspects of the problem of characterizing the emissivity are being addressed in the context of the Aquarius mission. First, laboratory measurements are being made of the dielectric constant of sea water. This is being done at the George Washington University using a resonant cavity. In this technique, sea water of known salinity and temperature is fed into the cavity along its axis through a narrow tube. The sea water changes the resonant frequency and Q of the cavity which, if the sample is small enough, can be related to the dielectric constant of the sample. An extensive set of measurements have been conducted at 1.413 GHz to develop a model for the real and imaginary part of the dielectric constant as a function of salinity and temperature. The results are compared to the predictions of models based on parameterization of the Debye resonance of the water molecule. The models and measurements are close; however, the differences are significant for remote sensing of salinity. This is especially true at low temperatures where the sensitivity to salinity is lowest.

  20. Multi-Model Simulations of Aerosol and Ozone Radiative Forcing Due to Anthropogenic Emission Changes During the Period 1990-2015

    Science.gov (United States)

    Myhre, Gunnar; Aas, Wenche; Ribu, Cherian; Collins, William; Faluvegi, Gregory S.; Flanner, Mark; Forster, Piers; Hodnebrog, Oivind; Klimont, Zbigniew; Lund, Marianne T.

    2017-01-01

    Over the past few decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and air pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990-2015, as simulated by seven global atmospheric composition models. The models broadly reproduce large-scale changes in surface aerosol and ozone based on observations (e.g. 1 to 3 percent per year in aerosols over the USA and Europe). The global mean radiative forcing due to ozone and aerosol changes over the 1990-2015 period increased by 0.17 plus or minus 0.08 watts per square meter, with approximately one-third due to ozone. This increase is more strongly positive than that reported in IPCC AR5 (Intergovernmental Panel on Climate Change Fifth Assessment Report). The main reasons for the increased positive radiative forcing of aerosols over this period are the substantial reduction of global mean SO2 emissions, which is stronger in the new emission inventory compared to that used in the IPCC analysis, and higher black carbon emissions.

  1. Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

    Directory of Open Access Journals (Sweden)

    P. Q. Fu

    2013-02-01

    Full Text Available Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m−3 (mean 47.6 ng m−3, accounting for 1.8–11.0% (4.8% of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA tracers formed from the oxidation of biogenic volatile organic compounds (VOCs such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m−3 (9.2 ng m−3, followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC, we estimate that an average of 10.7% (up to 26.2% of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8% and α-pinene SOC (2.9%. In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

  2. Analysis of aerosol emission and hazard evaluation of electrical discharge machining (EDM) process.

    Science.gov (United States)

    Jose, Mathew; Sivapirakasam, S P; Surianarayanan, M

    2010-01-01

    The safety and environmental aspects of a manufacturing process are important due to increased environmental regulations and life quality. In this paper, the concentration of aerosols in the breathing zone of the operator of Electrical Discharge Machining (EDM), a commonly used non traditional manufacturing process is presented. The pattern of aerosol emissions from this process with varying process parameters such as peak current, pulse duration, dielectric flushing pressure and the level of dielectric was evaluated. Further, the HAZOP technique was employed to identify the inherent safety aspects and fire risk of the EDM process under different working conditions. The analysis of aerosol exposure showed that the concentration of aerosol was increased with increase in the peak current, pulse duration and dielectric level and was decreased with increase in the flushing pressure. It was also found that at higher values of peak current (7A) and pulse duration (520 micros), the concentration of aerosols at breathing zone of the operator was above the permissible exposure limit value for respirable particulates (5 mg/m(3)). HAZOP study of the EDM process showed that this process is vulnerable to fire and explosion hazards. A detailed discussion on preventing the fire and explosion hazard is presented in this paper. The emission and risk of fire of the EDM process can be minimized by selecting proper process parameters and employing appropriate control strategy.

  3. Final Report, The Influence of Organic-Aerosol Emissions and Aging on Regional and Global Aerosol Size Distributions and the CCN Number Budget

    Energy Technology Data Exchange (ETDEWEB)

    Donahue, Neil M. [Carnegie Mellon Univ., Pittsburgh, PA (United States)

    2015-12-23

    We conducted laboratory experiments and analyzed data on aging of organic aerosol and analysis of field data on volatility and CCN activity. With supplemental ASR funding we participated in the FLAME-IV campaign in Missoula MT in the Fall of 2012, deploying a two-chamber photochemical aging system to enable experimental exploration of photochemical aging of biomass burning emissions. Results from that campaign will lead to numerous publications, including demonstration of photochemical production of Brown Carbon (BrC) from secondary organic aerosol associated with biomass burning emissions as well as extensive characterization of the effect of photochemical aging on the overall concentrations of biomass burning organic aerosol. Excluding publications arising from the FLAME-IV campaign, project research resulted in 8 papers: [11, 5, 3, 10, 12, 4, 8, 7], including on in Nature Geoscience addressing the role of organic compounds in nanoparticle growth [11

  4. High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

    Science.gov (United States)

    Satheesh, S. K.

    2017-12-01

    Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on

  5. Refined Use of Satellite Aerosol Optical Depth Snapshots to Constrain Biomass Burning Emissions in the GOCART Model

    Science.gov (United States)

    Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James

    2017-10-01

    Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength for BB aerosol sources. Our previous work shows that to first order, satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the smoke source strength. We now refine the satellite-snapshot method and investigate where applying simple multiplicative emission adjustment factors alone to the widely used Global Fire Emission Database version 3 emission inventory can achieve regional-scale consistency between Moderate Resolution Imaging Spectroradiometer (MODIS) AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport model. The model and satellite AOD are compared globally, over a set of BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. Regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. We refine our approach to address physically based limitations of our earlier work (1) by expanding the number of fire cases from 124 to almost 900, (2) by using scaled reanalysis-model simulations to fill missing AOD retrievals in the MODIS observations, (3) by distinguishing the BB components of the total aerosol load from background aerosol in the near-source regions, and (4) by including emissions from fires too small to be identified explicitly in the satellite observations. The small-fire emission adjustment shows the complimentary nature of correcting for source strength and adding geographically distinct missing sources. Our analysis indicates that the method works best for fire cases where the BB fraction of total AOD is high, primarily evergreen or deciduous forests. In heavily polluted or agricultural burning regions, where smoke and background AOD values tend to be comparable, this approach

  6. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

    Data.gov (United States)

    U.S. Environmental Protection Agency — The uploaded data consists of the BRACE Na aerosol observations paired with CMAQ model output, the updated model's parameterization of sea salt aerosol emission size...

  7. Inorganic aerosols responses to emission changes in Yangtze River Delta, China.

    Science.gov (United States)

    Dong, Xinyi; Li, Juan; Fu, Joshua S; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    The new Chinese National Ambient Air Quality standards (CH-NAAQS) published on Feb. 29th, 2012 listed PM2.5 as criteria pollutant for the very first time. In order to probe into PM2.5 pollution over Yangtze River Delta, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Total PM2.5 concentration over YRD was found to have strong seasonal variation with higher values in winter months (up to 89.9 μg/m(3) in January) and lower values in summer months (down to 28.8 μg/m(3) in July). Inorganic aerosols were found to have substantial contribution to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3(-)) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3(-) concentration throughout the year. In winter, NO3(-) was found to increase under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4(+)) and sulfate (SO4(2-)), while other seasons showed decrease response of NO3(-). Sensitivity responses of NO3(-) under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3(-) formation was actually more sensitive to VOC than NOx due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols. Copyright © 2014 Elsevier B.V. All rights reserved.

  8. Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

    Energy Technology Data Exchange (ETDEWEB)

    Schroeder, F P

    2000-07-01

    A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

  9. Origin of surface and columnar Indian Ocean Experiment (INDOEX) aerosols using source- and region-tagged emissions transport in a general circulation model

    Science.gov (United States)

    Verma, S.; Venkataraman, C.; Boucher, O.

    2008-12-01

    We study the relative influence of aerosols emitted from different sectors and geographical regions on aerosol loading in south Asia. Sectors contributing aerosol emissions include biofuel and fossil fuel combustion, open biomass burning, and natural sources. Geographical regions include India (the Indo-Gangetic plain, central India, south India, and northwest India), southeast Asia, east Asia, Africa-west Asia, and the rest of the world. Simulations of the Indian Ocean Experiment (INDOEX), from January to March 1999, are made in the general circulation model of Laboratoire de Météorologie Dynamique (LMD-ZT GCM) with emissions tagged by sector and geographical region. Anthropogenic emissions dominate (54-88%) the predicted aerosol optical depth (AOD) over all the receptor regions. Among the anthropogenic sectors, fossil fuel combustion has the largest overall influence on aerosol loading, primarily sulfate, with emissions from India (50-80%) and rest of the world significantly influencing surface concentrations and AOD. Biofuel combustion has a significant influence on both the surface and columnar black carbon (BC) in particular over the Indian subcontinent and Bay of Bengal with emissions largely from the Indian region (60-80%). Open biomass burning emissions influence organic matter (OM) significantly, and arise largely from Africa-west Asia. The emissions from Africa-west Asia affect the carbonaceous aerosols AOD in all receptor regions, with their largest influence (AOD-BC: 60%; and AOD-OM: 70%) over the Arabian Sea. Among Indian regions, the Indo-Gangetic Plain is the largest contributor to anthropogenic surface mass concentrations and AOD over the Bay of Bengal and India. Dust aerosols are contributed mainly through the long-range transport from Africa-west Asia over the receptor regions. Overall, the model estimates significant intercontinental incursion of aerosol, for example, BC, OM, and dust from Africa-west Asia and sulfate from distant regions (rest

  10. Time-resolved analysis of primary volatile emissions and secondary aerosol formation potential from a small-scale pellet boiler

    Science.gov (United States)

    Czech, Hendryk; Pieber, Simone M.; Tiitta, Petri; Sippula, Olli; Kortelainen, Miika; Lamberg, Heikki; Grigonyte, Julija; Streibel, Thorsten; Prévôt, André S. H.; Jokiniemi, Jorma; Zimmermann, Ralf

    2017-06-01

    Small-scale pellet boilers and stoves became popular as a wood combustion appliance for domestic heating in Europe, North America and Asia due to economic and environmental aspects. Therefore, an increasing contribution of pellet boilers to air pollution is expected despite their general high combustion efficiency. As emissions of primary organic aerosol (POA) and permanent gases of pellet boilers are well investigated, the scope of this study was to investigate the volatile organic emissions and the formation potential of secondary aerosols for this type of appliance. Fresh and aged emissions were analysed by a soot-particle aerosol time-of-flight mass spectrometry (SP-AMS) and the molecular composition of the volatile precursors with single-photon ionisation time-of-flight mass spectrometry (SPI-TOFMS) at different pellet boiler operation conditions. Organic emissions in the gas phase were dominated by unsaturated hydrocarbons while wood-specific VOCs, e.g. phenolic species or substituted furans, were only detected during the starting phase. Furthermore, organic emissions in the gas phase were found to correlate with fuel grade and combustion technology in terms of secondary air supply. Secondary organic aerosols of optimised pellet boiler conditions (OPT, state-of-the-art combustion appliance) and reduced secondary air supply (RSA, used as a proxy for pellet boilers of older type) were studied by simulating atmospheric ageing in a Potential Aerosol Mass (PAM) flow reactor. Different increases in OA mass (55% for OPT, 102% for RSA), associated with higher average carbon oxidation state and O:C, could be observed in a PAM chamber experiment. Finally, it was found that derived SOA yields and emission factors were distinctly lower than reported for log wood stoves.

  11. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

    Science.gov (United States)

    Lu, Z.; Zhang, Q.; Streets, D. G.

    2011-09-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and

  12. Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect

    Science.gov (United States)

    Wang, Z. L.; Zhang, H.; Zhang, X. Y.

    2015-04-01

    Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in the short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate atmosphere-only model BCC_AGCM2.0.1_CUACE/Aero with prescribed sea surface temperature and sea ice cover, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with recent past year 2000 levels if the emissions of only BC are reduced to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial~for the mitigation of global warming. However, both aerosol negative direct and indirect radiative effects are weakened when BC and its co-emitted species (sulfur dioxide and organic carbon) are simultaneously reduced. Relative to year 2000 levels, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 if the emissions of all these aerosols are decreased to the levels projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

  13. Primary emissions and secondary aerosol production potential from woodstoves for residential heating: Influence of the stove technology and combustion efficiency

    Science.gov (United States)

    Bertrand, Amelie; Stefenelli, Giulia; Bruns, Emily A.; Pieber, Simone M.; Temime-Roussel, Brice; Slowik, Jay G.; Prévôt, André S. H.; Wortham, Henri; El Haddad, Imad; Marchand, Nicolas

    2017-11-01

    To reduce the influence of biomass burning on air quality, consumers are encouraged to replace their old woodstove with new and cleaner appliances. While their primary emissions have been extensively investigated, the impact of atmospheric aging on these emissions, including secondary organic aerosol (SOA) formation, remains unknown. Here, using an atmospheric smog chamber, we aim at understanding the chemical nature and quantify the emission factors of the primary organic aerosols (POA) from three types of appliances for residential heating, and to assess the influence of aging thereon. Two, old and modern, logwood stoves and one pellet burner were operated under typical conditions. Emissions from an entire burning cycle (past the start-up operation) were injected, including the smoldering and flaming phases, resulting in highly variable emission factors. The stoves emitted a significant fraction of POA (up to 80%) and black carbon. After ageing, the total mass concentration of organic aerosol (OA) increased on average by a factor of 5. For the pellet stove, flaming conditions were maintained throughout the combustion. The aerosol was dominated by black carbon (over 90% of the primary emission) and amounted to the same quantity of primary aerosol emitted by the old logwood stove. However, after ageing, the OA mass was increased by a factor of 1.7 only, thus rendering OA emissions by the pellet stove almost negligible compared to the other two stoves tested. Therefore, the pellet stove was the most reliable and least polluting appliance out of the three stoves tested. The spectral signatures of the POA and aged emissions by a High Resolution - Time of Flight - Aerosol Mass Spectrometer (Electron Ionization (EI) at 70 eV) were also investigated. The m/z 44 (CO2+) and high molecular weight fragments (m/z 115 (C9H7+), 137 (C8H9O2+), 167 (C9H11O3+) and 181 (C9H9O4+, C14H13+)) correlate with the modified combustion efficiency (MCE) allowing us to discriminate further

  14. Accessing the Impact of Sea-Salt Emissions on Aerosol Chemical Formation and Deposition Over Pearl River Delta, China

    Science.gov (United States)

    Fan, Q.; Wang, X.; Liu, Y.; Wu, D.; Chan, P. W.; Fan, S.; Feng, Y.

    2015-12-01

    Sea-salt aerosol (SSA) emissions have a significant impact on aerosol pollution and haze formation in the coastal areas. In this study, Models-3/CMAQ modeling system was utilized to access the impact of SSA emissions on aerosol chemical formation and deposition over Pearl River Delta (PRD), China in July 2006. More SSAs were transported inland from the open-ocean under the southeast wind in summertime. Two experiments (with and without SSA emissions in the CMAQ model) were set up to compare the modeling results with each other. The results showed that the increase of sulfate concentrations were more attributable to the primary emissions of coarse SO42- particles in SSA, while the increase of nitrate concentrations were more attributable to secondary chemical formations, known as the mechanisms of chloride depletion in SSA. In the coastal areas, 17.62 % of SO42-, 26.6% of NO3- and 38.2% of PM10 were attributed to SSA emissions, while those portions were less than 1% in the inland areas. The increases of PM10 and its components due to SSA emissions resulted in higher deposition fluxes over PRD, particularly in the coastal areas, except for the wet deposition of nitrate. Nitrate was more sensitive to SSA emissions in chemical formations than sulfate and dry deposition of aerosol was also more sensitive than that for wet deposition. Process analysis of sulfate and nitrate was applied to find out the difference of physical and chemical mechanisms between Guangzhou (the inland areas) and Zhuhai (the coastal areas). The negative contributions of dry deposition process to both sulfate and nitrate concentrations increased if SSA emissions were taken into account in the model, especially for Zhuhai. The negative contributions of cloud process also increased due to cloud scavenging and wet deposition process. In the coastal area, the gas-to-particle conversions became more active with high contributions of aerosol process to nitrate concentrations.

  15. Characterization of Wildfire-Induced Aerosol Emissions From the Maritime Continent Peatland and Central African Dry Savannah with MISR and CALIPSO Aerosol Products

    Science.gov (United States)

    Lee, Huikyo; Jeong, Su-Jong; Kalashnikova, Olga; Tosca, Mika; Kim, Sang-Woo; Kug, Jong-Seong

    2018-03-01

    Aerosol plumes from wildfires affect the Earth's climate system through regulation of the radiative budget and clouds. However, optical properties of aerosols from individual wildfire smoke plumes and their resultant impact on regional climate are highly variable. Therefore, there is a critical need for observations that can constrain the partitioning between different types of aerosols. Here we present the apparent influence of regional ecosystem types on optical properties of wildfire-induced aerosols based on remote sensing observations from two satellite instruments and three ground stations. The independent observations commonly show that the ratio of the absorbing aerosols is significantly lower in smoke plumes from the Maritime Continent than those from Central Africa, so that their impacts on regional climate are different. The observed light-absorbing properties of wildfire-induced aerosols are explained by dominant ecosystem types such as wet peatlands for the Maritime Continent and dry savannah for Central Africa, respectively. These results suggest that the wildfire-aerosol-climate feedback processes largely depend on the terrestrial environments from which the fires originate. These feedbacks also interact with climate under greenhouse warming. Our analysis shows that aerosol optical properties retrieved based on satellite observations are critical in assessing wildfire-induced aerosols forcing in climate models. The optical properties of carbonaceous aerosol mixtures used by state-of-the-art chemistry climate models may overestimate emissions for absorbing aerosols from wildfires over the Maritime Continent.

  16. Methods of analysis for complex organic aerosol mixtures from urban emission sources of particulate carbon

    International Nuclear Information System (INIS)

    Mazurek, M.A.; Hildemann, L.M.; Simoneit, B.R.T.

    1990-10-01

    Organic aerosols comprise approximately 30% by mass of the total fine particulate matter present in urban atmospheres. The chemical composition of such aerosols is complex and reflects input from multiple sources of primary emissions to the atmosphere, as well as from secondary production of carbonaceous aerosol species via photochemical reactions. To identify discrete sources of fine carbonaceous particles in urban atmospheres, analytical methods must reconcile both bulk chemical and molecular properties of the total carbonaceous aerosol fraction. This paper presents an overview of the analytical protocol developed and used in a study of the major sources of fine carbon particles emitted to an urban atmosphere. 23 refs., 1 fig., 2 tabs

  17. Aerosol characterization during project POLINAT

    Energy Technology Data Exchange (ETDEWEB)

    Hagen, D.E.; Hopkins, A.R.; Paladino, J.D.; Whitefield, P.D. [Missouri Univ., Rolla, MO (United States). Cloud and Aerosol Sciences Lab.; Lilenfeld, H.V. [McDonnell Douglas Aerospace-East, St. Louis, MO (United States)

    1997-12-31

    The objectives of the aerosol/particulate characterization measurements of project POLINAT (POLlution from aircraft emissions In the North ATlantic flight corridor) are: to search for aerosol/particulate signatures of air traffic emissions in the region of the North Atlantic Flight Corridor; to search for the aerosol/particulate component of large scale enhancement (`corridor effects`) of air traffic related species in the North Atlantic region; to determine the effective emission indices for the aerosol/particulate component of engine exhaust in both the near and far field of aircraft exhaust plumes; to measure the dispersion and transformation of the aerosol/particulate component of aircraft emissions as a function of ambient condition; to characterize background levels of aerosol/particulate concentrations in the North Atlantic Region; and to determine effective emission indices for engine exhaust particulates for regimes beyond the jet phase of plume expansion. (author) 10 refs.

  18. Aerosol characterization during project POLINAT

    Energy Technology Data Exchange (ETDEWEB)

    Hagen, D E; Hopkins, A R; Paladino, J D; Whitefield, P D [Missouri Univ., Rolla, MO (United States). Cloud and Aerosol Sciences Lab.; Lilenfeld, H V [McDonnell Douglas Aerospace-East, St. Louis, MO (United States)

    1998-12-31

    The objectives of the aerosol/particulate characterization measurements of project POLINAT (POLlution from aircraft emissions In the North ATlantic flight corridor) are: to search for aerosol/particulate signatures of air traffic emissions in the region of the North Atlantic Flight Corridor; to search for the aerosol/particulate component of large scale enhancement (`corridor effects`) of air traffic related species in the North Atlantic region; to determine the effective emission indices for the aerosol/particulate component of engine exhaust in both the near and far field of aircraft exhaust plumes; to measure the dispersion and transformation of the aerosol/particulate component of aircraft emissions as a function of ambient condition; to characterize background levels of aerosol/particulate concentrations in the North Atlantic Region; and to determine effective emission indices for engine exhaust particulates for regimes beyond the jet phase of plume expansion. (author) 10 refs.

  19. Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

    Science.gov (United States)

    Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

    2017-12-01

    Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

  20. Determination of the power of multielement aerosol composition emission from distant industrial sources

    International Nuclear Information System (INIS)

    Popova, S.A.; Kutsenogij, K.P.; Chankina, O.V.

    2008-01-01

    The results from the monitoring of the temporal variability of the multielement composition of atmospheric aerosols are presented. They are used to determine the emission power of a series of elements from distant sources.

  1. Mass yields of secondary organic aerosols from the oxidation of α-pinene and real plant emissions

    Directory of Open Access Journals (Sweden)

    J. N. Smith

    2011-02-01

    Full Text Available Biogenic volatile organic compounds (VOCs are a significant source of global secondary organic aerosol (SOA; however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L. and Norway spruce (Picea abies, by hydroxyl radical (OH and ozone (O3. Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorized as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 17.7% at 26.0 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.

  2. The effect of South American biomass burning aerosol emissions on the regional climate

    Science.gov (United States)

    Thornhill, Gillian D.; Ryder, Claire L.; Highwood, Eleanor J.; Shaffrey, Len C.; Johnson, Ben T.

    2018-04-01

    The impact of biomass burning aerosol (BBA) on the regional climate in South America is assessed using 30-year simulations with a global atmosphere-only configuration of the Met Office Unified Model. We compare two simulations of high and low emissions of biomass burning aerosol based on realistic interannual variability. The aerosol scheme in the model has hygroscopic growth and optical properties for BBA informed by recent observations, including those from the recent South American Biomass Burning Analysis (SAMBBA) intensive aircraft observations made during September 2012. We find that the difference in the September (peak biomass emissions month) BBA optical depth between a simulation with high emissions and a simulation with low emissions corresponds well to the difference in the BBA emissions between the two simulations, with a 71.6 % reduction from high to low emissions for both the BBA emissions and the BB AOD in the region with maximum emissions (defined by a box of extent 5-25° S, 40-70° W, used for calculating mean values given below). The cloud cover at all altitudes in the region of greatest BBA difference is reduced as a result of the semi-direct effect, by heating of the atmosphere by the BBA and changes in the atmospheric stability and surface fluxes. Within the BBA layer the cloud is reduced by burn-off, while the higher cloud changes appear to be responding to stability changes. The boundary layer is reduced in height and stabilized by increased BBA, resulting in reduced deep convection and reduced cloud cover at heights of 9-14 km, above the layer of BBA. Despite the decrease in cloud fraction, September downwelling clear-sky and all-sky shortwave radiation at the surface is reduced for higher emissions by 13.77 ± 0.39 W m-2 (clear-sky) and 7.37 ± 2.29 W m-2 (all-sky), whilst the upwelling shortwave radiation at the top of atmosphere is increased in clear sky by 3.32 ± 0.09 W m-2, but decreased by -1.36±1.67 W m-2 when cloud changes are

  3. Distinguishing the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks in ;APEC Blue;

    Science.gov (United States)

    Gao, Meng; Liu, Zirui; Wang, Yuesi; Lu, Xiao; Ji, Dongsheng; Wang, Lili; Li, Meng; Wang, Zifa; Zhang, Qiang; Carmichael, Gregory R.

    2017-10-01

    Air quality are strongly influenced by both emissions and meteorological conditions. During the Asia Pacific Economic Cooperation (APEC) week (November 5-11, 2014), the Chinese government implemented unprecedented strict emission control measures in Beijing and surrounding provinces, and then a phenomenon referred to as ;APEC Blue; (rare blue sky) occurred. It is challenging to quantify the effectiveness of the implemented strict control measures solely based on observations. In this study, we use the WRF-Chem model to distinguish the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks during APEC week. In general, meteorological variables, PM2.5 concentrations and PM2.5 chemical compositions are well reproduced in Beijing. Positive weather conditions (lower temperature, lower relative humidity, higher wind speeds and enhanced boundary layer heights) play important roles in ;APEC Blue;. Applying strict emission control measures in Beijing and five surrounding provinces can only explain an average decrease of 17.7 μg/m3 (-21.8%) decreases in PM2.5 concentrations, roughly more than half of which is caused by emission controls that implemented in the five surrounding provinces (12.5 μg/m3). During the APEC week, non-local emissions contributed to 41.3% to PM2.5 concentrations in Beijing, and the effectiveness of implementing emission control measures hinges on dominant pathways and transport speeds. Besides, we also quantified the contribution of reduced aerosol feedbacks due to strict emission control measures in this study. During daytime, co-benefits of reduced aerosol feedbacks account for about 10.9% of the total decreases in PM2.5 concentrations in urban Beijing. The separation of contributions from aerosol absorption and scattering restates the importance of controlling BC to accelerate the effectiveness of aerosol pollution control.

  4. Study of radioactive aerosols emissions and establishment of a model in a nuclear medicine environment during the use of a technetium generator

    International Nuclear Information System (INIS)

    Bombardier, Pierre

    2012-01-01

    This work deals with the control of radioactive aerosols emissions inside the nuclear medicine facilities. These emissions occur during pulmonary scintigraphy examinations using aerosols marked with 99m Tc. Using a test chamber, we have developed a method permitting to quantify these emissions around the aerosol generator. A method dedicated to emissions measurement coming from the patient during the pulmonary ventilation is also described. The results obtained on one patient are exposed in this thesis. We characterized and modelled the ventilation of a complete nuclear medicine department with a CFD (Computational Fluid Dynamics) software. This permitted us to study the dissemination of the radioactive aerosol and to compare it with measures of ambient air activity. The numerical model of this department was then employed to test containment solutions and to help defining the best location for air contaminations sensors. An original method combining staff position information and the simulation of the dissemination for the aerosol released has been used to confirm the exposure levels for several professional groups and enhance the workplace studies. (author)

  5. Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

    Science.gov (United States)

    Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

    2009-04-01

    Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

  6. Estimate of biogenic VOC emissions in Japan and their effects on photochemical formation of ambient ozone and secondary organic aerosol

    Science.gov (United States)

    Chatani, Satoru; Matsunaga, Sou N.; Nakatsuka, Seiji

    2015-11-01

    A new gridded database has been developed to estimate the amount of isoprene, monoterpene, and sesquiterpene emitted from all the broadleaf and coniferous trees in Japan with the Model of Emissions of Gases and Aerosols from Nature (MEGAN). This database reflects the vegetation specific to Japan more accurately than existing ones. It estimates much lower isoprene emitted from other vegetation than trees, and higher sesquiterpene emissions mainly emitted from Cryptomeria japonica, which is the most abundant plant type in Japan. Changes in biogenic emissions result in the decrease in ambient ozone and increase in organic aerosol simulated by the air quality simulation over the Tokyo Metropolitan Area in Japan. Although newly estimated biogenic emissions contribute to a better model performance on overestimated ozone and underestimated organic aerosol, they are not a single solution to solve problems associated with the air quality simulation.

  7. Morphology of the Ovaries in Condition of Inhalation Intoxication with Dust-Saline Aerosols of the Aral Sea in Female White Rats

    Directory of Open Access Journals (Sweden)

    Yasminur G. Turdybekova

    2018-06-01

    CONCLUSIONS: Taking into account the proven effect of dust-saline aerosols on the production of estrogen, the violation of the postovulatory phase of the ovarian cycle, we trace the mechanism of folliculogenesis disturbance. This confirms the data of our previous studies on primary and secondary infertility in women living in the Aral Sea region and the necessity of creation and development of preventive measures for the inhabitants of the region.

  8. Changes in future air quality, deposition, and aerosol-cloud interactions under future climate and emission scenarios

    Energy Technology Data Exchange (ETDEWEB)

    Glotfelty, Timothy; Zhang, Yang; Karamchandani, Prakash; Streets, David G.

    2016-08-01

    The prospect of global climate change will have wide scale impacts, such as ecological stress and human health hazards. One aspect of concern is future changes in air quality that will result from changes in both meteorological forcing and air pollutant emissions. In this study, the GU-WRF/Chem model is employed to simulate the impact of changing climate and emissions following the IPCC AR4 SRES A1B scenario. An average of 4 future years (2020, 2030, 2040, and 2050) is compared against an average of 2 current years (2001 and 2010). Under this scenario, by the Mid-21st century global air quality is projected to degrade with a global average increase of 2.5 ppb in the maximum 8-hr O3 level and of 0.3 mg m3 in 24-hr average PM2.5. However, PM2.5 changes are more regional due to regional variations in primary aerosol emissions and emissions of gaseous precursor for secondary PM2.5. Increasing NOx emissions in this scenario combines with a wetter climate elevating levels of OH, HO2, H2O2, and the nitrate radical and increasing the atmosphere’s near surface oxidation state. This differs from findings under the RCP scenarios that experience declines in OH from reduced NOx emissions, stratospheric recovery of O3, and increases in CH4 and VOCs. Increasing NOx and O3 levels enhances the nitrogen and O3 deposition, indicating potentially enhanced crop damage and ecosystem stress under this scenario. The enhanced global aerosol level results in enhancements in aerosol optical depth, cloud droplet number concentration, and cloud optical thickness. This leads to dimming at the Earth’s surface with a global average reduction in shortwave radiation of 1.2 W m2 . This enhanced dimming leads to a more moderate warming trend and different trends in radiation than those found in NCAR’s CCSM simulation, which does not include the advanced chemistry and aerosol

  9. A study of photochemical againg of ambient air using Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions

    Science.gov (United States)

    Lee, T.; Son, J.; Kim, J.; Kim, S.; Sung, K.; Park, G.; Link, M.; Park, T.; Kim, K.; Kang, S.; Ban, J.; Kim, D. S.

    2016-12-01

    Recent research proposed that Secondary Aerosol (SA) is important class of predicting future climate change scenarios, health effect, and a general air quality. However, there has been lack of studies to investigate SA formation all over the world. This study tried to focus on understanding potential secondary aerosol formation and its local impact by the photochemical aging of inorganic and organic aerosols in the ambient air using the Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions. PAM chamber manufactured by Aerodyne make an oxidizing environment that simulates oxidation processes on timescales of 12-15 hrs in the atmosphere. Chemical compositions of ambient aerosol and aerosol that was aged in the PAM chamber were alternately measured every 2-minutes using the High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS). HR-ToF-AMS provides non-refractory aerosol mass concentrations including nitrate, sulfate, hydrocarbon-like and oxygenated organic aerosol in real time. This study includes a residence area of mixture of sources, a forest site of dominant source of biogenic VOCs, an underground parking lot of dominant vehicle emission, and laboratory experiment of vehicle emissions under different fuels and speeds using the chassis dynamometer. As a result, it was revealed that gasoline and LPG vehicle relatively made more potential SA than diesel vehicle.

  10. Numerical simulations of Aerosol and Trace Gas Emissions and Transformations over the North China Plain

    Science.gov (United States)

    He, H.; Ren, X.; Li, Z.; Dickerson, R. R.

    2016-12-01

    The North China Plain (NCP) is one of the most populated and polluted regions on Earth. In the past decades the rapid economic development has resulted in heavy atmospheric aerosol loadings in this region. The high aerosol concentrations induce severe environmental and climate problems, and aerosols can also affect human health and visibility. So there is a continued need to understand air quality in this region and transport of air pollutants from this region as populations grow, energy use increases, and industrial activity evolves. The unique mix of species over the NCP makes understanding the processes leading to transformations of primary pollutants and formation of secondary pollutants essential to predicting regional and global impacts. WRF-Chem simulations were performed for the NCP to investigate the emissions and transformations of air pollutants. MIX emission inventory of year 2010 (developed for MICS-Asia III and HTAP projects) was used to drive the WRF-Chem model. Modeling results were evaluated with observation data including OMI SO2/NO2 and MODIS AOD products to improve our knowledge of emission changes in the NCP between 2010 and 2016. We also estimated the regional transport of air pollutants from the NCP to downwind areas such as South Korea and Japan with WRF-Chem simulations constrained by these observations.

  11. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

    Science.gov (United States)

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

  12. Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

    Science.gov (United States)

    Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

    2018-04-01

    In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and

  13. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996–2010

    Directory of Open Access Journals (Sweden)

    Z. Lu

    2011-09-01

    Full Text Available China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2 and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC emissions from these two countries for the period 1996–2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %–17 % due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs of SO2, BC, and OC emissions are estimated to be −16 %–17 %, −43 %–93 %, and −43 %–80 % for China, and −15 %–16 %, −41 %–87 %, and −44 %–92

  14. The influence of soil salinity on volatile organic compounds emission and photosynthetic parameters of Solanum lycopersicum L. varieties

    Directory of Open Access Journals (Sweden)

    Tomescu Daniel

    2017-05-01

    Full Text Available Soil salinity is one of the best known stress factors of plants that can lead to crop yield reduction. Therefore, it is important to identify new tolerance varieties of plants that can grow on saline soils. We have studied the influence of salt on five different tomato varieties from the Western region of Romania and compared them with a commercial hybrid and found that one of them (Rudna is a very salt-tolerant variety (up to 200 mM NaCl. The assimilation rates and stomata conductance of water vapour are affected by salinity but some of the local varieties of tomato exhibit quite good tolerance. We found that all plants under salinity stress emit (Z-3-hexenol (a C6, green leaf volatile and the emission of all terpenes increased in proportion to the salt concentration. The emission of three terpenes, (Z-beta-ocimene. 2-carene and beta-phellandrene, have been quantitatively correlated with salt concentration.

  15. Historical (1750-2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

    Science.gov (United States)

    Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang; Klimont, Zbigniew; Janssens-Maenhout, Greet; Pitkanen, Tyler; Seibert, Jonathan J.; Vu, Linh; Andres, Robert J.; Bolt, Ryan M.; Bond, Tami C.; Dawidowski, Laura; Kholod, Nazar; Kurokawa, June-ichi; Li, Meng; Liu, Liang; Lu, Zifeng; Moura, Maria Cecilia P.; O'Rourke, Patrick R.; Zhang, Qiang

    2018-01-01

    We present a new data set of annual historical (1750-2014) anthropogenic chemically reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs), carbonaceous aerosols (black carbon - BC, and organic carbon - OC), and CO2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.

  16. Emission of intermediate, semi and low volatile organic compounds from traffic and their impact on secondary organic aerosol concentrations over Greater Paris

    Science.gov (United States)

    Sartelet, K.; Zhu, S.; Moukhtar, S.; André, M.; André, J. M.; Gros, V.; Favez, O.; Brasseur, A.; Redaelli, M.

    2018-05-01

    Exhaust particle emissions are mostly made of black carbon and/or organic compounds, with some of these organic compounds existing in both the gas and particle phases. Although emissions of volatile organic compounds (VOC) are usually measured at the exhaust, emissions in the gas phase of lower volatility compounds (POAvapor) are not. However, these gas-phase emissions may be oxidised after emission and enhance the formation of secondary organic aerosols (SOA). They are shown here to contribute to most of the SOA formation in Central Paris. POAvapor emissions are usually estimated from primary organic aerosol emissions in the particle phase (POA). However, they could also be estimated from VOC emissions for both gasoline and diesel vehicles using previously published measurements from chamber measurements. Estimating POAvapor from VOC emissions and ageing exhaust emissions with a simple model included in the Polyphemus air-quality platform compare well to measurements of SOA formation performed in chamber experiments. Over Greater Paris, POAvapor emissions estimated using POA and VOC emissions are compared using the HEAVEN bottom-up traffic emissions model. The impact on the simulated atmospheric concentrations is then assessed using the Polyphemus/Polair3D chemistry-transport model. Estimating POAvapor emissions from VOC emissions rather than POA emissions lead to lower emissions along motorway axes (between -50% and -70%) and larger emissions in urban areas (up to between +120% and +140% in Central Paris). The impact on total organic aerosol concentrations (gas plus particle) is lower than the impact on emissions: between -8% and 25% along motorway axes and in urban areas respectively. Particle-phase organic concentrations are lower when POAvapor emissions are estimated from VOC than POA emissions, even in Central Paris where the total organic aerosol concentration is higher, because of different assumptions on the emission volatility distribution, stressing the

  17. Primary emissions and secondary organic aerosol formation from the exhaust of a flex-fuel (ethanol) vehicle

    Science.gov (United States)

    Suarez-Bertoa, R.; Zardini, A. A.; Platt, S. M.; Hellebust, S.; Pieber, S. M.; El Haddad, I.; Temime-Roussel, B.; Baltensperger, U.; Marchand, N.; Prévôt, A. S. H.; Astorga, C.

    2015-09-01

    Incentives to use biofuels may result in increasing vehicular emissions of compounds detrimental to air quality. Therefore, regulated and unregulated emissions from a Euro 5a flex-fuel vehicle, tested using E85 and E75 blends (gasoline containing 85% and 75% of ethanol (vol/vol), respectively), were investigated at 22 and -7 °C over the New European Driving Cycle, at the Vehicle Emission Laboratory at the European Commission Joint Research Centre Ispra, Italy. Vehicle exhaust was comprehensively analyzed at the tailpipe and in a dilution tunnel. A fraction of the exhaust was injected into a mobile smog chamber to study the photochemical aging of the mixture. We found that emissions from a flex-fuel vehicle, fueled by E85 and E75, led to secondary organic aerosol (SOA) formation, despite the low aromatic content of these fuel blends. Emissions of regulated and unregulated compounds, as well as emissions of black carbon (BC) and primary organic aerosol (POA) and SOA formation were higher at -7 °C. The flex-fuel unregulated emissions, mainly composed of ethanol and acetaldehyde, resulted in very high ozone formation potential and SOA, especially at low temperature (860 mg O3 km-1 and up to 38 mg C kg-1). After an OH exposure of 10 × 106 cm-3 h, SOA mass was, on average, 3 times larger than total primary particle mass emissions (BC + POA) with a high O:C ratio (up to 0.7 and 0.5 at 22 and -7 °C, respectively) typical of highly oxidized mixtures. Furthermore, high resolution organic mass spectra showed high 44/43 ratios (ratio of the ions m/z 44 and m/z 43) characteristic of low-volatility oxygenated organic aerosol. We also hypothesize that SOA formation from vehicular emissions could be due to oxidation products of ethanol and acetaldehyde, both short-chain oxygenated VOCs, e.g. methylglyoxal and acetic acid, and not only from aromatic compounds.

  18. Characterizing the influence of anthropogenic emissions and transport variability on sulfate aerosol concentrations at Mauna Loa Observatory

    Science.gov (United States)

    Potter, Lauren E.

    Sulfate aerosol in the atmosphere has substantial impacts on human health and environmental quality. Most notably, atmospheric sulfate has the potential to modify the earth's climate system through both direct and indirect radiative forcing mechanisms (Meehl et al., 2007). Emissions of sulfur dioxide, the primary precursor of sulfate aerosol, are now globally dominated by anthropogenic sources as a result of widespread fossil fuel combustion. Economic development in Asian countries since 1990 has contributed considerably to atmospheric sulfur loading, particularly China, which currently emits approximately 1/3 of global anthropogenic SO2 (Klimont et al., 2013). Observational and modeling studies have confirmed that anthropogenic pollutants from Asian sources can be transported long distances with important implications for future air quality and global climate change. Located in the remote Pacific Ocean (19.54°N, 155.58°W) at an elevation of 3.4 kilometers above sea level, Mauna Loa Observatory (MLO) is an ideal measurement site for ground-based, free tropospheric observations and is well situated to experience influence from springtime Asian outflow. This study makes use of a 14-year data set of aerosol ionic composition, obtained at MLO by the University of Hawaii at Manoa. Daily filter samples of total aerosol concentrations were made during nighttime downslope (free-tropospheric) transport conditions, from 1995 to 2008, and were analyzed for aerosol-phase concentrations of the following species: nitrate (NO3-), sulfate (SO42-), methanesulfonate (MSA), chloride (Cl-), oxalate, sodium (Na+), ammonium (NH 4+), potassium (K+), magnesium (Mg 2+), and calcium (Ca2+). An understanding of the factors controlling seasonal and interannual variations in aerosol speciation and concentrations at this site is complicated by the relatively short lifetimes of aerosols, compared with greenhouse gases which have also been sampled over long time periods at MLO. Aerosol filter

  19. Retrieving global aerosol sources from satellites using inverse modeling

    Directory of Open Access Journals (Sweden)

    O. Dubovik

    2008-01-01

    Full Text Available Understanding aerosol effects on global climate requires knowing the global distribution of tropospheric aerosols. By accounting for aerosol sources, transports, and removal processes, chemical transport models simulate the global aerosol distribution using archived meteorological fields. We develop an algorithm for retrieving global aerosol sources from satellite observations of aerosol distribution by inverting the GOCART aerosol transport model.

    The inversion is based on a generalized, multi-term least-squares-type fitting, allowing flexible selection and refinement of a priori algorithm constraints. For example, limitations can be placed on retrieved quantity partial derivatives, to constrain global aerosol emission space and time variability in the results. Similarities and differences between commonly used inverse modeling and remote sensing techniques are analyzed. To retain the high space and time resolution of long-period, global observational records, the algorithm is expressed using adjoint operators.

    Successful global aerosol emission retrievals at 2°×2.5 resolution were obtained by inverting GOCART aerosol transport model output, assuming constant emissions over the diurnal cycle, and neglecting aerosol compositional differences. In addition, fine and coarse mode aerosol emission sources were inverted separately from MODIS fine and coarse mode aerosol optical thickness data, respectively. These assumptions are justified, based on observational coverage and accuracy limitations, producing valuable aerosol source locations and emission strengths. From two weeks of daily MODIS observations during August 2000, the global placement of fine mode aerosol sources agreed with available independent knowledge, even though the inverse method did not use any a priori information about aerosol sources, and was initialized with a "zero aerosol emission" assumption. Retrieving coarse mode aerosol emissions was less successful

  20. Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

    Science.gov (United States)

    A. A. May; G. R. McMeeking; T. Lee; J. W. Taylor; J. S. Craven; I. Burling; A. P. Sullivan; S. Akagi; J. L. Collett; M. Flynn; H. Coe; S. P. Urbanski; J. H. Seinfeld; R. J. Yokelson; S. M. Kreidenweis

    2014-01-01

    Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California...

  1. Future aerosols of the southwest - Implications for fundamental aerosol research

    International Nuclear Information System (INIS)

    Friedlander, S.K.

    1980-01-01

    It is shown that substantial increases in the use of coal in the U.S. will lead to substantial increases in emissions of particulate matter, SO/sub x/, and NO/sub x/ in the part of the U.S. west of the Mississippi. A shift in the primary particulate emissions from coarse to submicron particles is predicted. Attention is given to the nature of the submicron aerosol in the southwest, the distribution of sulfur with respect to particle size, the formation of new particles in the atmosphere, and the ammonium nitrate equilibrium. It is concluded that increased coal use will result in a 50% increase in SO/sub x/ emissions and a doubling of NO/sub x/ emissions in the western U.S. by the year 2000, that ambient levels of aerosol sulfates and nitrates will increase, and that a large increase in submicron aerosol mass is likely

  2. Factors Affecting Aerosol Radiative Forcing

    Science.gov (United States)

    Wang, J.; Lin, J.; Ni, R.

    2016-12-01

    Rapid industrial and economic growth has meant large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RFof aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissionsper unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size.South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions,its aerosol RF is alleviated by its lowest chemical efficiency.The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is loweredbyasmall per capita GDP.Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The resulting

  3. Applications of particle induced X-ray emission analysis to ambient aerosol studies

    International Nuclear Information System (INIS)

    Lannefors, H.

    1982-01-01

    The characteristics of Particle Induced X-ray Emission (PIXE) analysis in conjunction with different ambient aerosol samplers have been studied. Correction factors have been calculated for homogeneous and inhomogeneous rural and urban aerosol samples. The Nuclepore two stage filter sampler provided the most useful combination of the resolution and particle size fractionation in urban, rural and remote environments. The PIXE-analysis technique in combination with different samplers was employed in aerosol composition studies in rural and remote environments. Particular emphasis was laid on studies of aerosol long range transport. Based on air mass trajectory analysis and aerosol composition measurements the foreign contribution in southern Sweden was estimated to be 70 - 80% for S and Pb but only 30 - 50% for V and Ni. The spatial and temporal extension of a long range transport episode was studied using high time resolution continuous filter samplers in a network in southern Sweden. The variation in the concentration levels of sulphur agreed well with changes in the air mass history. Arctic summer elemental concentration levels as measured during the Swedish YMER-80 icebreaker expedition were typically one order of magnitude lower than Arctic winter levels. The combination of chemical information, optical properties and size distribution data supports the hypothesis of long range transport of air pollution into the Arctic especially during the winter. This takes place during the winter season because the Polar front is further south making conditions for long range transport up to the Arctic more favourable. (Auth.)

  4. Historical (1750–2014 anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS

    Directory of Open Access Journals (Sweden)

    R. M. Hoesly

    2018-01-01

    Full Text Available We present a new data set of annual historical (1750–2014 anthropogenic chemically reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs, carbonaceous aerosols (black carbon – BC, and organic carbon – OC, and CO2 developed with the Community Emissions Data System (CEDS. We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.

  5. Laboratory Measurements of Biomass Cook-stove Emissions Aged in an Oxidation Flow Reactor: Influence of Combustion and Aging Conditions on Aerosols

    Science.gov (United States)

    Grieshop, A. P.; Reece, S. M.; Sinha, A.; Wathore, R.

    2016-12-01

    Combustion in rudimentary and improved cook-stoves used by billions in developing countries can be a regionally dominant contributor to black carbon (BC), primary organic aerosols (POA) and precursors for secondary organic aerosol (SOA). Recent studies suggest that SOA formed during photo-oxidation of primary emissions from biomass burning may make important contribution to its atmospheric impacts. However, the extent to which stove type and operating conditions affect the amount, composition and characteristics of SOA formed from the aging of cookstoves emissions is still largely undetermined. Here we present results from experiments with a field portable oxidation flow reactor (F-OFR) designed to assess aging of cook-stove emissions in both laboratory and field settings. Laboratory tests results are used to compare the quantity and properties of fresh and aged emissions from a traditional open fire and twp alternative stove designs operated on the standard and alternate testing protocols. Diluted cookstove emissions were exposed to a range of oxidant concentrations in the F-OFR. Primary emissions were aged both on-line, to study the influence of combustion variability, and sampled from batched emissions in a smog chamber to examine different aging conditions. Data from real-time particle- and gas-phase instruments and integrated filter samples were collected up and down stream of the OFR. The properties of primary emissions vary strongly with stove type and combustion conditions (e.g. smoldering versus flaming). Experiments aging diluted biomass emissions from distinct phases of stove operation (smoldering and flaming) showed peak SOA production for both phases occurred between 3 and 6 equivalent days of aging with slightly greater production observed in flaming phase emissions. Changing combustion conditions had a stronger influence than aging on POA+SOA `emission factors'. Aerosol Chemical Speciation Monitor data show a substantial evolution of aerosol

  6. Attribution of aerosol radiative forcing over India during the winter monsoon to emissions from source categories and geographical regions

    Science.gov (United States)

    Verma, S.; Venkataraman, C.; Boucher, O.

    2011-08-01

    We examine the aerosol radiative effects due to aerosols emitted from different emission sectors (anthropogenic and natural) and originating from different geographical regions within and outside India during the northeast (NE) Indian winter monsoon (January-March). These studies are carried out through aerosol transport simulations in the general circulation (GCM) model of the Laboratoire de Météorologie Dynamique (LMD). The model estimates of aerosol single scattering albedo (SSA) show lower values (0.86-0.92) over the region north to 10°N comprising of the Indian subcontinent, Bay of Bengal, and parts of the Arabian Sea compared to the region south to 10°N where the estimated SSA values lie in the range 0.94-0.98. The model estimated SSA is consistent with the SSA values inferred through measurements on various platforms. Aerosols of anthropogenic origin reduce the incoming solar radiation at the surface by a factor of 10-20 times the reduction due to natural aerosols. At the top-of-atmosphere (TOA), aerosols from biofuel use cause positive forcing compared to the negative forcing from fossil fuel and natural sources in correspondence with the distribution of SSA which is estimated to be the lowest (0.7-0.78) from biofuel combustion emissions. Aerosols originating from India and Africa-west Asia lead to the reduction in surface radiation (-3 to -8 W m -2) by 40-60% of the total reduction in surface radiation due to all aerosols over the Indian subcontinent and adjoining ocean. Aerosols originating from India and Africa-west Asia also lead to positive radiative effects at TOA over the Arabian Sea, central India (CNI), with the highest positive radiative effects over the Bay of Bengal and cause either negative or positive effects over the Indo-Gangetic plain (IGP).

  7. Brown carbon aerosols from burning of boreal peatlands: microphysical properties, emission factors, and implications for direct radiative forcing

    Directory of Open Access Journals (Sweden)

    R. K. Chakrabarty

    2016-03-01

    Full Text Available The surface air warming over the Arctic has been almost twice as much as the global average in recent decades. In this region, unprecedented amounts of smoldering peat fires have been identified as a major emission source of climate-warming agents. While much is known about greenhouse gas emissions from these fires, there is a knowledge gap on the nature of particulate emissions and their potential role in atmospheric warming. Here, we show that aerosols emitted from burning of Alaskan and Siberian peatlands are predominantly brown carbon (BrC – a class of visible light-absorbing organic carbon (OC – with a negligible amount of black carbon content. The mean fuel-based emission factors for OC aerosols ranged from 3.8 to 16.6 g kg−1. Their mass absorption efficiencies were in the range of 0.2–0.8 m2 g−1 at 405 nm (violet and dropped sharply to 0.03–0.07 m2 g−1 at 532 nm (green, characterized by a mean Ångström exponent of  ≈  9. Electron microscopy images of the particles revealed their morphologies to be either single sphere or agglomerated “tar balls”. The shortwave top-of-atmosphere aerosol radiative forcing per unit optical depth under clear-sky conditions was estimated as a function of surface albedo. Only over bright surfaces with albedo greater than 0.6, such as snow cover and low-level clouds, the emitted aerosols could result in a net warming (positive forcing of the atmosphere.

  8. Carbonaceous aerosols over China--review of observations, emissions, and climate forcing.

    Science.gov (United States)

    Wang, Linpeng; Zhou, Xuehua; Ma, Yujie; Cao, Zhaoyu; Wu, Ruidong; Wang, Wenxing

    2016-01-01

    Carbonaceous aerosols have been attracting attention due to the influence on visibility, air quality, and regional climate. Statistical analyses based on concentration levels, spatial-temporal variations, correlations, and organic carbon (OC) to element carbon (EC) ratios from published data of OC and EC in particulate matter (PM2.5 and PM10) were carried out in order to give a carbonaceous aerosol profile in China. The results showed maxima for OC of 29.5 ± 18.2 μg C m(-3) and for EC of 8.4 ± 6.3 μg C m(-3) in winter and minima for OC of 12.9 ± 7.7 μg C m(-3) in summer and for EC of 4.6 ± 2.8 μg C m(-3) in spring. In addition, OC and EC both had higher concentrations in urban than those in rural sites. Carbonaceous aerosol levels in China are about three to seven times higher compared to those in the USA and Europe. OC and EC occupied 20 ± 6 and 7 ± 3% of PM2.5 mass and 17 ± 7 and 5 ± 3% of PM10 mass, respectively, implying that carbonaceous aerosols are the main component of PM, especially OC. Secondary organic carbon (SOC) was a significant portion of PM and contributed 41 ± 26% to OC and 8 ± 6% to PM2.5 mass. The OC/EC ratio was 3.63 ± 1.73, which, along with the good correlation between OC and EC and the OC to EC slope of 2.29, signifies that coal combustion and/or vehicular exhaust is the dominated carbonaceous aerosol source in China. These provide a primary observation-based understanding of carbonaceous aerosol pollution in China and have a great significance in improving the emission inventory and climate forcing evaluation.

  9. Updated African biomass burning emission inventories in the framework of the AMMA-IDAF program, with an evaluation of combustion aerosols

    Directory of Open Access Journals (Sweden)

    C. Liousse

    2010-10-01

    Full Text Available African biomass burning emission inventories for gaseous and particulate species have been constructed at a resolution of 1 km by 1km with daily coverage for the 2000–2007 period. These inventories are higher than the GFED2 inventories, which are currently widely in use. Evaluation specifically focusing on combustion aerosol has been carried out with the ORISAM-TM4 global chemistry transport model which includes a detailed aerosol module. This paper compares modeled results with measurements of surface BC concentrations and scattering coefficients from the AMMA Enhanced Observations period, aerosol optical depths and single scattering albedo from AERONET sunphotometers, LIDAR vertical distributions of extinction coefficients as well as satellite data. Aerosol seasonal and interannual evolutions over the 2004–2007 period observed at regional scale and more specifically at the Djougou (Benin and Banizoumbou (Niger AMMA/IDAF sites are well reproduced by our global model, indicating that our biomass burning emission inventory appears reasonable.

  10. Arctic Aerosols and Sources

    DEFF Research Database (Denmark)

    Nielsen, Ingeborg Elbæk

    2017-01-01

    Since the Industrial Revolution, the anthropogenic emission of greenhouse gases has been increasing, leading to a rise in the global temperature. Particularly in the Arctic, climate change is having serious impact where the average temperature has increased almost twice as much as the global during......, ammonium, black carbon, and trace metals. This PhD dissertation studies Arctic aerosols and their sources, with special focus on black carbon, attempting to increase the knowledge about aerosols’ effect on the climate in an Arctic content. The first part of the dissertation examines the diversity...... of aerosol emissions from an important anthropogenic aerosol source: residential wood combustion. The second part, characterizes the chemical and physical composition of aerosols while investigating sources of aerosols in the Arctic. The main instrument used in this research has been the state...

  11. Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions

    Directory of Open Access Journals (Sweden)

    R. Ots

    2018-04-01

    Full Text Available Evidence is accumulating that emissions of primary particulate matter (PM from residential wood and coal combustion in the UK may be underestimated and/or spatially misclassified. In this study, different assumptions for the spatial distribution and total emission of PM from solid fuel (wood and coal burning in the UK were tested using an atmospheric chemical transport model. Modelled concentrations of the PM components were compared with measurements from aerosol mass spectrometers at four sites in central and Greater London (ClearfLo campaign, 2012, as well as with measurements from the UK black carbon network.The two main alternative emission scenarios modelled were Base4x and combRedist. For Base4x, officially reported PM2.5 from the residential and other non-industrial combustion source sector were increased by a factor of four. For the combRedist experiment, half of the baseline emissions from this same source were redistributed by residential population density to simulate the effect of allocating some emissions to the smoke control areas (that are assumed in the national inventory to have no emissions from this source. The Base4x scenario yielded better daily and hourly correlations with measurements than the combRedist scenario for year-long comparisons of the solid fuel organic aerosol (SFOA component at the two London sites. However, the latter scenario better captured mean measured concentrations across all four sites. A third experiment, Redist – all emissions redistributed linearly to population density, is also presented as an indicator of the maximum concentrations an assumption like this could yield.The modelled elemental carbon (EC concentrations derived from the combRedist experiments also compared well with seasonal average concentrations of black carbon observed across the network of UK sites. Together, the two model scenario simulations of SFOA and EC suggest both that residential solid fuel emissions may be higher than

  12. Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions

    Science.gov (United States)

    Ots, Riinu; Heal, Mathew R.; Young, Dominique E.; Williams, Leah R.; Allan, James D.; Nemitz, Eiko; Di Marco, Chiara; Detournay, Anais; Xu, Lu; Ng, Nga L.; Coe, Hugh; Herndon, Scott C.; Mackenzie, Ian A.; Green, David C.; Kuenen, Jeroen J. P.; Reis, Stefan; Vieno, Massimo

    2018-04-01

    Evidence is accumulating that emissions of primary particulate matter (PM) from residential wood and coal combustion in the UK may be underestimated and/or spatially misclassified. In this study, different assumptions for the spatial distribution and total emission of PM from solid fuel (wood and coal) burning in the UK were tested using an atmospheric chemical transport model. Modelled concentrations of the PM components were compared with measurements from aerosol mass spectrometers at four sites in central and Greater London (ClearfLo campaign, 2012), as well as with measurements from the UK black carbon network.The two main alternative emission scenarios modelled were Base4x and combRedist. For Base4x, officially reported PM2.5 from the residential and other non-industrial combustion source sector were increased by a factor of four. For the combRedist experiment, half of the baseline emissions from this same source were redistributed by residential population density to simulate the effect of allocating some emissions to the smoke control areas (that are assumed in the national inventory to have no emissions from this source). The Base4x scenario yielded better daily and hourly correlations with measurements than the combRedist scenario for year-long comparisons of the solid fuel organic aerosol (SFOA) component at the two London sites. However, the latter scenario better captured mean measured concentrations across all four sites. A third experiment, Redist - all emissions redistributed linearly to population density, is also presented as an indicator of the maximum concentrations an assumption like this could yield.The modelled elemental carbon (EC) concentrations derived from the combRedist experiments also compared well with seasonal average concentrations of black carbon observed across the network of UK sites. Together, the two model scenario simulations of SFOA and EC suggest both that residential solid fuel emissions may be higher than inventory

  13. Inventory of aerosol and sulphur dioxide emissions from India. Part 1 - Fossil fuel combustion

    International Nuclear Information System (INIS)

    Shekar Reddy, M.; Venkataraman, C.

    2002-01-01

    A comprehensive, spatially resolved (0.25 o x 0.25 o ) fossil fuel consumption database and emissions inventory was constructed, for India, for the first time. Emissions of sulphur dioxide and aerosol chemical constituents were estimated for 1996-1997 and extrapolated to the Indian Ocean Experiment (INDOEX) study period (1998-1999). District level consumption of coal/lignite, petroleum and natural gas in power plants, industrial, transportation and domestic sectors was 9411 PJ, with major contributions from coal (54%) followed by diesel (18%). Emission factors for various pollutants were derived using India specific fuel characteristics and information on combustion/air pollution control technologies for the power and industrial sectors. Domestic and transportation emission factors, appropriate for Indian source characteristics, were compiled from literature. SO 2 emissions from fossil fuel combustion for 1996-1997 were 4.0Tg SO 2 yr -1 , with 756 large point sources (e.g. utilities, iron and steel, fertilisers, cement, refineries and petrochemicals and non-ferrous metals), accounting for 62%. PM 2.5 emitted was 0.5 and 2.0Tgyr -1 for the 100% and the 50% control scenario, respectively, applied to coal burning in the power and industrial sectors. Coal combustion was the major source of PM 2.5 (92%) primarily consisting of fly ash, accounting for 98% of the 'inorganic fraction' emissions (difference between PM 2.5 and black carbon + organic matter) of 1.6Tgyr -1 . Black carbon emissions were estimated at 0.1Tgyr -1 , with 58% from diesel transport, and organic matter emissions at 0.3Tgyr -1 , with 48% from brick-kilns. Fossil fuel consumption and emissions peaked at the large point industrial sources and 22 cities, with elevated area fluxes in northern and western India. The spatial resolution of this inventory makes it suitable for regional-scale aerosol-climate studies. These results are compared to previous studies and differences discussed. Measurements of

  14. Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

    Science.gov (United States)

    Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

    2017-12-01

    Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

  15. Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

    Directory of Open Access Journals (Sweden)

    E. A. Marais

    2016-02-01

    Full Text Available Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA, but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS and ground-based (SOAS observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2 over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2 react significantly with both NO (high-NOx pathway and HO2 (low-NOx pathway, leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA and formaldehyde (a product of isoprene oxidation. Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA from the low-NOx pathway and glyoxal (28 % from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation, but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume. The US Environmental Protection Agency (EPA projects 2013–2025 decreases in

  16. Assessment of Biomass Burning Smoke Influence on Environmental Conditions for Multi-Year Tornado Outbreaks by Combining Aerosol-Aware Microphysics and Fire Emission Constraints

    Science.gov (United States)

    Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; Da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

    2016-01-01

    We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRFChem for its use in applications such as NWP and cloud-resolving simulations.

  17. Aerosols from biomass combustion

    Energy Technology Data Exchange (ETDEWEB)

    Nussbaumer, T

    2001-07-01

    This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

  18. Aerosols from biomass combustion

    Energy Technology Data Exchange (ETDEWEB)

    Nussbaumer, T.

    2001-07-01

    This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

  19. Mechanism of negative hydrogen ion emission from heated saline hydrides

    Energy Technology Data Exchange (ETDEWEB)

    Kawano, Hiroyuki; Serizawa, Naoshi; Takeda, Makiko; Hasegawa, Seiji [Ehime Univ., Matsuyama (Japan). Faculty of Science

    1997-02-01

    To find a clue to the mechanism of negative hydrogen ion emission from a heated sample ({approx}10 mg) of powdery saline hydride (LiH or CaH{sub 2}) deposited on a molybdenum ribbon ({approx}0.1 cm{sup 2}), both the ionic and electronic emission currents were measured as a function of sample temperature ({approx}700 - 800 K), thereby yielding {approx}10{sup -15} - 10{sup -12} A of H{sup -} after mass analysis and {approx}10{sup -7} - 10{sup -5} A of thermal electron. Thermophysical analysis of these data indicates that the desorption energy (E{sup -}) of H{sup -} and work function ({phi}) of the emitting sample surface are 5.1 {+-} 0.3 and 3.1 {+-} 0.2 eV for LiH, respectively, while E{sup -} is 7.7 {+-} 0.3 eV and {phi} is 5.0 {+-} 0.2 eV for CaH{sub 2}. Thermochemical analysis based on our simple model on the emissions indicates that the values of E{sup -} - {phi} are 2.35 and 2.31 eV for LiH and CaH{sub 2}, respectively, which are in fair agreement with the respective values (2.1 {+-} 0.3 and 2.6 {+-} 0.3 eV) determined experimentally. This agreement indicates that the emission of H{sup -} is reasonably explained by our model from the viewpoint of reaction energy. (author)

  20. Modeling and Evaluation of the Global Sea-Salt Aerosol Distribution: Sensitivity to Emission Schemes and Resolution Effects at Coastal/Orographic Sites

    Science.gov (United States)

    Spada, M.; Jorba, O.; Perez Garcia-Pando, C.; Janjic, Z.; Baldasano, J. M.

    2013-01-01

    One of the major sources of uncertainty in model estimates of the global sea-salt aerosol distribution is the emission parameterization. We evaluate a new sea-salt aerosol life cycle module coupled to the online multi-scale chemical transport model NMMB/BSC-CTM. We compare 5 year global simulations using five state-of-the-art sea-salt open-ocean emission schemes with monthly averaged coarse aerosol optical depth (AOD) from selected AERONET sun photometers, surface concentration measurements from the University of Miami's Ocean Aerosol Network, and measurements from two NOAA/PMEL cruises (AEROINDOEX and ACE1). Model results are highly sensitive to the introduction of sea-surface-temperature (SST)-dependent emissions and to the accounting of spume particles production. Emission ranges from 3888 teragrams per year to 8114 teragrams per year, lifetime varies between 7.3 hours and 11.3 hours, and the average column mass load is between 5.0 teragrams and 7.2 teragrams. Coarse AOD is reproduced with an overall correlation of around 0.5 and with normalized biases ranging from +8.8 percent to +38.8 percent. Surface concentration is simulated with normalized biases ranging from minus 9.5 percent to plus 28 percent and the overall correlation is around 0.5. Our results indicate that SST-dependent emission schemes improve the overall model performance in reproducing surface concentrations. On the other hand, they lead to an overestimation of the coarse AOD at tropical latitudes, although it may be affected by uncertainties in the comparison due to the use of all-sky model AOD, the treatment of water uptake, deposition and optical properties in the model and/or an inaccurate size distribution at emission.

  1. Emissions of Black Carbon, Organic, and Inorganic Aerosols From Biomass Burning in North America and Asia in 2008

    Science.gov (United States)

    Kondo, Y.; Matsui, H.; Moteki, N.; Sahu, L.; Takegawa, N.; Kajino, M.; Zhao, Y.; Cubison, M. J.; Jimenez, J. L.; Vay, S.; hide

    2011-01-01

    Reliable assessment of the impact of aerosols emitted from boreal forest fires on the Arctic climate necessitates improved understanding of emissions and the microphysical properties of carbonaceous (black carbon (BC) and organic aerosols (OA)) and inorganic aerosols. The size distributions of BC were measured by an SP2 based on the laser-induced incandescence technique on board the DC-8 aircraft during the NASA ARCTAS campaign. Aircraft sampling was made in fresh plumes strongly impacted by wildfires in North America (Canada and California) in summer 2008 and in those transported from Asia (Siberia in Russia and Kazakhstan) in spring 2008. We extracted biomass burning plumes using particle and tracer (CO, CH3CN, and CH2Cl2) data. OA constituted the dominant fraction of aerosols mass in the submicron range. The large majority of the emitted particles did not contain BC. We related the combustion phase of the fire as represented by the modified combustion efficiency (MCE) to the emission ratios between BC and other species. In particular, we derived the average emission ratios of BC/CO = 2.3 +/- 2.2 and 8.5 +/- 5.4 ng/cu m/ppbv for BB in North America and Asia, respectively. The difference in the BC/CO emission ratios is likely due to the difference in MCE. The count median diameters and geometric standard deviations of the lognormal size distribution of BC in the BB plumes were 136-141 nm and 1.32-1.36, respectively, and depended little on MCE. These BC particles were thickly coated, with shell/core ratios of 1.3-1.6. These parameters can be used directly for improving model estimates of the impact of BB in the Arctic.

  2. Monsoon sensitivity to aerosol direct radiative forcing in the ...

    Indian Academy of Sciences (India)

    to the total, scattering aerosols and black carbon aerosols. ... acts as an internal damping mechanism spinning down the regional hydrological cycle and leading to sig- ... tion and emission of longwave radiation. ... effect of aerosols over India, where the emission of .... that aerosol effects on monsoon water cycle dynam-.

  3. Long term atmospheric aerosol characterization in the Amazon Basin

    Science.gov (United States)

    Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

    This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

  4. The Emissions of Carbon Dioxide, Methane, and Nitrous Oxide during Winter without Cultivation in Local Saline-Alkali Rice and Maize Fields in Northeast China

    Directory of Open Access Journals (Sweden)

    Hao Zhang

    2017-10-01

    Full Text Available Agricultural ecosystems are important contributors to atmospheric greenhouse gasses (GHGs; however, in situ winter emission data in saline-alkali fields are scarce. Gas samples were collected during different periods, from three rice (R1–R3 and three maize (M1–M3 fields with different soil pH levels and salinity conditions. Carbon dioxide (CO2 emissions in the rice and maize fields decreased with decreasing temperature during the freezing period and increased with the rising temperature during the thawing period, with the majority of winter CO2 emissions occurring during these two periods. Peaks in methane (CH4 emissions were observed during the freezing period in the rice fields and during the snow-melting period in the rice and maize fields. CH4 emissions in the rice fields and CH4 uptake rates in the maize fields were significantly (P < 0.05 related to surface soil temperature. Nitrous oxide (N2O emissions remained relatively low, except for during the peaks observed during the snow-melting period in both the rice and maize fields, leading to the high GHG contribution of the snow-melting period throughout the winter. Higher pH and salinity conditions consistently resulted in lower CO2, CH4, and N2O emissions, CH4 uptake, and lower global warming potential (GWP. These results can contribute to the assessment of the GWP during winter in saline-alkali regions.

  5. Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols. Part 1; Aerosol Trends and Radiative Forcing

    Science.gov (United States)

    Leibensperger, E. M.; Mickley, L. J.; Jacob, D. J.; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.

    2012-01-01

    We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of -2.0Wm(exp-2 for direct forcing including contributions from sulfate (-2.0Wm-2), nitrate (-0.2Wm(exp-2), organic carbon (-0.2Wm(exp-2), and black carbon (+0.4Wm(exp-2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp-2) direct and 1.0Wm(exp-2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp-2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

  6. Study of emission episodes of urban aerosol by ion beam analytical techniques

    International Nuclear Information System (INIS)

    Angyal, A.; Kertesz, Zs.; Szikszai, Z.; Szoboszlai, Z.; Furu, E.; Csedreki, L.; Daroczi, L.

    2010-01-01

    Complete text of publication follows. Aerosol pollution has impact on the climate and on human health. Thus investigation of atmospheric aerosol is important in urban environment such as Debrecen. One of the main goals of our study was to define the sources of the particles. The hourly evolution of atmospheric aerosol concentration was used to identify sources of fine (aerodynamic diameter < 2,5 μm) and coarse (10 μm ≥ aerodynamic diameter ≥ 2.5 μm) urban particulate matter in Debrecen. In both size fractions sources were found which were characterized by high heavy metal content. In this study we provide accurate information of the sources of coarse mode heavy metals by using nuclear and scanning electron microscopy. Single particle analysis of chosen samples was carried out on the ATOMKI Scanning Nuclear Microprobe Facility. Elemental composition for Z ≥ 6, morphology and size of around 500 coarse mode particles were determined by Scanning Transmission Ion Microscopy, light-element PIXE and PIXE analytical methods. Furthermore Scanning Electron Microscopy (SEM) was used to investigate particles morphology. The main components of the particles were Na, K, Ca, S, P and Fe with traces of Ti, V, Cr, Mn, Ni, Cu, Zn, Co, Pb. S-rich particles were enriched in one or more of the following elements: Na, Ca, K, Fe, Zn. Trace metals (Mn, Cu, Zn, Cr) occurred together Fe supposedly originated from industrial emission or traffic. P appeared in the Ca-rich particles. Particles with high concentration of Ni were rich in V, Fe and S. Thus this source was identified as residual combustion. V-rich particles occurred together with Fe, Mn and Cr. Their possible source was industry. Pb was attached to Ca, Fe, S containing particles. As result of the SEM study the following particle types (Figure 1.) were identified: semitransparent material (S-K-rich, S-Zn-rich, PCa-rich), spherical (FeO, Fe-Ni-Cr-V-rich), cubic (KCl, CaCl) and crystalline (S-Ca-rich). The main sources of

  7. Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

    Directory of Open Access Journals (Sweden)

    J. Zábori

    2012-11-01

    Full Text Available Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known.

    In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity, and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1°C and 9°C. Aerosol number concentrations decreased from at least 1400 cm−3 to 350 cm−3. In general, the aerosol number size distribution exhibited a robust shape with one mode close to dry diameter Dp 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.

  8. Temperature and burning history affect emissions of greenhouse gases and aerosol particles from tropical peatland fire

    Science.gov (United States)

    Kuwata, Mikinori; Kai, Fuu Ming; Yang, Liudongqing; Itoh, Masayuki; Gunawan, Haris; Harvey, Charles F.

    2017-01-01

    Tropical peatland burning in Asia has been intensifying over the last decades, emitting huge amounts of gas species and aerosol particles. Both laboratory and field studies have been conducted to investigate emission from peat burning, yet a significant variability in data still exists. We conducted a series of experiments to characterize the gas and particulate matter emitted during burning of a peat sample from Sumatra in Indonesia. Heating temperature of peat was found to regulate the ratio of CH4 to CO2 in emissions (ΔCH4/ΔCO2) as well as the chemical composition of particulate matter. The ΔCH4/ΔCO2 ratio was larger for higher temperatures, meaning that CH4 emission is more pronounced at these conditions. Mass spectrometric analysis of organic components indicated that aerosol particles emitted at higher temperatures had more unsaturated bonds and ring structures than that emitted from cooler fires. The result was consistently confirmed by nuclear magnetic resonance analysis. In addition, CH4 emitted by burning charcoal, which is derived from previously burned peat, was lower by at least an order of magnitude than that from fresh peat. These results highlight the importance of both fire history and heating temperature for the composition of tropical peat-fire emissions. They suggest that remote sensing technologies that map fire histories and temperatures could provide improved estimates of emissions.

  9. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

    2013-05-10

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  10. Time evolution and emission factors of aerosol particles from day and night time savannah fires

    Science.gov (United States)

    Vakkari, Ville; Beukes, Johan Paul; Tiitta, Petri; Venter, Andrew; Jaars, Kerneels; Josipovic, Miroslav; van Zyl, Pieter; Kulmala, Markku; Laakso, Lauri

    2013-04-01

    The largest uncertainties in the current global climate models originate from aerosol particle effects (IPCC, 2007) and at the same time aerosol particles also pose a threat to human health (Pope and Dockery, 2006). In southern Africa wild fires and prescribed burning are one of the most important sources of aerosol particles, especially during the dry season from June to September (e.g. Swap et al., 2003; Vakkari et al., 2012). The aerosol particle emissions from savannah fires in southern Africa have been studied in several intensive campaigns such as SAFARI 1992 and 2000 (Swap et al., 2003). However, all previous measurements have been carried out during the daytime, whereas most of the prescribed fires in southern Africa are lit up only after sunset. Furthermore, the previous campaigns followed the plume evolution for up to one hour after emission only. In this study, combining remote sensing fire observations to ground-based long-term measurements of aerosol particle and trace gas properties at the Welgegund measurement station (www.welgegund.org), we have been able to follow the time evolution of savannah fire plumes up to several hours in the atmosphere. For the first time the aerosol particle size distribution measurements in savannah fire plumes cover both day and night time plumes and also the ultrafine size range below 100 nm. During the period from May 20th 2010 to April 15th 2012 altogether 61 savannah fire plumes were observed at Welgegund. The evolution of the aerosol size distribution remained rapid for at least five hours after the fire: during this period the growth rate of the aerosol particle count mean diameter (size range 12 to 840 nm) was 24 nm h-1 for daytime plumes and 8 nm h-1 for night time plumes. The difference in the day and night time growth rate shows that photochemical reactions significantly increase the condensable vapour concentration in the plume. Furthermore, the condensable vapour concentration was found to affect both the

  11. Secondary organic aerosol formation from road vehicle emissions

    Science.gov (United States)

    Pieber, Simone M.; Platt, Stephen M.; El Haddad, Imad; Zardini, Alessandro A.; Suarez-Bertoa, Ricardo; Slowik, Jay G.; Huang, Ru-Jin; Hellebust, Stig; Temime-Roussel, Brice; Marchand, Nicolas; Drinovec, Luca; Mocnik, Grisa; Baltensperger, Urs; Astorga, Covadogna; Prévôt, André S. H.

    2014-05-01

    Organic aerosol particles (OA) are a major fraction of the submicron particulate matter. OA consists of directly emitted primary (POA) and secondary OA (SOA). SOA is formed in-situ in the atmosphere via the reaction of volatile organic precursors. The partitioning of SOA species depends not only on the exposure to oxidants, but for instance also on temperature, relative humidity (RH), and the absorptive mass chemical composition (presence of inorganics) and concentration. Vehicle exhaust is a known source of POA and likely contributes to SOA formation in urban areas [1;2]. This has recently been estimated by (i) analyzing ambient data from urban areas combined with fuel consumption data [3], (ii) by examining the chemical composition of raw fuels [4], or (iii) smog chamber studies [5, 6]. Contradictory and thus somewhat controversial results in the relative quantity of SOA from diesel vs. gasoline vehicle exhaust were observed. In order to elucidate the impact of variable ambient conditions on the potential SOA formation of vehicle exhaust, and its relation to the emitted gas phase species, we studied SOA formed from the exhaust of passenger cars and trucks as a function of fuel and engine type (gasoline, diesel) at different temperatures (T 22 vs. -7oC) and RH (40 vs. 90%), as well as with different levels of inorganic salt concentrations. The exhaust was sampled at the tailpipe during regulatory driving cycles on chassis dynamometers, diluted (200 - 400x) and introduced into the PSI mobile smog chamber [6], where the emissions were subjected to simulated atmospheric ageing. Particle phase instruments (HR-ToF-AMS, aethalometers, CPC, SMPS) and gas phase instruments (PTR-TOF-MS, CO, CO2, CH4, THC, NH3 and other gases) were used online during the experiments. We found that gasoline emissions, because of cold starts, were generally larger than diesel, especially during cold temperatures driving cycles. Gasoline vehicles also showed the highest SOA formation

  12. Secondary Organic Aerosol Production from Gasoline Vehicle Exhaust: Effects of Engine Technology, Cold Start, and Emission Certification Standard.

    Science.gov (United States)

    Zhao, Yunliang; Lambe, Andrew T; Saleh, Rawad; Saliba, Georges; Robinson, Allen L

    2018-02-06

    Secondary organic aerosol (SOA) formation from dilute exhaust from 16 gasoline vehicles was investigated using a potential aerosol mass (PAM) oxidation flow reactor during chassis dynamometer testing using the cold-start unified cycle (UC). Ten vehicles were equipped with gasoline direct injection engines (GDI vehicles) and six with port fuel injection engines (PFI vehicles) certified to a wide range of emissions standards. We measured similar SOA production from GDI and PFI vehicles certified to the same emissions standard; less SOA production from vehicles certified to stricter emissions standards; and, after accounting for differences in gas-particle partitioning, similar effective SOA yields across different engine technologies and certification standards. Therefore the ongoing, dramatic shift from PFI to GDI vehicles in the United States should not alter the contribution of gasoline vehicles to ambient SOA and the natural replacement of older vehicles with newer ones certified to stricter emissions standards should reduce atmospheric SOA levels. Compared to hot operations, cold-start exhaust had lower effective SOA yields, but still contributed more SOA overall because of substantially higher organic gas emissions. We demonstrate that the PAM reactor can be used as a screening tool for vehicle SOA production by carefully accounting for the effects of the large variations in emission rates.

  13. Long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometer

    Science.gov (United States)

    Xu, J.; Zhang, X.; Liu, Y.; Shichang, K.; Ma, Y.

    2017-12-01

    An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize high time-resolved submicron particulate matter (PM1) and obtain the influence of biomass burning emissions to the Himalayas, frequently transported from south Asia during pre-monsoon season. Two high aerosol loading periods were observed during the study. Overall, the average (± 1σ) PM1 mass concentration was 4.44 (± 4.54) µg m-3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosols (OA) was the dominant PM1 species (accounting for 54.3% of total PM1 mass on average) and its contribution increased with the increase of total PM1 mass loading. The average size distributions of PM1 species all peaked at an overlapping accumulation mode ( 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportations. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a biomass burning related OA (BBOA, 43.7%) and two oxygenated OA (Local-OOA and LRT-OOA; 13.9% and 42.4%) represented sources from local emissions and long-range transportations, respectively. Two polluted air mass origins (generally from the west and southwest of QOMS) and two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions were observed, respectively, suggesting the important sources of wildfires from south Asia. One of polluted aerosol plumes was investigated in detail to illustrate the evolution of aerosol characteristics at QOMS driving by different impacts of wildfires, air mass origins, meteorological conditions and

  14. Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

    Science.gov (United States)

    Persad, Geeta Gayatri

    Short-lived anthropogenic aerosols are concentrated in regions of high human activity, where they interact with radiation and clouds, causing horizontally heterogeneous radiative forcing between polluted and unpolluted regions. Aerosols can absorb shortwave energy in the atmosphere, but deplete it at the surface, producing opposite radiative perturbations between the surface and atmosphere. This thesis investigates climate and policy implications of this horizontal and vertical heterogeneity of anthropogenic aerosol forcing, employing the Geophysical Fluid Dynamics Laboratory's AM2.1 and AM3 models, both at a global scale and using East Asia as a regional case study. The degree of difference between spatial patterns of climate change due to heterogeneous aerosol forcing versus homogeneous greenhouse gas forcing deeply impacts the detection, attribution, and prediction of regional climate change. This dissertation addresses a gap in current understanding of these two forcings' response pattern development, using AM2.1 historical forcing simulations. The results indicate that fast atmospheric and land-surface processes alone substantially homogenize the global pattern of surface energy flux response to heterogeneous aerosol forcing. Aerosols' vertical redistribution of energy significantly impacts regional climate, but is incompletely understood. It is newly identified here, via observations and historical and idealized forcing simulations, that increased aerosol-driven atmospheric absorption may explain half of East Asia's recent surface insolation decline. Further, aerosols' surface and atmospheric effects counteract each other regionally---atmospheric heating enhances summer monsoon circulation, while surface dimming suppresses it---but absorbing aerosols' combined effects reduce summer monsoon rainfall. This thesis constitutes the first vertical decomposition of aerosols' impacts in this high-emissions region and elucidates the monsoonal response to aerosols

  15. Temporal variability in aerosol characteristics and its radiative properties over Patiala, northwestern part of India: Impact of agricultural biomass burning emissions.

    Science.gov (United States)

    Sharma, D; Srivastava, A K; Ram, K; Singh, A; Singh, D

    2017-12-01

    A comprehensive measurements of aerosol optical depth (AOD), particulate matter (PM) and black carbon (BC) mass concentrations have been carried out over Patiala, a semi-urban site in northwest India during October 2008 to September 2010. The measured aerosol data was incorporated in an aerosol optical model to estimate various aerosol optical parameters, which were subsequently used for radiative forcing estimation. The measured AOD at 500 nm (AOD 500 ) shows a significant seasonal variability, with maximum value of 0.81 during post-monsoon (PoM) and minimum of 0.56 during winter season. The Ångström exponent (α) has higher values (i.e. more fine-mode fraction) during the PoM/winter periods, and lower (i.e. more coarse-mode fraction) during pre-monsoon (PrM). In contrast, turbidity coefficient (β) exhibits an opposite trend to α during the study period. BC mass concentration varies from 2.8 to 13.9 μg m -3 (mean: 6.5 ± 3.2 μg m -3 ) during the entire study period, with higher concentrations during PoM/winter and lower during PrM/monsoon seasons. The average single scattering albedo (SSA at 500 nm) values are 0.70, 0.72, 0.82 and 0.75 during PoM, winter, PrM and monsoon seasons, respectively. However, inter-seasonal and inter-annual variability in measured aerosol parameters are statistically insignificant at Patiala. These results suggest strong changes in emission sources, aerosol composition, meteorological parameters as well as transport of aerosols over the station. Higher values of AOD, α and BC, along with lower SSA during PoM season are attributed to agriculture biomass burning emissions over and around the station. The estimated aerosol radiative forcing within the atmosphere is positive (i.e. warming) during all the seasons with higher values (∼60 Wm -2 ) during PoM-08/PoM-09 and lower (∼40 Wm -2 ) during winter-09/PrM-10. The present study highlights the role of BC aerosols from agricultural biomass burning emissions during post

  16. Impact of Emissions and Long-Range Transport on Multi-Decadal Aerosol Trends: Implications for Air Quality and Climate

    Science.gov (United States)

    Chin, Mian

    2012-01-01

    We present a global model analysis of the impact of long-range transport and anthropogenic emissions on the aerosol trends in the major pollution regions in the northern hemisphere and in the Arctic in the past three decades. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze the multi-spatial and temporal scale data, including observations from Terra, Aqua, and CALIPSO satellites and from the long-term surface monitoring stations. We will analyze the source attribution (SA) and source-receptor (SR) relationships in North America, Europe, East Asia, South Asia, and the Arctic at the surface and free troposphere and establish the quantitative linkages between emissions from different source regions. We will discuss the implications for regional air quality and climate change.

  17. Impact of anthropogenic emissions and open biomass burning on regional carbonaceous aerosols in South China

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Gan, E-mail: zhanggan@gig.ac.c [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Li Jun [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Li Xiangdong [Department of Civil and Structural Engineering, Hong Kong Polytechnic University, Hung Hom, Kowloon (Hong Kong); Xu Yue; Guo Lingli [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Tang Jianhui [Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003 (China); Lee, Celine S.L. [Department of Civil and Structural Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon (Hong Kong); Liu Xiang [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Chen Yingjun [Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003 (China)

    2010-11-15

    Carbonaceous aerosols were studied at three background sites in south and southwest China. Hok Tsui in Hong Kong had the highest concentrations of carbonaceous aerosols (OC = 8.7 {+-} 4.5 {mu}g/m{sup 3}, EC = 2.5 {+-} 1.9 {mu}g/m{sup 3}) among the three sites, and Jianfeng Mountains in Hainan Island (OC = 5.8 {+-} 2.6 {mu}g/m{sup 3}, EC = 0.8 {+-} 0.4 {mu}g/m{sup 3}) and Tengchong mountain over the east edge of the Tibetan Plateau (OC = 4.8 {+-} 4.0 {mu}g/m{sup 3}, EC = 0.5 {+-} 0.4 {mu}g/m{sup 3}) showed similar concentration levels. Distinct seasonal patterns with higher concentrations during the winter, and lower concentrations during the summertime were observed, which may be caused by the changes of the regional emissions, and monsoon effects. The industrial and vehicular emissions in East, Southeast and South China, and the regional open biomass burning in the Indo-Myanmar region of Asia were probably the two major potential sources for carbonaceous matters in this region. - Anthropogenic emissions in China and open biomass burning in the Indo-Myanmar region were the two major potential sources for carbonaceous matters in South China region.

  18. The possible influence of volcanic emissions on atmospheric aerosols in the city of Colima, Mexico

    International Nuclear Information System (INIS)

    Miranda, Javier; Zepeda, Francisco; Galindo, Ignacio

    2004-01-01

    An elemental composition study of atmospheric aerosols from the City of Colima, in the Western Coast of Mexico, is presented. Samples of PM 15 -PM 2.5 and PM 2.5 were collected with Stacked Filter Units (SFU) of the Davis design, in urban and rural sites, the latter located between the City of Colima and the Volcan de Colima, an active volcano. Elemental analyses were carried out using Particle Induced X-ray Emission (PIXE). The gravimetric mass concentrations for the fine fraction were slightly higher in the urban site, while the mean concentrations in the coarse fraction were equal within the uncertainties. High Cl contents were determined in the coarse fraction, a fact also observed in emissions from the Volcan de Colima by other authors. In addition to average elemental concentrations, cluster analysis based on elemental contents was performed, with wind speed and direction data, showing that there is an industrial contributor to aerosols North of the urban area. Moreover, a contribution from the volcanic emissions was identified from the grouping of S, Cl, Cu, and Zn, elements associated to particles emitted by the Volcan de Colima. - Elemental analyses of PM 15 in the City of Colima, Mexico, were done to identify possible contributions from the Volcan de Colima, an active volcano

  19. Impact of anthropogenic emissions and open biomass burning on regional carbonaceous aerosols in South China

    International Nuclear Information System (INIS)

    Zhang Gan; Li Jun; Li Xiangdong; Xu Yue; Guo Lingli; Tang Jianhui; Lee, Celine S.L.; Liu Xiang; Chen Yingjun

    2010-01-01

    Carbonaceous aerosols were studied at three background sites in south and southwest China. Hok Tsui in Hong Kong had the highest concentrations of carbonaceous aerosols (OC = 8.7 ± 4.5 μg/m 3 , EC = 2.5 ± 1.9 μg/m 3 ) among the three sites, and Jianfeng Mountains in Hainan Island (OC = 5.8 ± 2.6 μg/m 3 , EC = 0.8 ± 0.4 μg/m 3 ) and Tengchong mountain over the east edge of the Tibetan Plateau (OC = 4.8 ± 4.0 μg/m 3 , EC = 0.5 ± 0.4 μg/m 3 ) showed similar concentration levels. Distinct seasonal patterns with higher concentrations during the winter, and lower concentrations during the summertime were observed, which may be caused by the changes of the regional emissions, and monsoon effects. The industrial and vehicular emissions in East, Southeast and South China, and the regional open biomass burning in the Indo-Myanmar region of Asia were probably the two major potential sources for carbonaceous matters in this region. - Anthropogenic emissions in China and open biomass burning in the Indo-Myanmar region were the two major potential sources for carbonaceous matters in South China region.

  20. Temporal variability in aerosol characteristics and its radiative properties over Patiala, northwestern part of India: Impact of agricultural biomass burning emissions

    International Nuclear Information System (INIS)

    Sharma, D.; Srivastava, A.K.; Ram, K.; Singh, A.; Singh, D.

    2017-01-01

    A comprehensive measurements of aerosol optical depth (AOD), particulate matter (PM) and black carbon (BC) mass concentrations have been carried out over Patiala, a semi-urban site in northwest India during October 2008 to September 2010. The measured aerosol data was incorporated in an aerosol optical model to estimate various aerosol optical parameters, which were subsequently used for radiative forcing estimation. The measured AOD at 500 nm (AOD 500 ) shows a significant seasonal variability, with maximum value of 0.81 during post-monsoon (PoM) and minimum of 0.56 during winter season. The Ångström exponent (α) has higher values (i.e. more fine-mode fraction) during the PoM/winter periods, and lower (i.e. more coarse-mode fraction) during pre-monsoon (PrM). In contrast, turbidity coefficient (β) exhibits an opposite trend to α during the study period. BC mass concentration varies from 2.8 to 13.9 μg m −3 (mean: 6.5 ± 3.2 μg m −3 ) during the entire study period, with higher concentrations during PoM/winter and lower during PrM/monsoon seasons. The average single scattering albedo (SSA at 500 nm) values are 0.70, 0.72, 0.82 and 0.75 during PoM, winter, PrM and monsoon seasons, respectively. However, inter-seasonal and inter-annual variability in measured aerosol parameters are statistically insignificant at Patiala. These results suggest strong changes in emission sources, aerosol composition, meteorological parameters as well as transport of aerosols over the station. Higher values of AOD, α and BC, along with lower SSA during PoM season are attributed to agriculture biomass burning emissions over and around the station. The estimated aerosol radiative forcing within the atmosphere is positive (i.e. warming) during all the seasons with higher values (∼60 Wm −2 ) during PoM–08/PoM–09 and lower (∼40 Wm −2 ) during winter–09/PrM–10. The present study highlights the role of BC aerosols from agricultural biomass burning

  1. Climatic effects of 1950–2050 changes in US anthropogenic aerosols – Part 1: Aerosol trends and radiative forcing

    Directory of Open Access Journals (Sweden)

    D. G. Streets

    2012-04-01

    Full Text Available We calculate decadal aerosol direct and indirect (warm cloud radiative forcings from US anthropogenic sources over the 1950–2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970–1990, with values over the eastern US (east of 100° W of −2.0 W m−2 for direct forcing including contributions from sulfate (−2.0 W m−2, nitrate (−0.2 W m−2, organic carbon (−0.2 W m−2, and black carbon (+0.4 W m−2. The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50%. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m−2 indirect, mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3 W m−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide suggests that a US emission control strategy focused on BC would have only limited climate benefit.

  2. Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

    Directory of Open Access Journals (Sweden)

    S. Guo

    2013-08-01

    Full Text Available To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m−3 and 64.3 ± 36.2 μg m−3 (average ± standard deviation, below as the same at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance model and secondary organic aerosol (SOA tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

  3. Field study of a Brownian Demister Unit to reduce aerosol based emission from a Post Combustion CO2 Capture plant

    NARCIS (Netherlands)

    Khakharia, P.M.; Kvamsdal, H.M.; Da Silva, E.F.; Vlugt, T.J.H.; Goetheer, E.L.V.

    2014-01-01

    Emission of solvent and its degradation products from a typical absorption-desorption based Post Combustion CO2 Capture (PCCC) process is inevitable and thus, an area of growing concern. Recently, it has been pointed out that emissions can also occur by means of aerosol droplets. Conventional

  4. The primary volcanic aerosol emission from Mt Etna: Size-resolved particles with SO2 and role in plume reactive halogen chemistry

    Science.gov (United States)

    Roberts, T. J.; Vignelles, D.; Liuzzo, M.; Giudice, G.; Aiuppa, A.; Coltelli, M.; Salerno, G.; Chartier, M.; Couté, B.; Berthet, G.; Lurton, T.; Dulac, F.; Renard, J.-B.

    2018-02-01

    Volcanoes are an important source of aerosols to the troposphere. Within minutes after emission, volcanic plume aerosol catalyses conversion of co-emitted HBr, HCl into highly reactive halogens (e.g. BrO, OClO) through chemical cycles that cause substantial ozone depletion in the dispersing downwind plume. This study quantifies the sub-to-supramicron primary volcanic aerosol emission (0.2-5 μm diameter) and its role in this process. An in-situ ground-based study at Mt Etna (Italy) during passive degassing co-deployed an optical particle counter and Multi-Gas SO2 sensors at high time resolution (0.1 Hz) enabling to characterise the aerosol number, size-distribution and emission flux. A tri-modal volcanic aerosol size distribution was found, to which lognormal distributions are fitted. Total particle volume correlates to SO2 (as a plume tracer). The measured particle volume:SO2 ratio equates to a sulfate:SO2 ratio of 1-2% at the observed meteorological conditions (40% Relative Humidity). A particle mass flux of 0.7 kg s-1 is calculated for the measured Mt Etna SO2 flux of 1950 tonnes/day. A numerical plume atmospheric chemistry model is used to simulate the role of the hygroscopic primary aerosol surface area and its humidity dependence on volcanic plume BrO and OClO chemistry. As well as predicting volcanic BrO formation and O3 depletion, the model achieves OClO/SO2 in broad quantitative agreement with recently reported Mt Etna observations, with a predicted maximum a few minutes downwind. In addition to humidity - that enhances aerosols surface area for halogen cycling - background ozone is predicted to be an important control on OClO/SO2. Dependence of BrO/SO2 on ambient humidity is rather low near-to-source but increases further downwind. The model plume chemistry also exhibits strong across-plume spatial variations between plume edge and centre.

  5. Will Aerosol Hygroscopicity Change with Biodiesel, Renewable Diesel Fuels and Emission Control Technologies?

    Science.gov (United States)

    Vu, Diep; Short, Daniel; Karavalakis, Georgios; Durbin, Thomas D; Asa-Awuku, Akua

    2017-02-07

    The use of biodiesel and renewable diesel fuels in compression ignition engines and aftertreatment technologies may affect vehicle exhaust emissions. In this study two 2012 light-duty vehicles equipped with direct injection diesel engines, diesel oxidation catalyst (DOC), diesel particulate filter (DPF), and selective catalytic reduction (SCR) were tested on a chassis dynamometer. One vehicle was tested over the Federal Test Procedure (FTP) cycle on seven biodiesel and renewable diesel fuel blends. Both vehicles were exercised over double Environmental Protection Agency (EPA) Highway fuel economy test (HWFET) cycles on ultralow sulfur diesel (ULSD) and a soy-based biodiesel blend to investigate the aerosol hygroscopicity during the regeneration of the DPF. Overall, the apparent hygroscopicity of emissions during nonregeneration events is consistently low (κ diesel vehicles. As such, the contribution of regeneration emissions from a growing fleet of diesel vehicles will be important.

  6. Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

    Science.gov (United States)

    Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

  7. Plutonium-aerosol emission rates and human pulmonary deposition calculations for Nuclear Site 201, Nevada Test Site

    International Nuclear Information System (INIS)

    Shinn, J.H.; Homan, D.N.

    1982-01-01

    This study determined the plutonium-aerosol fluxes from the soil to quantify (1) the extent of potential human exposure by deep-lung retention of alpha-emitting particles; (2) the source term should there be any significant, long-term, transport of plutonium aerosols; and (3) the resuspension factor and rate so that, for the first time at any nuclear site, one may calculate how long it will take for wind erosion to carry away a significant amount of the contaminated soil. High-volume air samplers and cascade impactors were used to characterize the plutonium aerosols. Meteorological flux-profile methods were used to calculate dust and plutonium aerosol emission rates. A floorless wind tunnel (10-m long) was used to examine resuspension under steady-state, high wind speed. The resuspension factor was two orders of magnitude lower than the other comparable sites at NTS and elsewhere, and the average resuspension rate of 5.3 x 10 -8 /d was also very low, so that the half-time for resuspension by wind erosion was about 36,000 y

  8. Aerosol composition and source apportionment in Santiago de Chile

    Science.gov (United States)

    Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

    1999-04-01

    Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dpsource apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.

  9. Determination of light elements concentration in aerosols by X emission induced by deuteron

    International Nuclear Information System (INIS)

    Morales, J.R.; Romo, C.

    1983-01-01

    Absolute concentrations for Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe and Cu were obtained in the range from 10 ng/m 3 to 10 4 ng/m 3 in aerosols from Santiago. A 4,2 MeV deuteron beam was used to induce characteristic X-ray emission. It was found that relative abundance of these elements is maintained for days of high and low total suspended particulates. (Author)

  10. Polar and non-polar organic aerosols from large-scale agricultural-waste burning emissions in Northern India: Implications to organic mass-to-organic carbon ratio.

    Science.gov (United States)

    Rajput, Prashant; Sarin, M M

    2014-05-01

    This study focuses on characteristics of organic aerosols (polar and non-polar) and total organic mass-to-organic carbon ratio (OM/OC) from post-harvest agricultural-waste (paddy- and wheat-residue) burning emissions in Northern India. Aerosol samples from an upwind location (Patiala: 30.2°N, 76.3°E) in the Indo-Gangetic Plain were analyzed for non-polar and polar fractions of organic carbon (OC1 and OC2) and their respective mass (OM1 and OM2). On average, polar organic aerosols (OM2) contribute nearly 85% of the total organic mass (OM) from the paddy- and wheat-residue burning emissions. The water-soluble-OC (WSOC) to OC2 ratio, within the analytical uncertainty, is close to 1 from both paddy- and wheat-residue burning emissions. However, temporal variability and relatively low WSOC/OC2 ratio (Av: 0.67±0.06) is attributed to high moisture content and poor combustion efficiency during paddy-residue burning, indicating significant contribution (∼30%) of aromatic carbon to OC2. The OM/OC ratio for non-polar (OM1/OC1∼1.2) and polar organic aerosols (OM2/OC2∼2.2), hitherto unknown for open agricultural-waste burning emissions, is documented in this study. The total OM/OC ratio is nearly identical, 1.9±0.2 and 1.8±0.2, from paddy- and wheat-residue burning emissions. Copyright © 2013 Elsevier Ltd. All rights reserved.

  11. Prevention of PCDD/Fs emission from a municipal wastewater sludge incinerator through enhanced control of copper aerosol

    Directory of Open Access Journals (Sweden)

    Peña, E.

    2012-10-01

    Full Text Available Municipal wastewater sludge incineration (MWSI leads to products of incomplete combustion, including chlorinated species such as dioxins and furans (PCDD/Fs. Other pollutants, such as heavy metals (HM, are released too as a consequence of feed traces, which depend on the specific activities of each area. The main aim of this work is to determine whether the early separation of the potential catalysts on the PCDD/Fs formation –HM as copper or zinc– offers a promising way to prevent the emission of these trace pollutants, considering that the current end-of-pipe measures don’t ensure their stable emission. Experimental results cover the size distributed target metal contents along the incineration line. These results show a high concentration of copper in the most penetrating aerosol size range of the electrostatic precipitator (0.6 μm - 1.0 μm, and how low emission values of both, total and metallic aerosol (mass basis, are compatible with irregular and unexplained outliers of PCDD/Fs emission.

    La incineración de lodos de aguas residuales urbanas acarrea la formación de compuestos derivados de combustiones incompletas, incluyendo especies cloradas como dioxinas y furanos (PCDD/Fs. Otros contaminantes, como metales pesados, se emiten como consecuencia de las trazas del lodo, las cuales dependen de las actividades del entorno. El objetivo principal es determinar si la separación de catalizadores potenciales en reacciones de formación de PCDD/Fs (cobre o zinc puede abrir vías para prevenir la emisión de contaminantes traza, considerando que ninguna de las técnicas de prevención actuales aseguran emisiones estables de metales pesados o PCDD/Fs. Se determinan concentraciones de metales pesados segregados por tamaño de partícula a lo largo de la línea de incineración. Los resultados muestran concentraciones elevadas de cobre en el aerosol de máxima penetración del electrofiltro (0,6 μm - 1,0 μm, y cómo concentraciones

  12. The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

    Science.gov (United States)

    Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

    The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

  13. Small global effect on terrestrial net primary production due to increased fossil fuel aerosol emissions from East Asia during the last decade.

    Science.gov (United States)

    O'Sullivan, Michael; Rap, Alex; Reddington, Carly; Spracklen, Dominick; Buermann, Wolfgang

    2016-04-01

    The global terrestrial carbon sink has increased since the start of this century at a time of rapidly growing carbon dioxide emissions from fossil fuel burning. Here we test the hypothesis that increases in atmospheric aerosols from fossil fuel burning have increased the diffuse fraction of incoming solar radiation and the efficiency of photosynthesis leading to increased plant carbon uptake. Using a combination of atmospheric and biospheric models, we find that changes in diffuse light associated with fossil fuel aerosol emission accounts for only 2.8% of the increase in global net primary production (1.221 PgC/yr) over the study period 1998 to 2007. This relatively small global signal is however a result of large regional compensations. Over East Asia, the strong increase in fossil fuel emissions contributed nearly 70% of the increased plant carbon uptake (21 TgC/yr), whereas the declining fossil fuel aerosol emissions in Europe and North America contributed negatively (-16% and -54%, respectively) to increased plant carbon uptake. At global scale, we also find the CO2 fertilization effect on photosynthesis to be the dominant driver of increased plant carbon uptake, in line with previous studies. These results suggest that further research into alternative mechanisms by which fossil fuel emissions could increase carbon uptake, such as nitrogen deposition and carbon-nitrogen interactions, is required to better understand a potential link between the recent changes in fossil fuel emissions and terrestrial carbon uptake.

  14. Impacts of Future Climate, Emission, and Land Use Changes on Aerosols and Air Quality over the Continental

    Science.gov (United States)

    Changes in climate, emission, and land use in the U.S. over the next century are imminent. The response of geologic, biogenic, and anthropogenic aerosol to interactions between these changes, however, are more uncertain and difficult to quantify. To explore these interactions, ...

  15. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

    OpenAIRE

    Gantt, B.; Kelly, J. T.; Bash, J. O.

    2015-01-01

    Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the...

  16. Evaluation of the health impact of aerosols emitted from different combustion sources: Comprehensive characterization of the aerosol physicochemical properties as well as the molecular biological and toxicological effects of the aerosols on human lung cells and macrophages.

    Science.gov (United States)

    Zimmermann, R.; Dittmar, G.; Kanashova, T.; Buters, J.; Öder, S.; Paur, H. R.; Mülhopt, S.; Dilger, M.; Weiss, C.; Harndorf, H.; Stengel, B.; Hirvonen, M. R.; Jokiniemi, J.; Hiller, K.; Sapcariu, S.; Sippula, O.; Streibel, T.; Karg, E.; Weggler, B.; Schnelle-Kreis, J.; Lintelmann, J.; Sklorz, M.; Orasche, J.; Müller, L.; Passig, J.; Gröger, T.; Jalava, P. I.; Happo, M.; Uski, O.

    2017-12-01

    A novel approach to evaluate the health effects of anthropogenic combustion emissions is the detailed comparison of comprehensive physicochemical data on the combustion aerosol properties with the biological response of aerosol-exposed lung cells. In this context the "HICE-Aerosol and Health" project consortium studies the properties as well as the biological and toxicological effects on lung cells induced by different combustion aerosol emissions (e.g. ship diesel exhaust, wood combustion effluents or automobile aerosol). Human alveolar epithelial cells (e.g. A549 cells) as well as murine macrophages were exposed to diluted emissions, using field deployable ALI-exposition systems in a mobile S2-biological laboratory. This allows a realistic lung-cell exposure by simulation of the lung situation. The cellular effects were then comprehensively characterized (cytotoxicology, transcriptomics, proteomics etc.) effects monitoring and put in context with the chemical and physical aerosol data. Emissions of wood combustion, a ship engine as well as diesel and gasoline engines were investigated. Furthermore for some experiments the atmospheric aging of the emission was simulated in a flow tube reactor using UV-light and ozone. Briefly the following order of cellular response-strength was observed: A relatively mild cellular effect is observed for the diluted wood combustion emissions, regardless if log-wood and pellet burner emissions are investigated. Similarly mild biological effects are observed for gasoline car emissions. The ship diesel engine emissions and construction machine diesel engine induced much more intense biological responses. A surprising result in this context is, that heavy fuel oil (HFO)-emissions show lower biological effect strengths than the supposedly cleaner diesel fuel emissions (DF). The HFO-emissions contain high concentrations of known toxicants (metals, polycyclic aromatics). This result was confirmed by experiments with murine macrophages

  17. Aerosol composition and source apportionment in Santiago de Chile

    International Nuclear Information System (INIS)

    Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

    1999-01-01

    Santiago de Chile, Sao Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3 . Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10 ). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2 . In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of

  18. Characterizing the Sources and Processing of Submicron Aerosols at a Coastal Site near Houston, TX, with a Specific Focus on the Impact of Regional Shipping Emissions

    Science.gov (United States)

    Schulze, B.; Wallace, H. W., IV; Bui, A.; Flynn, J. H., III; Erickson, M. H.; Griffin, R. J.

    2017-12-01

    The Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recent establishment of the North American Emissions Control Area (ECA) on aerosol properties in this region are presently unknown. In order to understand better the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for three weeks at a coastal location during May-June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Using estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA:non-sea-salt-sulfate (nss-SO4) ratios, we determined that over 70% of nss-SO4 over the Gulf was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backward-trajectory-averaged meteorological conditions, air masses influenced by shipping emissions have an increased mass fraction of ions related to carboxylic acids and a significantly larger oxygen-to-carbon (O:C) ratio than air masses that stay within the ECA boundary, suggesting that shipping emissions impact marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were positively correlated with anthropogenic nss-SO4 during onshore flow, implying anthropogenic-biogenic interaction in marine OA production. Five OA factors were resolved by positive matrix factorization, corresponding to a hydrocarbon-like OA, a semi-volatile OA, and three different oxygenated organic aerosols ranked by their O:C ratio (OOA-1, OOA-2, and OOA-3). OOA-1 constituted the majority of OA mass during a period likely influenced by aqueous-phase processing and may be linked to local glyoxal/methylglyoxal-related sources. OOA-2 was produced within the Houston urban region and was

  19. Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo campaign

    Directory of Open Access Journals (Sweden)

    R. Ots

    2016-05-01

    Full Text Available We present high-resolution (5 km  ×  5 km atmospheric chemical transport model (ACTM simulations of the impact of newly estimated traffic-related emissions on secondary organic aerosol (SOA formation over the UK for 2012. Our simulations include additional diesel-related intermediate-volatility organic compound (IVOC emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA components derived from aerosol mass spectrometer (AMS measurements also made during the ClearfLo campaign at three sites in the London area. According to the model simulations, diesel-related IVOCs can explain on average  ∼  30 % of the annual SOA in and around London. Furthermore, the 90th percentile of modelled daily SOA concentrations for the whole year is 3.8 µg m−3, constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

  20. Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

    OpenAIRE

    Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

    2014-01-01

    Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as d...

  1. Aerosol emissions factors from traditional biomass cookstoves in India: insights from field measurements

    Directory of Open Access Journals (Sweden)

    A. Pandey

    2017-11-01

    Full Text Available Residential solid biomass cookstoves are important sources of aerosol emissions in India. Cookstove emissions rates are largely based on laboratory experiments conducted using the standard water-boiling test, but real-world emissions are often higher owing to different stove designs, fuels, and cooking methods. Constraining mass emissions factors (EFs for prevalent cookstoves is important because they serve as inputs to bottom-up emissions inventories used to evaluate health and climate impacts. Real-world EFs were measured during winter 2015 for a traditional cookstove (chulha burning fuel wood, agricultural residue, and dung from different regions of India. Average (±95 % confidence interval EFs for fuel wood, agricultural residue, and dung were (1 PM2.5 mass: 10.5 (7.7–13.4 g kg−1, 11.1 (7.7–15.5 g kg−1, and 22.6 (14.9–32.9 g kg−1, respectively; (2 elemental carbon (EC: 0.9 (0.6–1.4 g kg−1, 1.6 (0.6–3.0 g kg−1, and 1.0 (0.4–2.0 g kg−1, respectively; and (3 organic carbon (OC: 4.9 (3.2–7.1 g kg−1, 7.0 (3.5–12.5 g kg−1, and 12.9 (4.2–15.01 g kg−1, respectively. The mean (±95 % confidence interval OC ∕ EC mass ratios were 6.5 (4.5–9.1, 7.6 (4.4–12.2, and 12.7 (6.5–23.3, respectively, with OC and EC quantified by the IMPROVE_A thermal-optical reflectance protocol. These real-world EFs are higher than those from previous laboratory-based measurements. Combustion conditions have larger effects on EFs than the fuel types. We also report the carbon mass fractions of our aerosol samples determined using the thermal-optical reflectance method. The mass fraction profiles are consistent between the three fuel categories but markedly different from those reported in past literature – including the source profiles for wood stove PM2.5 emissions developed as inputs to receptor modeling studies conducted by the Central Pollution Control Board of India. Thermally

  2. Response of gaseous carbon emissions to low-level salinity increase in tidal marsh ecosystem of the Min River estuary, southeastern China.

    Science.gov (United States)

    Hu, Minjie; Ren, Hongchang; Ren, Peng; Li, Jiabing; Wilson, Benjamin J; Tong, Chuan

    2017-02-01

    Although estuarine tidal marshes are important contributors to the emission of greenhouse gases into the atmosphere, the relationship between carbon dioxide (CO 2 ), methane (CH 4 ) emission, and environmental factors, with respect to estuarine marshes, has not been clarified thoroughly. This study investigated the crucial factors controlling the emission of CO 2 and CH 4 from a freshwater marsh and a brackish marsh located in a subtropical estuary in southeastern China, as well as their magnitude. The duration of the study period was November 2013 to October 2014. Relevant to both the field and incubation experiments, the CO 2 and CH 4 emissions from the two marshes showed pronounced seasonal variations. The CO 2 and CH 4 emissions from both marshes demonstrated significant positive correlations with the air/soil temperature (pemissions between the freshwater and brackish marshes in the subtropical estuary, whereas there was a difference in the CH 4 emissions between the two sites (pemissions from the estuarine freshwater marshes, these factors had little effect on the CO 2 emissions with respect to an increase in salinity of less than 5‰. The findings of this study could have important implications for estimating the global warming contributions of estuarine marshes along differing salinity gradients. Copyright © 2016. Published by Elsevier B.V.

  3. Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

    Science.gov (United States)

    C. J. Hennigan; M. A. Miracolo; G. J. Engelhart; A. A. May; A. A. Presto; T. Lee; A. P. Sullivan; G. R. McMeeking; H. Coe; C. E. Wold; W.-M. Hao; J. B. Gilman; W. C. Kuster; J. de Gouw; B. A. Schichtel; J. L. Collett; S. M. Kreidenweis; A. L. Robinson

    2011-01-01

    Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA) during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III). We investigated emissions from 12 different...

  4. In-situ studies on volatile jet exhaust particle emissions - impacts of fuel sulfur content and environmental conditions on nuclei-mode aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Schroeder, F.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Brock, C.A. [Denver Univ., CO (United States). Dept. of Engineering

    2000-02-01

    In-situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the DLR ATTAS research jet (RR M45H M501 engines) and a B737-300 aircraft (CFM56-3B1 engines). Measurements were made 0.15-20 seconds after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56 or 118 mg kg{sup -1}. Particle size distributions of from 3 to 60 nm diameter were determined using CN-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60 mg kg{sup -1}, reaching minimum values of about 2 x 10{sup 17} kg{sup -1} and 2 x 10{sup 16} kg{sup -1} for particles >3 nm and >5 nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60 mg kg{sup -1}. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4 x 10{sup 14} kg{sup -1}) than from the older RR M45H M501 engines (1.8 x 10{sup 15} kg{sup -1}). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors 2-10 depending on particle size.

  5. Emission and chemistry of organic carbon in the gas and aerosol phase at a sub-urban site near Mexico City in March 2006 during the MILAGRO study

    Directory of Open Access Journals (Sweden)

    J. A. de Gouw

    2009-05-01

    Full Text Available Volatile organic compounds (VOCs and carbonaceous aerosol were measured at a sub-urban site near Mexico City in March of 2006 during the MILAGRO study (Megacity Initiative: Local and Global Research Objectives. Diurnal variations of hydrocarbons, elemental carbon (EC and hydrocarbon-like organic aerosol (HOA were dominated by a high peak in the early morning when local emissions accumulated in a shallow boundary layer, and a minimum in the afternoon when the emissions were diluted in a significantly expanded boundary layer and, in case of the reactive gases, removed by OH. In comparison, diurnal variations of species with secondary sources such as the aldehydes, ketones, oxygenated organic aerosol (OOA and water-soluble organic carbon (WSOC stayed relatively high in the afternoon indicating strong photochemical formation. Emission ratios of many hydrocarbon species relative to CO were higher in Mexico City than in the U.S., but we found similar emission ratios for most oxygenated VOCs and organic aerosol. Secondary formation of acetone may be more efficient in Mexico City than in the U.S., due to higher emissions of alkane precursors from the use of liquefied petroleum gas. Secondary formation of organic aerosol was similar between Mexico City and the U.S. Combining the data for all measured gas and aerosol species, we describe the budget of total observed organic carbon (TOOC, and find that the enhancement ratio of TOOC relative to CO is conserved between the early morning and mid afternoon despite large compositional changes. Finally, the influence of biomass burning is investigated using the measurements of acetonitrile, which was found to correlate with levoglucosan in the particle phase. Diurnal variations of acetonitrile indicate a contribution from local burning sources. Scatter plots of acetonitrile versus CO suggest that the contribution of biomass burning to the enhancement of most gas and aerosol species was not dominant and perhaps

  6. Emission and Chemistry of Organic Carbon in the Gas and Aerosol Phase at a Sub-Urban Site Near Mexico City in March 2006 During the MILAGRO Study

    Energy Technology Data Exchange (ETDEWEB)

    de Gouw, Joost A.; Welsh-Bon, Daniel; Warneke, Carsten; Kuster, W. C.; Alexander, M. L.; Baker, Angela K.; Beyersdorf, Andreas J.; Blake, D. R.; Canagaratna, Manjula R.; Celada, A. T.; Huey, L. G.; Junkermann, W.; Onasch, Timothy B.; Salcido, A.; Sjostedt, S. J.; Sullivan, Amy; Tanner, David J.; Vargas-Ortiz, Leroy; Weber, R. J.; Worsnop, Douglas R.; Yu, Xiao-Ying; Zaveri, Rahul A.

    2009-05-28

    Volatile organic compounds (VOCs) and carbonaceous aerosol were measured at a sub-urban site near Mexico City in March of 2006 during the MILAGRO study (Megacity Initiative: Local and Global Research Objectives). Diurnal variations of hydrocarbons, elemental carbon (EC) and hydrocarbon-like organic aerosol (HOA) were dominated by a high peak in the early morning when local emissions accumulated in a shallow boundary layer, and a minimum in the afternoon when the emissions were diluted in a significantly expanded boundary layer and, in case of the reactive gases, removed by OH. In comparison, diurnal variations of species with secondary sources such as the aldehydes, ketones, oxygenated organic aerosol (OOA) and water-soluble organic carbon (WSOC) stayed relatively high in the afternoon indicating strong photochemical formation. Emission ratios of many hydrocarbon species relative to CO were higher in Mexico City than in the U.S., but we found similar emission ratios for most oxygenated VOCs and organic aerosol. Secondary formation of acetone may be more efficient in Mexico City than in the U.S., due to higher emissions of alkane precursors from the use of liquefied petroleum gas. Secondary formation of organic aerosol was similar between Mexico City and the U.S. Combining the data for all measured gas and aerosol species, we describe the budget of total observed organic carbon (TOOC), and find that the enhancement ratio of TOOC relative to CO is conserved between the early morning and mid afternoon despite large compositional changes. Finally, the influence of biomass burning is investigated using the measurements of acetonitrile, which was found to correlate with levoglucosan in the particle phase. Diurnal variations of acetonitrile indicate a contribution from local burning sources. Scatter plots of acetonitrile versus CO suggest that the contribution of biomass burning to the enhancement of most gas and aerosol species was not dominant and perhaps not dissimilar

  7. Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

    Science.gov (United States)

    Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

    2014-12-01

    Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

  8. The economics and ethics of aerosol geoengineering strategies

    Science.gov (United States)

    Goes, Marlos; Keller, Klaus; Tuana, Nancy

    2010-05-01

    Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for a different approach: geoengineering climate by injecting aerosol precursors into the stratosphere. Published economic studies typically neglect the risks of aerosol geoengineering due to (i) a potential failure to sustain the aerosol forcing and (ii) due to potential negative impacts associated with aerosol forcings. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcings. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes considerable caveats. For example, the analysis is based on a globally aggregated model and is hence silent on intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of future learning and is based on a simple representation of climate change impacts. We use this integrated assessment model to show three main points. First, substituting aerosol geoengineering for the reduction of greenhouse gas emissions can fail the test of economic efficiency. One key to this finding is that a failure to sustain the aerosol forcing can lead to sizeable and abrupt climatic changes. The monetary damages due to such a discontinuous aerosol geoengineering can dominate the cost-benefit analysis because the monetary damages of climate change are expected to increase with

  9. Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

    Science.gov (United States)

    Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

    2008-12-01

    The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

  10. Secondary inorganic aerosols in Europe: sources and the significant influence of biogenic VOC emissions, especially on ammonium nitrate

    Science.gov (United States)

    Aksoyoglu, Sebnem; Ciarelli, Giancarlo; El-Haddad, Imad; Baltensperger, Urs; Prévôt, André S. H.

    2017-06-01

    Contributions of various anthropogenic sources to the secondary inorganic aerosol (SIA) in Europe as well as the role of biogenic emissions on SIA formation were investigated using the three-dimensional regional model CAMx (comprehensive air quality model with extensions). Simulations were carried out for two periods of EMEP field campaigns, February-March 2009 and June 2006, which are representative of cold and warm seasons, respectively. Biogenic volatile organic compounds (BVOCs) are known mainly as precursors of ozone and secondary organic aerosol (SOA), but their role on inorganic aerosol formation has not attracted much attention so far. In this study, we showed the importance of the chemical reactions of BVOCs and how they affect the oxidant concentrations, leading to significant changes, especially in the formation of ammonium nitrate. A sensitivity test with doubled BVOC emissions in Europe during the warm season showed a large increase in secondary organic aerosol (SOA) concentrations (by about a factor of two), while particulate inorganic nitrate concentrations decreased by up to 35 %, leading to a better agreement between the model results and measurements. Sulfate concentrations decreased as well; the change, however, was smaller. The changes in inorganic nitrate and sulfate concentrations occurred at different locations in Europe, indicating the importance of precursor gases and biogenic emission types for the negative correlation between BVOCs and SIA. Further analysis of the data suggested that reactions of the additional terpenes with nitrate radicals at night were responsible for the decline in inorganic nitrate formation, whereas oxidation of BVOCs with OH radicals led to a decrease in sulfate. Source apportionment results suggest that the main anthropogenic source of precursors leading to formation of particulate inorganic nitrate is road transport (SNAP7; see Table 1 for a description of the categories), whereas combustion in energy and

  11. Evolution of aerosol downwind of a major highway

    Science.gov (United States)

    Liggio, J.; Staebler, R. M.; Brook, J.; Li, S.; Vlasenko, A. L.; Sjostedt, S. J.; Gordon, M.; Makar, P.; Mihele, C.; Evans, G. J.; Jeong, C.; Wentzell, J. J.; Lu, G.; Lee, P.

    2010-12-01

    Primary aerosol from traffic emissions can have a considerable impact local and regional scale air quality. In order to assess the effect of these emissions and of future emissions scenarios, air quality models are required which utilize emissions representative of real world conditions. Often, the emissions processing systems which provide emissions input for the air quality models rely on laboratory testing of individual vehicles under non-ambient conditions. However, on the sub-grid scale particle evolution may lead to changes in the primary emitted size distribution and gas-particle partitioning that are not properly considered when the emissions are ‘instantly mixed’ within the grid volume. The affect of this modeling convention on model results is not well understood. In particular, changes in organic gas/particle partitioning may result in particle evaporation or condensation onto pre-existing aerosol. The result is a change in the particle distribution and/or an increase in the organic mass available for subsequent gas-phase oxidation. These effects may be missing from air-quality models, and a careful analysis of field data is necessary to quantify their impact. A study of the sub-grid evolution of aerosols (FEVER; Fast Evolution of Vehicle Emissions from Roadways) was conducted in the Toronto area in the summer of 2010. The study included mobile measurements of particle size distributions with a Fast mobility particle sizer (FMPS), aerosol composition with an Aerodyne aerosol mass spectrometer (AMS), black carbon (SP2, PA, LII), VOCs (PTR-MS) and other trace gases. The mobile laboratory was used to measure the concentration gradient of the emissions at perpendicular distances from the highway as well as the physical and chemical evolution of the aerosol. Stationary sites at perpendicular distances and upwind from the highway also monitored the particle size distribution. In addition, sonic anemometers mounted on the mobile lab provided measurements of

  12. Nitrous Oxide Emissions from Biofuel Crops and Atmospheric Aerosols: Associations with Air Quality and Regional Climate

    Science.gov (United States)

    Pillai, Priya Ramachandran

    Emissions of greenhouse gases (GHG) and primary release and secondary formation of aerosols alter the earth's radiative balance and therefore have important climatic implications. Savings in carbon dioxide (CO2) emissions accomplished by replacing fossil fuels with biofuels may increase the nitrous oxide (N2O) emissions. Among various atmospheric trace gases, N2O, irrespective of its low atmospheric concentration, is the fourth most important gas in causing the global greenhouse effect. Major processes, those affect the concentration of atmospheric N2O, are soil microbial activities leading to nitrification and denitrification. Therefore, anthropogenic activities such as industrial emissions, and agricultural practices including application of nitrogenous fertilizers, land use changes, biomass combustion all contribute to the atmospheric N2O concentration. The emission rates of N2O related to biofuel production depend on the nitrogen (N) fertilizer uptake efficiency of biofuel crops. However, crops with less N demand, such as switchgrass may have more favorable climate impacts when compared to crops with high N demands, such as corn. Despite its wide environmental tolerance, the regional adaptability of the potential biofuel crop switch grass varies considerably. Therefore, it is important to regionally quantify the GHG emissions and crop yield in response to N-fertilization. A major objective of this study is to quantify soil emissions of N2O from switchgrass and corn fields as a function of N-fertilization. The roles of soil moisture and soil temperature on N2O fluxes were analyzed. These N2O observations may be used to parameterize the biogeochemical models to better understand the impact of different N2O emission scenarios. This study allows for improvements in climate models that focus on understanding the environmental impacts of the climate change mitigation strategy of replacing fossil fuels with biofuels. As a second major objective, the top of the

  13. Electrostatic charge characteristics of jet nebulized aerosols.

    Science.gov (United States)

    Kwok, Philip Chi Lip; Trietsch, Sebastiaan J; Kumon, Michiko; Chan, Hak-Kim

    2010-06-01

    Liquid droplets can be spontaneously charged in the absence of applied electric fields by spraying. It has been shown by computational simulation that charges may influence particle deposition in the airways. The electrostatic properties of jet nebulized aerosols and their potential effects on lung deposition have hardly been studied. A modified electrical low pressure impactor (ELPI) was employed to characterize the aerosol charges generated from jet nebulized commercial products. The charge and size measurements were conducted at 50% RH and 22 degrees C with a modified ELPI. Ventolin, Bricanyl, and Atrovent were nebulized using PARI LC Plus jet nebulizers coupled to a DeVilbiss Pulmo-Aide compressor. The aerosols were sampled in 30-sec durations. The drug deposits on the impactor stages were assayed chemically using high-performance liquid chromatography (HPLC). The charges of nebulized deionized water, isotonic saline, and the three commercial products diluted with saline were also measured to analyze the contributions of the major nebule ingredients on charging. No mass assays were performed on these runs. All three commercial nebules generated net negative charges. The magnitude of the charges reduced over the period of nebulization. Ventolin and Bricanyl yielded similar charge profiles. Highly variable charges were produced from deionized water. On the other hand, nebulized saline reproducibly generated net positive charges. Diluted commercial nebules showed charge polarity inversion. The charge profiles of diluted salbutamol and terbutaline solutions resembled those of saline, while the charges from diluted ipratropium solutions fluctuated near neutrality. The charge profiles were shown to be influenced by the concentration and physicochemical properties of the drugs, as well as the history of nebulization. The drugs may have unique isoelectric concentrations in saline at which the nebulized droplets would carry near-zero charges. According to results from

  14. Primary Emission and the Potential of Secondary Aerosol Formation from Chinese Gasoline Engine Exhaust

    Science.gov (United States)

    Hu, Min; Peng, Jianfei; Qin, Yanhong; Du, Zhuofei; Li, Mengjin; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Lu, Sihua; Wu, Yusheng; Zeng, Limin; Guo, Song; Shao, Min; Wang, Yinhui; Shuai, Shijin

    2017-04-01

    Along with the urbanization and economic growth, vehicle population in China reached 269 million, ranked the second in the world in 2015. Gasoline vehicle is identified to be the main source for urban PM2.5 in China, accounting for 15%-31%. In this study the impact of fuel components on PM2.5 and volatile organic compounds (VOCs) emissions from a gasoline port fuel injection (PFI) engine and a gasoline direct injection (GDI) engine are discussed. Results show that, higher proportion of aromatics, alkenes or sulfur in gasoline fuel will lead to higher PM emissions. The PM from the PFI engine mainly consists of OC and a small amount of EC and inorganic ions, while the PM discharge from the GDI engine mainly consists of EC, OM and a small amount of inorganic ions. Since the GDI engines can reduce fuel consumption and CO2 emissions, and it would become more and more popular in the near future. The characteristics of POM component, emission factors and source profile were investigated from GDI engine, particularly focused on the effect of engine speed, load and the catalyst, which will be very much helpful for source identification as source indicators. Chamber experiments were conducted to quantify the potential of secondary aerosol formation from exhaust of a PFI gasoline engine and China V gasoline fuel. During 4-5 h simulation, equivalent to10 days of atmospheric photo-oxidation in Beijing, the extreme SOA production was 426 ± 85 mg/kg fuel, with high precursors and OH exposure. 14% of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatility organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reduction of emissions of aerosol precursor gases from vehicles is essential to mediate pollution in China.

  15. Natural and Anthropogenic Influences on Atmospheric Aerosol Variability

    Energy Technology Data Exchange (ETDEWEB)

    Asmi, A.

    2012-07-01

    Aerosol particles are everywhere in the atmosphere. They are a key factor in many important processes in the atmosphere, including cloud formation, scattering of incoming solar radiation and air chemistry. The aerosol particles have relatively short lifetimes in lower atmosphere, typically from days to weeks, and thus they have a high spatial and temporal variability. This thesis concentrates on the extent and reasons of sub-micron aerosol particle variability in the lower atmosphere, using both global atmospheric models and analysis of observational data. Aerosol number size distributions in the lower atmosphere are affected strongly by the new particle formation. Perhaps more importantly, a strong influence new particle formation is also evident in the cloud condensation nuclei (CCN) concentrations, suggesting a major role of the sulphuric acid driven new particle formation in the climate system. In this thesis, the sub-micron aerosol number size distributions in the European regional background air were characterized for the first time from consistent, homogenized and comparable datasets. Some recent studies have suggested that differences in aerosol emissions between weekdays could also affect the weather via aerosol-cloud interactions. In this thesis, the weekday-to-weekday variation of CCN sized aerosol number concentrations in Europe were found to be much smaller than expected from earlier studies, based on particle mass measurements. This result suggests that a lack of week-day variability in meteorology is not necessarily a sign of weak aerosol-cloud interactions. An analysis of statistically significant trends in past decades of measured aerosol number concentrations from Europe, North America, Pacific islands and Antarctica generally show decreases in concentrations. The analysis of these changes show that a potential explanation for the decreasing trends is the general reduction of anthropogenic emissions, especially SO{sub 2}, although a combination of

  16. Characterization of carbonaceous aerosol emissions from selected combustion sources

    International Nuclear Information System (INIS)

    Martinez, J.P.G.; Espino, M.P.M.; Pabroa, P.C.B.; Bautista, A.T. VII

    2015-01-01

    Carbonaceous Particulates are carbon-containing solid or liquid matter which form a significant portion of the fine particulate mass (PM2.5) and these have known profound adverse effects on health, climate and visibility. This study aims to characterize carbonaceous aerosol emissions from different combustion sources to establish fingerprints for these for use in the refinement of improvement of the resolution of sources apportionment studies being done by the Philippine Nuclear Research Institute (PNRI), i.e. to resolve vehicular emission sources. Fine air particulate sample were collected in pre-baked Quartz filters using an improvised collection set-up with a Gent sampler. Concentrations of organic and elemental carbon (OC and EC, respectively) in PM2.5 were measured for the different combustion sources—vehicular emissions, tire pyrolysis, and biomass burning, using a thermal-optical method of analysis following the IMPROVE_A protocol. Measured OC ad EC concentrations are shown as percentages with respect to the total carbon (TC) and are illustrated in a 100% stacked chart. Predominance of the EC2 fraction is exhibited in both the diesel fuelled vehicle and tire pyrolysis emissions with EC2/OC2 ratio distinguishing one from the other, EC2/OC2 is 1.63 and 8.41, respectively. Predominance of either OC2 or OC3 fraction is shown in the unleaded gasoline and LPG Fuelled vehicles and in biomass burning with the OC2/OC3 ratio distinguishing one from the others. OC2/OC3 ratios are 1.33 for unleaded gasoline fuelled vehicle, 1.89 for LPG-fuelled vehicle, 0.55 for biomass burning (leaves) and 0.82 biomass burning (wood). The study has shown probable use of the EC2/OC2 and OC2/OC3 ratios to distinguish fingerprints for combustion sources covered in this study. (author)

  17. Light absorption of biomass burning and vehicle emission-sourced carbonaceous aerosols of the Tibetan Plateau.

    Science.gov (United States)

    Hu, Zhaofu; Kang, Shichang; Li, Chaoliu; Yan, Fangping; Chen, Pengfei; Gao, Shaopeng; Wang, Zhiyong; Zhang, Yulan; Sillanpää, Mika

    2017-06-01

    Carbonaceous aerosols over the Tibetan Plateau originate primarily from biomass burning and vehicle emissions (BB and VEs, respectively). The light absorption characteristics of these carbonaceous aerosols are closely correlated with the burning conditions and represent key factors that influence climate forcing. In this study, the light absorption characteristics of elemental carbon (EC) and water-soluble organic carbon (WSOC) in PM 2.5 (fine particulate matter smaller than 2.5 μm) generated from BB and VEs were investigated over the Tibetan Plateau (TP). The results showed that the organic carbon (OC)/EC ratios from BB- and VE-sourced PM 2.5 were 17.62 ± 10.19 and 1.19 ± 0.36, respectively. These values were higher than the ratios in other regions, which was primarily because of the diminished amount of oxygen over the TP. The mass absorption cross section of EC (MAC EC ) at 632 nm for the BB-sourced PM 2.5 (6.10 ± 1.21 m 2 .g -1 ) was lower than that of the VE-sourced PM 2.5 (8.10 ± 0.98 m 2 .g -1 ), indicating that the EC content of the BB-sourced PM 2.5 was overestimated because of the high OC/EC ratio. The respective absorption per mass (α/ρ) values at 365 nm for the VE- and BB-sourced PM 2.5 were 0.71 ± 0.17 m 2 .g -1 and 0.91 ± 0.18 m 2 .g -1 . The α/ρ value of the VEs was loaded between that of gasoline and diesel emissions, indicating that the VE-sourced PM 2.5 originated from both types of emissions. Because OC and WSOC accounts for most of the carbonaceous aerosols at remote area of the TP, the radiative forcing contributed by the WSOC should be high, and requires further investigation.

  18. Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

    Science.gov (United States)

    Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

    2007-12-01

    Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

  19. Aerosol Optical Properties and Trace Gas Emissions From Laboratory-Simulated Western US Wildfires

    Science.gov (United States)

    Selimovic, V.; Yokelson, R. J.; Warneke, C.; Roberts, J. M.; De Gouw, J. A.; Reardon, J.; Griffith, D. W. T.

    2017-12-01

    Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 fires were burned in the large-scale combustion facility at the US Forest Service Missoula Fire Sciences Laboratory as part of the Fire Influence on Regional and Global Environments Experiment (FIREX). Canopy, litter, duff, dead wood, and other fuels from various widespread coniferous and chaparral ecosystems were burned in combinations to represent relevant configurations in the field and as pure components to investigate the effects of individual fuels. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, g compound emitted per kg fuel burned) measurements in fresh smoke of a diverse suite of critically-important trace gases measured by open-path Fourier transform infrared spectroscopy (OP-FTIR). We also report aerosol optical properties (absorption EF, single scattering albedo (SSA) and Ångström absorption exponent (AAE)) as well as black carbon (BC) EF measured by photoacoustic extinctiometers (PAX) at 870 and 401 nm. A careful comparison with available field measurements of wildfires confirms that representative data can be extracted from the lab fire data. The OP-FTIR data show that ammonia (1.65 g kg-1), acetic acid (2.44 g kg-1), and other trace gases are significant emissions not previously measured for US wildfires. The PAX measurements show that brown carbon (BrC) absorption is most dominant for combustion of duff (AAE 7.13) and rotten wood (AAE 4.60): fuels that are consumed in greater amounts during wildfires than prescribed fires. We confirm that about 86% of the aerosol absorption at 401 nm in typical fresh wildfire smoke is due to BrC.

  20. A global perspective on aerosol from low-volatility organic compounds

    Directory of Open Access Journals (Sweden)

    H. O. T. Pye

    2010-05-01

    Full Text Available Global production of organic aerosol from primary emissions of semivolatile (SVOCs and intermediate (IVOCs volatility organic compounds is estimated using the global chemical transport model, GEOS-Chem. SVOC oxidation is predicted to be a larger global source of net aerosol production than oxidation of traditional parent hydrocarbons (terpenes, isoprene, and aromatics. Using a prescribed rate constant and reduction in volatility for atmospheric oxidation, the yield of aerosol from SVOCs is predicted to be about 75% on a global, annually-averaged basis. For IVOCs, the use of a naphthalene-like surrogate with different high-NOx and low-NOx parameterizations produces a global aerosol yield of about 30%, or roughly 5 Tg/yr of aerosol. Estimates of the total global organic aerosol source presented here range between 60 and 100 Tg/yr. This range reflects uncertainty in the parameters for SVOC volatility, SVOC oxidation, SVOC emissions, and IVOC emissions, as well as wet deposition. The highest estimates result if SVOC emissions are significantly underestimated (by more than a factor of 2 or if wet deposition of the gas-phase semivolatile species is less effective than previous estimates. A significant increase in SVOC emissions, a reduction of the volatility of the SVOC emissions, or an increase in the enthalpy of vaporization of the organic aerosol all lead to an appreciable reduction of prediction/measurement discrepancy. In addition, if current primary organic aerosol (POA inventories capture only about one-half of the SVOC emission and the Henrys Law coefficient for oxidized semivolatiles is on the order of 103 M/atm, a global estimate of OA production is not inconsistent with the top-down estimate of 140 Tg/yr by (Goldstein and Galbally, 2007. Additional information is needed to constrain the emissions and treatment of SVOCs and IVOCs, which have traditionally not been included in models.

  1. The economics (or lack thereof) of aerosol geoengineering

    Science.gov (United States)

    Goes, M.; Keller, K.; Tuana, N.

    2009-04-01

    Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for the deployment of a different approach: to geoengineer climate by injecting aerosol precursors into the stratosphere. Published economic studies typically suggest that substituting aerosol geoengineering for abatement of carbon dioxide emissions results in large net monetary benefits. However, these studies neglect the risks of aerosol geoengineering due to (i) the potential for future geoengineering failures and (ii) the negative impacts associated with the aerosol forcing. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcing. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes severe caveats on the interpretation of the results. For example, the analysis is based on a globally aggregated model and is hence silent on the question of intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of endogenous learning about the climate system. We show that the risks associated with a future geoengineering failure and negative impacts of aerosol forcings can cause geoenginering strategies to fail an economic cost-benefit test. One key to this finding is that a geoengineering failure would lead to dramatic and abrupt climatic changes. The monetary damages due to this failure can

  2. Influences of natural emission sources (wildfires and Saharan dust) on the urban organic aerosol in Barcelona (Western Mediterranean Basis) during a PM event.

    Science.gov (United States)

    van Drooge, Barend L; Lopez, Jordi F; Grimalt, Joan O

    2012-11-01

    The urban air quality in Barcelona in the Western Mediterranean Basin is characterized by overall high particulate matter (PM) concentrations, due to intensive local anthropogenic emissions and specific meteorological conditions. Moreover, on several days, especially in summer, natural PM sources, such as long-range transported Saharan dust from Northern Africa or wildfires on the Iberian Peninsula and around the Mediterranean Basin, may influence the levels and composition of the organic aerosol. In the second half of July 2009, daily collected PM(10) filter samples in an urban background site in Barcelona were analyzed on organic tracer compounds representing several emission sources. During this period, an important PM peak event was observed. Individual organic compound concentrations increased two to five times during this event. Although highest increase was observed for the organic tracer of biomass burning, the contribution to the organic aerosol was estimated to be around 6 %. Organic tracers that could be related to Saharan dust showed no correlation with the PM and OC levels, while this was the case for those related to fossil fuel combustion from traffic emissions. Moreover, a change in the meteorological conditions gave way to an overall increase of the urban background contamination. Long-range atmospheric transport of organic compounds from primary emissions sources (i.e., wildfires and Saharan dust) has a relatively moderate impact on the organic aerosol in an urban area where the local emissions are dominating.

  3. Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

    Science.gov (United States)

    Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

    2009-01-01

    The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

  4. Is the aerosol emission detectable in the thermal infrared?

    Science.gov (United States)

    Hollweg, H.-D.; Bakan, S.; Taylor, J. P.

    2006-08-01

    The impact of aerosols on the thermal infrared radiation can be assessed by combining observations and radiative transfer calculations. Both have uncertainties, which are discussed in this paper. Observational uncertainties are obtained for two FTIR instruments operated side by side on the ground during the LACE 1998 field campaign. Radiative transfer uncertainties are assessed using a line-by-line model taking into account the uncertainties of the HITRAN 2004 spectroscopic database, uncertainties in the determination of the atmospheric profiles of water vapor and ozone, and differences in the treatment of the water vapor continuum absorption by the CKD 2.4.1 and MT_CKD 1.0 algorithms. The software package OPAC was used to describe the optical properties of aerosols for climate modeling. The corresponding radiative signature is a guideline to the assessment of the uncertainty ranges of observations and models. We found that the detection of aerosols depends strongly on the measurement accuracy of atmospheric profiles of water vapor and ozone and is easier for drier conditions. Within the atmospheric window, only the forcing of downward radiation at the surface by desert aerosol emerges clearly from the uncertainties of modeling and FTIR measurement. Urban and polluted continental aerosols are only partially detectable depending on the wave number and on the atmospheric water vapor amount. Simulations for the space-borne interferometer IASI show that only upward radiation above transported mineral dust aloft emerges out of the uncertainties. The detection of aerosols with weak radiative impact by FTIR instruments like ARIES and OASIS is made difficult by noise as demonstrated by the signal to noise ratio for clean continental aerosols. Altogether, the uncertainties found suggest that it is difficult to detect the optical depths of nonmineral and unpolluted aerosols.

  5. Impact of anthropogenic aerosols on present and future climate

    International Nuclear Information System (INIS)

    Deandreis, C.

    2008-03-01

    Aerosols influence the Earth radiative budget both through their direct effect (scattering and absorption of solar radiation) and their indirect effect (impacts on cloud microphysics). The role of anthropogenic aerosol in climate change has been recognized to be significant when compared to the one of greenhouse gases. Despite many studies on this topic, the assessments of both anthropogenic aerosol radiative forcing and their impacts on meteorological variables are still very uncertain. Major reasons for these uncertainties stem from the insufficient knowledge of the emissions sources and of the processes of formation, transformation and deposition. Models used to study climate are often inadequate to study aerosol processes because of coarse spatial and temporal scales. Uncertainties due to the parameterization of the aerosol are added to the uncertainties in the representation of large scale dynamics and physical processes such as transport, hydrological cycle and radiative budget. To predict, the role of the anthropogenic aerosol impact in the future climate change, I have addressed some of these key uncertainties. In this study, I simulate interactively aerosols processes in a climate model in order to improve the estimation of their direct and indirect effects. I estimate a modification of the top of the atmosphere net flux of 60% for the present period. I also show that, for future projection, the representation of the emissions source is an other important source of error. I assess that aerosols radiative forcing differ by 40% between simulations performed with 2 different emissions inventories. These inventories are representative for a high and a low limit in term of carbonaceous aerosols emissions for the 2050 horizon. (author)

  6. 0D-modelling of carbonaceous aerosols; L'aerosol de combustion dans une region en grande mutation, l'Asie

    Energy Technology Data Exchange (ETDEWEB)

    Michel, Ch.

    2005-06-15

    One of the main uncertainties in the estimate of the climatic impact of aerosols is linked to our knowledge of gases and aerosols emissions. This is particularly crucial over Asia, where a strong regional fingerprint is observed, with different emission types, depending on the various vegetation and climate conditions (biomass burning emissions) and on the very fast changes of the population and industrialization (biofuel and fossil fuel emissions). The main goal of this work was first to derive a biomass burning inventory for gases and particles over Asia for the 2001 ACE-Asia (Aerosol Characterization Experiment) and TRACE-P (Transport and Chemical Evolution over the Pacific) campaigns (March to May 2001). I implemented a methodology that is the most adapted to my study, and based on the burnt area cartography (GBA-2000 project (Global Burnt Area 2000) [Tansey et al., 2005]). The results of this study, ABBI (Asian Biomass Burning Inventory) [Michel et al., 2005] have been compared with another biomass burning emission inventory (ACESS: ACE-Asia and TRACE-P Modelling and Emission Support System) [Streets et al., 2003], built from fire counts and not from burnt areas. This comparison shows the limits of the use of fire counts in the emission inventory maps and underlines the importance and the relevance of the method used in my study. A comparison with the year 2000 emission inventory, obtained with the same method, underlines the importance of the inter-annual variations. The ABBI inventory has been introduced in the Meso-NH-C mesoscale model combined with an aerosol module: ORISAM (ORganic and Inorganic Spectral Aerosol Module) Bessagnet, 2000]. I have focused in particular on the impact of the burnt vegetation emissions over the asian continent. Comparisons between simulated and ground and airborne measured data showed satisfactory results in some cases, but showed also some limits. Sensitivity tests have been carried out firstly to test the impact of fire

  7. Local emission of primary air pollutants and its contribution to wet deposition and concentrations of aerosols and gases in ambient air in Japan

    Science.gov (United States)

    Aikawa, Masahide; Hiraki, Takatoshi; Tomoyose, Nobutaka; Ohizumi, Tsuyoshi; Noguchi, Izumi; Murano, Kentaro; Mukai, Hitoshi

    2013-11-01

    We studied wet deposition by precipitation and the concentrations of aerosols and gases in ambient air in relation to the primary air pollutants discharged from domestic areas. The concentrations of aerosols and gases were influenced by nearby emissions except for non-sea-salt SO, which is transported long distances. The area facing the Sea of Japan showed much larger wet deposition than other areas, although the domestic emissions of the primary air pollutants there were small and showed a peak in wet deposition from October to March, as distinct from April to September in other areas. We performed the correlation analyses between wet deposition of each component and the product of the concentrations of corresponding aerosols and gases in ambient air and the two-thirds power of the precipitation. From the results, following scavenging processes were suggested. • Sulfate and ammonium were scavenged in precipitation as particulate matter such as (NH4)2SO4 and NH4HSO4. • Nitrate was scavenged mainly in precipitation through gaseous HNO3. • Ammonium was complementarily scavenged in precipitation through aerosols such as (NH4)2SO4 and NH4HSO4 and through gaseous NH3.

  8. BVOC-aerosol-climate interactions in the global aerosol-climate model ECHAM5.5-HAM2

    Directory of Open Access Journals (Sweden)

    R. Makkonen

    2012-11-01

    Full Text Available The biosphere emits volatile organic compounds (BVOCs which, after oxidation in the atmosphere, can partition on the existing aerosol population or even form new particles. The large quantities emitted provide means for a large potential impact on both aerosol direct and indirect effects. Biogenic responses to atmospheric temperature change can establish feedbacks even in rather short timescales. However, due to the complexity of organic aerosol partitioning, even the sign of these feedbacks is of large uncertainty. We use the global aerosol-climate model ECHAM5.5-HAM2 to explore the effect of BVOC emissions on new particle formation, clouds and climate. Two BVOC emission models, MEGAN2 and LPJ-GUESS, are used. MEGAN2 shows a 25% increase while LPJ-GUESS shows a slight decrease in global BVOC emission between years 2000 and 2100. The change of shortwave cloud forcing from year 1750 to 2000 ranges from −1.4 to −1.8 W m−2 with 5 different nucleation mechanisms. We show that the change in shortwave cloud forcing from the year 2000 to 2100 ranges from 1.0 to 1.5 W m−2. Although increasing future BVOC emissions provide 3–5% additional CCN, the effect on the cloud albedo change is modest. Due to simulated decreases in future cloud cover, the increased CCN concentrations from BVOCs can not provide significant additional cooling in the future.

  9. Large contribution of natural aerosols to uncertainty in indirect forcing

    Science.gov (United States)

    Carslaw, K. S.; Lee, L. A.; Reddington, C. L.; Pringle, K. J.; Rap, A.; Forster, P. M.; Mann, G. W.; Spracklen, D. V.; Woodhouse, M. T.; Regayre, L. A.; Pierce, J. R.

    2013-11-01

    The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

  10. Large contribution of natural aerosols to uncertainty in indirect forcing.

    Science.gov (United States)

    Carslaw, K S; Lee, L A; Reddington, C L; Pringle, K J; Rap, A; Forster, P M; Mann, G W; Spracklen, D V; Woodhouse, M T; Regayre, L A; Pierce, J R

    2013-11-07

    The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

  11. Importance of Sulfate Aerosol in Evaluating the Relative Contributions of Regional Emissions to the Historical Global Temperature Change

    International Nuclear Information System (INIS)

    Andronova, N.; Schlesinger, M.

    2004-01-01

    During the negotiations of the Kyoto Protocol the delegation of Brazil presented an approach for distributing the burden of emissions reductions among the Parties based on the effect of their cumulative historical emissions on the global-average near-surface temperature. The Letter to the Parties does not limit the emissions to be considered to be only greenhouse gas (GHG) emissions. Thus, in this paper we explore the importance of anthropogenic SOx emissions that are converted to sulfate aerosol in the atmosphere, together with the cumulative greenhouse gas emissions, in attributing historical temperature change. We use historical emissions and our simple climate model to estimate the relative contributions to global warming of the regional emissions by four Parties: OECD90, Africa and Latin America, Asia, and Eastern Europe and the Former Soviet Union. Our results show that for most Parties the large warming contributed by their GHG emissions is largely offset by the correspondingly large cooling by their SOx emissions. Thus, OECD90 has become the dominant contributor to recent global warming following its large reduction in SOx emissions after 1980

  12. Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation

    Directory of Open Access Journals (Sweden)

    P. Q. Fu

    2010-03-01

    Full Text Available Organic molecular composition of PM10 samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs, and photooxidation products from biogenic Volatile Organic Compounds (VOCs. At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl phthalate, C16 fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning and terephthalic acid, suggesting that the field burning of municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24–43% was recognized as the most significant source for the total identified compounds, followed by plastic emission (16–33%, secondary oxidation (8.6–23%, and microbial/marine sources (7.2–17%. In contrast, the contributions of terrestrial plant waxes (5.9–11% and biomass burning (4.2–6.4% were relatively

  13. Comparison of two different dust emission mechanisms over the Horqin Sandy Land area: Aerosols contribution and size distributions

    Science.gov (United States)

    Ju, Tingting; Li, Xiaolan; Zhang, Hongsheng; Cai, Xuhui; Song, Yu

    2018-03-01

    Dust aerosols (PM10) emission fluxes due to convective turbulent dust emissions (CTDE) and saltation-bombardment and/or aggregation-disintegration dust emissions (SADE) events were comparatively studied using the data obtained from the Naiman station over the Horqin Sandy Land area in Inner Mongolia, China from 2011 to 2015. The annual cumulative dust fluxes released by CTDE events was about one third of that by SADE events, with the order of 103∼104 μg m-2 s-1. The particle size distributions (PSDs) with diameter between 0.1 and 20 μm during CTDE and SADE events over the Horqin Sandy Land area were simulated based on the fragmentation theory, respectively. The results indicated that an improved equation based on fragmentation theory could be applied to describe the PSDs over the Horqin site which may be because the scale-invariant fragmentation theory mainly explains the PSDs of free dust particles on the surface, which differ from the PSDs of suspend airborne dust and the improved equation was more applicable to the PSDs of SADE events because the dust emission mechanism of SADE are saltation bombardment and aggregation disintegration. The number-related mean aerosol diameters (DN) barely varied under different friction velocity (u*) for SADE events, while the volume-related mean aerosol diameters (DV) changed distinctly with the change of u*. For CTDE events, the DN and DV had no obvious relationship with the change of u* because the dominating influence factor during CTDE event was thermal convection rather than u*. The mass-related PSDs usually exhibited a peak between 0.45 and 0.70 μm during SADE events, while for CTDE events there was a wide peak in the range of 0.10 0.70 μm. The results suggest that DN should be not be recommended as an individual parameter to describe the PSDs. The mass-related PSDs can effectively distinguish the SADE and CTDE events.

  14. Aerosol typing - key information from aerosol studies

    Science.gov (United States)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  15. Hypertonic saline in treatment of pulmonary disease in cystic fibrosis.

    LENUS (Irish Health Repository)

    Reeves, Emer P

    2012-01-01

    The pathogenesis of lung disease in cystic fibrosis is characterised by decreased airway surface liquid volume and subsequent failure of normal mucociliary clearance. Mucus within the cystic fibrosis airways is enriched in negatively charged matrices composed of DNA released from colonizing bacteria or inflammatory cells, as well as F-actin and elevated concentrations of anionic glycosaminoglycans. Therapies acting against airway mucus in cystic fibrosis include aerosolized hypertonic saline. It has been shown that hypertonic saline possesses mucolytic properties and aids mucociliary clearance by restoring the liquid layer lining the airways. However, recent clinical and bench-top studies are beginning to broaden our view on the beneficial effects of hypertonic saline, which now extend to include anti-infective as well as anti-inflammatory properties. This review aims to discuss the described therapeutic benefits of hypertonic saline and specifically to identify novel models of hypertonic saline action independent of airway hydration.

  16. Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

    Science.gov (United States)

    Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

    2015-05-01

    . Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

  17. a Study of the Origin of Atmospheric Organic Aerosols

    Science.gov (United States)

    Hildemann, Lynn Mary

    1990-01-01

    The sources of ambient organic particulate matter in urban areas are investigated through a program of emission source measurements, atmospheric measurements, and mathematical modeling of source/receptor relationships. A dilution sampler intended to collect fine organic aerosol from combustion sources is designed to simulate atmospheric cooling and dilution processes, so that organic vapors which condense under ambient conditions will be collected as particulate matter. This system is used to measure the emissions from a boiler burning distillate oil, a home fireplace, catalyst and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat cooking operations. Alternate techniques are used to sample the particulate matter emitted from cigarette smoking, a roofing tar pot, paved road dust, brake lining wear, tire wear, and vegetative detritus. The bulk chemical characteristics of the fine aerosol fraction are presented for each source. Over half of the fine aerosol mass emitted from automobiles, wood burning, meat cooking, home appliances, cigarettes, and tar pots is shown to consist of organic compounds. The organic material collected from these sources is analyzed using high-resolution gas chromatography. Using a simple analytical protocol, a quantitative, 50-parameter characterization of the elutable fine organic aerosol emitted from each source type is obtained, which proves to be a unique fingerprint that can be used to distinguish most sources from each other. A mathematical model is used to predict the characteristics of fine ambient organic aerosol in the Los Angeles area that would prevail if the primary organic emissions are transported without chemical reaction. The model is found to track the seasonal variations observed in the ambient aerosol at the three sites studied. Emissions from vehicles and fireplaces are identified as significant sources of solvent-extractable organic aerosol. Differences between the model

  18. Generation and characterization of cyclosporine aerosols for administration by inhalation

    International Nuclear Information System (INIS)

    Hoover, M.D.; Muggenburg, B.A.; Snipes, M.B.; Wolff, R.K.; Yeh, H.C.; Griffith, B.P.; Burckart, G.J.; Mauderly, J.L.

    1988-01-01

    A method was developed for generating aerosols of the immunosuppressive agent cyclosporine and a gamma-emitting radiolabel ( 99m Tc) for administration by inhalation. Cyclosporine was dissolved in ethyl alcohol (EtOH) and nebulized with a Love- lace nebulizer operated with 50 psi compressed air. For a cyclosporine concentration of 25 mg/mL, the particle size of the aerosol was 0.7 μm activity median aerodynamic diameter (AMAD), with 1.8 geometric standard deviation (GSD). The clear solution of EtOH and cyclosporine became a cloudy suspension when a limited amount of saline solution containing a 99m Tc radiolabel was added. This occurred because cyclosporine is hydrophobic. If saline concentrations as high as 6% in EtOH by volume were used, a gummy residue formed in the nebulizer and the particle aerodynamic diameter became unacceptably large (4.7 μm). When the saline concentration was only 3 % (the minimum radiolabel volume needed for gamma camera studies of lung deposition), the suspensions of cyclosporine could be nebulized to give a particle size of 2.2 μm AMAD with 2.1 GSD. The radiolabel was uniformly distributed with the spherical cyclosporine particles. Concentrations and particle size distributions remained constant over 1-h generation periods. These aerosols have been used in inhalation studies with Beagle dogs. (author)

  19. TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

    Energy Technology Data Exchange (ETDEWEB)

    Annette Rohr

    2006-03-01

    TERESA (Toxicological Evaluation of Realistic Emissions of Source Aerosols) involves exposing laboratory rats to realistic coal-fired power plant and mobile source emissions to help determine the relative toxicity of these PM sources. There are three coal-fired power plants in the TERESA program; this report describes the results of fieldwork conducted at the first plant, located in the Upper Midwest. The project was technically challenging by virtue of its novel design and requirement for the development of new techniques. By examining aged, atmospherically transformed aerosol derived from power plant stack emissions, we were able to evaluate the toxicity of PM derived from coal combustion in a manner that more accurately reflects the exposure of concern than existing methodologies. TERESA also involves assessment of actual plant emissions in a field setting--an important strength since it reduces the question of representativeness of emissions. A sampling system was developed and assembled to draw emissions from the stack; stack sampling conducted according to standard EPA protocol suggested that the sampled emissions are representative of those exiting the stack into the atmosphere. Two mobile laboratories were then outfitted for the study: (1) a chemical laboratory in which the atmospheric aging was conducted and which housed the bulk of the analytical equipment; and (2) a toxicological laboratory, which contained animal caging and the exposure apparatus. Animal exposures were carried out from May-November 2004 to a number of simulated atmospheric scenarios. Toxicological endpoints included (1) pulmonary function and breathing pattern; (2) bronchoalveolar lavage fluid cytological and biochemical analyses; (3) blood cytological analyses; (4) in vivo oxidative stress in heart and lung tissue; and (5) heart and lung histopathology. Results indicated no differences between exposed and control animals in any of the endpoints examined. Exposure concentrations for the

  20. A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

    Directory of Open Access Journals (Sweden)

    D. V. Spracklen

    2005-01-01

    Full Text Available A GLObal Model of Aerosol Processes (GLOMAP has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3nm vary between about 250–500 cm-3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acid-water particles. Remote marine CN concentrations increase to around 2000–10 000 cm (at standard temperature and pressure in the upper troposphere, which agrees with typical observed vertical profiles. Cloud condensation nuclei (CCN at 0.2% supersaturation vary between about 1000 cm-3 in polluted regions and between 10 and 500 cm-3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. For this sulfur-sea salt system it is estimated that sea spray emissions account for only ~10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean. In a run with only natural sulfate and sea salt emissions the global mean surface CN concentration is more than 60% of that from a run with 1985 anthropogenic

  1. Quantification of regional radiative impacts and climate effects of tropical fire aerosols

    Science.gov (United States)

    Tosca, M. G.; Zender, C. S.; Randerson, J. T.

    2011-12-01

    Regionally expansive smoke clouds originating from deforestation fires in Indonesia can modify local precipitation patterns via direct aerosol scattering and absorption of solar radiation (Tosca et al., 2010). Here we quantify the regional climate impacts of fire aerosols for three tropical burning regions that together account for about 70% of global annual fire emissions. We use the Community Atmosphere Model, version 5 (CAM5) coupled to a slab ocean model (SOM) embedded within the Community Earth System Model (CESM). In addition to direct aerosol radiative effects, CAM5 also quantifies indirect, semi-direct and cloud microphysical aerosol effects. Climate impacts are determined using regionally adjusted emissions data that produce realistic aerosol optical depths in CAM5. We first analyzed a single 12-year transient simulation (1996-2007) forced with unadjusted emissions estimates from the Global Fire Emissions Database, version 3 (GFEDv3) and compared the resulting aerosol optical depths (AODs) for 4 different burning regions (equatorial Asia, southern Africa, South America and boreal North America) to observed MISR and MODIS AODs for the same period. Based on this analysis we adjusted emissions for each burning region between 150 and 300% and forced a second simulation with the regionally adjusted emissions. Improved AODs from this simulation are compared to AERONET observations available at 15 stations throughout the tropics. We present here two transient simulations--one with the adjusted fire emissions and one without fires--to quantify the cumulative fire aerosol climate impact for three major tropical burning regions (equatorial Asia, southern Africa and South America). Specifically, we quantify smoke effects on radiation, precipitation, and temperature. References Tosca, M.G., J.T. Randerson, C.S. Zender, M.G. Flanner and P.J. Rasch (2010), Do biomass burning aerosols intensify drought in equatorial Asia during El Nino?, Atmos. Chem. Phys., 10, 3515

  2. Sampling and chemical analysis by TXRF of size-fractionated ambient aerosols and emissions

    International Nuclear Information System (INIS)

    John, A.C.; Kuhlbusch, T.A.J.; Fissan, H.; Schmidt, K.-G-; Schmidt, F.; Pfeffer, H.-U.; Gladtke, D.

    2000-01-01

    Results of recent epidemiological studies led to new European air quality standards which require the monitoring of particles with aerodynamic diameters ≤ 10 μm (PM 10) and ≤ 2.5 μm (PM 2.5) instead of TSP (total suspended particulate matter). As these ambient air limit values will be exceeded most likely at several locations in Europe, so-called 'action plans' have to be set up to reduce particle concentrations, which requires information about sources and processes of PMx aerosols. For chemical characterization of the aerosols, different samplers were used and total reflection x-ray fluorescence analysis (TXRF) was applied beside other methods (elemental and organic carbon analysis, ion chromatography, atomic absorption spectrometry). For TXRF analysis, a specially designed sampling unit was built where the particle size classes 10-2.5 μm and 2.5-1.0 μm were directly impacted on TXRF sample carriers. An electrostatic precipitator (ESP) was used as a back-up filter to collect particles <1 μm directly on a TXRF sample carrier. The sampling unit was calibrated in the laboratory and then used for field measurements to determine the elemental composition of the mentioned particle size fractions. One of the field campaigns was carried out at a measurement site in Duesseldorf, Germany, in November 1999. As the composition of the ambient aerosols may have been influenced by a large construction site directly in the vicinity of the station during the field campaign, not only the aerosol particles, but also construction material was sampled and analyzed by TXRF. As air quality is affected by natural and anthropogenic sources, the emissions of particles ≤ 10 μm and ≤ 2.5 μm, respectively, have to be determined to estimate their contributions to the so called coarse and fine particle modes of ambient air. Therefore, an in-stack particle sampling system was developed according to the new ambient air quality standards. This PM 10/PM 2.5 cascade impactor was

  3. Aerosol impacts on regional trends in atmospheric stagnation

    Science.gov (United States)

    Mascioli, N. R.; Fiore, A. M.; Previdi, M. J.

    2017-12-01

    Extreme pollution events pose a significant threat to human health and are a leading cause of premature mortality worldwide. While emissions of atmospheric pollutants and their precursors are projected to decrease in the future due to air quality legislation, future climate change may affect the underlying meteorological conditions that contribute to extreme pollution events. Stagnation events, characterized by weak winds and an absence of precipitation, contribute to extreme pollution by halting the removal of pollutants via advection and wet deposition. Here, we use a global climate model (GFDL-CM3) to show that regional stagnation trends over the historical period (1860-2005) are driven by changes in anthropogenic aerosol emissions, rather than rising greenhouse gases. In the northeastern and central United States, aerosol-induced changes in surface and upper level winds have produced significant decreases in the number of stagnant summer days, while decreasing precipitation in the southeast US has increased the number of stagnant summer days. Significant drying over eastern China in response to aerosol forcing contributed to increased stagnation. Additionally, this region was found to be particularly sensitive to changes in local emissions, indicating that improving air quality will also lessen stagnation. In Europe, we find a dipole pattern wherein stagnation decreases over southern Europe and increases over northern Europe in response to global increases in aerosol emissions. We hypothesize that this is due to changes in the large-scale circulation patterns associated with a poleward shift of the North Atlantic storm track. We find that in the future, the combination of declining aerosol emissions and the continued rise of greenhouse gas emissions will lead to a reversal of the historical stagnation trends.

  4. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

    Directory of Open Access Journals (Sweden)

    D. V. Spracklen

    2011-09-01

    Full Text Available Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = −77 % unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52–64 % of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of −0.34 W m−2, with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of −0.23 W m−2. The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.

  5. A Simple Model of Global Aerosol Indirect Effects

    Science.gov (United States)

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, Kirsty; Carslaw, Kenneth; Pierce, Jeffrey; Bauer, Susanne; Adams, Peter

    2013-01-01

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth's energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically based model expresses the aerosol indirect effect (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

  6. Aerosol and monsoon climate interactions over Asia: AEROSOL AND MONSOON CLIMATE INTERACTIONS

    Energy Technology Data Exchange (ETDEWEB)

    Li, Zhanqing [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Lau, W. K. -M. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Ramanathan, V. [Department of Atmospheric and Climate Sciences, University of California, San Diego California USA; Wu, G. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Ding, Y. [National Climate Center, China Meteorological Administration, Beijing China; Manoj, M. G. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Liu, J. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Qian, Y. [Pacific Northwest National Laboratory, Richland Washington USA; Li, J. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Zhou, T. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Fan, J. [Pacific Northwest National Laboratory, Richland Washington USA; Rosenfeld, D. [Institute of Earth Sciences, Hebrew University, Jerusalem Israel; Ming, Y. [Geophysical Fluid Dynamic Laboratory, NOAA, Princeton New Jersey USA; Wang, Y. [Jet Propulsion Laboratory, California Institute of Technology, Pasadena California USA; Huang, J. [College of Atmospheric Sciences, Lanzhou University, Lanzhou China; Wang, B. [Department of Atmospheric Sciences, University of Hawaii, Honolulu Hawaii USA; School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing China; Xu, X. [Chinese Academy of Meteorological Sciences, Beijing China; Lee, S. -S. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Cribb, M. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Zhang, F. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Yang, X. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Zhao, C. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Takemura, T. [Research Institute for Applied Mechanics, Kyushu University, Fukuoka Japan; Wang, K. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Xia, X. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Yin, Y. [School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing China; Zhang, H. [National Climate Center, China Meteorological Administration, Beijing China; Guo, J. [Chinese Academy of Meteorological Sciences, Beijing China; Zhai, P. M. [Chinese Academy of Meteorological Sciences, Beijing China; Sugimoto, N. [National Institute for Environmental Studies, Tsukuba Japan; Babu, S. S. [Space Physics Laboratory, Vikram Sarabhai Space Centre, Thiruvananthapuram India; Brasseur, G. P. [Max Planck Institute for Meteorology, Hamburg Germany

    2016-11-15

    Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. The atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.

  7. Where and What Is Pristine Marine Aerosol?

    Science.gov (United States)

    Russell, L. M.; Frossard, A. A.; Long, M. S.; Burrows, S. M.; Elliott, S.; Bates, T. S.; Quinn, P.

    2014-12-01

    The sources and composition of atmospheric marine aerosol particles have been measured by functional group composition (from Fourier transform infrared spectroscopy) to identify the organic composition of the pristine primary marine (ocean-derived) particles as 65% hydroxyl, 21% alkane, 6% amine, and 7% carboxylic acid functional groups [Frossard et al., 2014a,b]. Pristine but non-primary components from photochemical reactions (likely from biogenic marine vapor emissions) add carboxylic acid groups. Non-pristine contributions include shipping effluent in seawater and ship emissions, which add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. The pristine primary marine (ocean-derived) organic aerosol composition is nearly identical to model generated primary marine aerosol particles from bubbled seawater, indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the generated primary marine aerosol particles remained nearly constant over a broad range of chlorophyll-a concentrations, the generated primary marine aerosol particle alkane group fraction increased with chlorophyll-a concentrations. In addition, the generated primary marine aerosol particles have a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater hydroxyl group peak location is closer to that of polysaccharides. References Cited Frossard, Amanda A., Lynn M. Russell, Paola Massoli, Timothy S. Bates, and Patricia K. Quinn, "Side-by-Side Comparison of Four Techniques Explains the Apparent Differences in the Organic Composition of Generated and Ambient Marine Aerosol Particles," Aerosol Science and Technology - Aerosol Research Letter

  8. Dust-wind interactions can intensify aerosol pollution over eastern China.

    Science.gov (United States)

    Yang, Yang; Russell, Lynn M; Lou, Sijia; Liao, Hong; Guo, Jianping; Liu, Ying; Singh, Balwinder; Ghan, Steven J

    2017-05-11

    Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with unusual meteorological conditions, including weaker wind speeds. Here we show, based on model simulations, that during years with decreased wind speed, large decreases in dust emissions (29%) moderate the wintertime land-sea surface air temperature difference and further decrease winds by -0.06 (±0.05) m s -1 averaged over eastern China. The dust-induced lower winds enhance stagnation of air and account for about 13% of increasing aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime aerosol concentrations, with important implications that need to be taken into account by air quality studies.

  9. Spacetime Distributions of Wildfire Areas and Emissions of Carbon-Containing Gases and Aerosols in Northern Eurasia according to Satellite-Monitoring Data

    Science.gov (United States)

    Bondur, V. G.; Gordo, K. A.; Kladov, V. L.

    2017-12-01

    Based on online wildfire satellite-monitoring data, distributions of burned-out areas, as well as emission volumes of carbon-containing gases (CO and CO2) and fine aerosols (PM2.5), for different regions and months in 2005-2016 (across the territory of Russia) and in 2010-2016 (northern Eurasia) are analyzed. Distinctive features of the seasonal behavior of wildfires and emission volumes of carbon-containing gases and fine aerosols for different regions of northern Eurasia are determined. It is shown that between 2005 and 2016 the annual area of territories burned out during wildfires in Russia decreased by almost a factor of 2.6 owing to early detection and suppression of fire sources. It is determined that in 2014-2016 the relative size of burned-out areas in Ukraine increased 6-9-fold and volumes of CO, CO2, and PM2.5 emissions by more than a factor of 6.5-7.5 times when compared to earlier years and these characteristics for other European countries.

  10. Evidence of a reduction in cloud condensation nuclei activity of water-soluble aerosols caused by biogenic emissions in a cool-temperate forest.

    Science.gov (United States)

    Müller, Astrid; Miyazaki, Yuzo; Tachibana, Eri; Kawamura, Kimitaka; Hiura, Tsutom

    2017-08-16

    Biogenic organic aerosols can affect cloud condensation nuclei (CCN) properties, and subsequently impact climate change. Large uncertainties exist in how the difference in the types of terrestrial biogenic sources and the abundance of organics relative to sulfate affect CCN properties. For the submicron water-soluble aerosols collected for two years in a cool-temperate forest in northern Japan, we show that the hygroscopicity parameter κ CCN (0.44 ± 0.07) exhibited a distinct seasonal trend with a minimum in autumn (κ CCN  = 0.32-0.37); these κ CCN values were generally larger than that of ambient particles, including water-insoluble fractions. The temporal variability of κ CCN was controlled by the water-soluble organic matter (WSOM)-to-sulfate ratio (R 2  > 0.60), where the significant reduction of κ CCN in autumn was linked to the increased WSOM/sulfate ratio. Positive matrix factorization analysis indicates that α-pinene-derived secondary organic aerosol (SOA) substantially contributed to the WSOM mass (~75%) in autumn, the majority of which was attributable to emissions from litter/soil microbial activity near the forest floor. These findings suggest that WSOM, most likely α-pinene SOA, originated from the forest floor can significantly suppress the aerosol CCN activity in cool-temperate forests, which have implications for predicting climate effects by changes in biogenic emissions in future.

  11. Landscape fires dominate terrestrial natural aerosol - climate feedbacks

    Science.gov (United States)

    Scott, C.; Arnold, S.; Monks, S. A.; Asmi, A.; Paasonen, P.; Spracklen, D. V.

    2017-12-01

    The terrestrial biosphere is an important source of natural aerosol including landscape fire emissions and secondary organic aerosol (SOA) formed from biogenic volatile organic compounds (BVOCs). Atmospheric aerosol alters the Earth's climate by absorbing and scattering radiation (direct radiative effect; DRE) and by perturbing the properties of clouds (aerosol indirect effect; AIE). Natural aerosol sources are strongly controlled by, and can influence, climate; giving rise to potential natural aerosol-climate feedbacks. Earth System Models (ESMs) include a description of some of these natural aerosol-climate feedbacks, predicting substantial changes in natural aerosol over the coming century with associated radiative perturbations. Despite this, the sensitivity of natural aerosols simulated by ESMs to changes in climate or emissions has not been robustly tested against observations. Here we combine long-term observations of aerosol number and a global aerosol microphysics model to assess terrestrial natural aerosol-climate feedbacks. We find a strong positive relationship between the summertime anomaly in observed concentration of particles greater than 100 nm diameter and the anomaly in local air temperature. This relationship is reproduced by the model and driven by variability in dynamics and meteorology, as well as natural sources of aerosol. We use an offline radiative transfer model to determine radiative effects due to changes in two natural aerosol sources: landscape fire and biogenic SOA. We find that interannual variability in the simulated global natural aerosol radiative effect (RE) is negatively related to the global temperature anomaly. The magnitude of global aerosol-climate feedback (sum of DRE and AIE) is estimated to be -0.15 Wm-2 K-1 for landscape fire aerosol and -0.06 Wm-2 K-1 for biogenic SOA. These feedbacks are comparable in magnitude, but opposite in sign to the snow albedo feedback, highlighting the need for natural aerosol feedbacks to

  12. Aerosol modelling and validation during ESCOMPTE 2001

    Science.gov (United States)

    Cousin, F.; Liousse, C.; Cachier, H.; Bessagnet, B.; Guillaume, B.; Rosset, R.

    The ESCOMPTE 2001 programme (Atmospheric Research. 69(3-4) (2004) 241) has resulted in an exhaustive set of dynamical, radiative, gas and aerosol observations (surface and aircraft measurements). A previous paper (Atmospheric Research. (2004) in press) has dealt with dynamics and gas-phase chemistry. The present paper is an extension to aerosol formation, transport and evolution. To account for important loadings of primary and secondary aerosols and their transformation processes in the ESCOMPTE domain, the ORISAM aerosol module (Atmospheric Environment. 35 (2001) 4751) was implemented on-line in the air-quality Meso-NH-C model. Additional developments have been introduced in ORganic and Inorganic Spectral Aerosol Module (ORISAM) to improve the comparison between simulations and experimental surface and aircraft field data. This paper discusses this comparison for a simulation performed during one selected day, 24 June 2001, during the Intensive Observation Period IOP2b. Our work relies on BC and OCp emission inventories specifically developed for ESCOMPTE. This study confirms the need for a fine resolution aerosol inventory with spectral chemical speciation. BC levels are satisfactorily reproduced, thus validating our emission inventory and its processing through Meso-NH-C. However, comparisons for reactive species generally denote an underestimation of concentrations. Organic aerosol levels are rather well simulated though with a trend to underestimation in the afternoon. Inorganic aerosol species are underestimated for several reasons, some of them have been identified. For sulphates, primary emissions were introduced. Improvement was obtained too for modelled nitrate and ammonium levels after introducing heterogeneous chemistry. However, no modelling of terrigeneous particles is probably a major cause for nitrates and ammonium underestimations. Particle numbers and size distributions are well reproduced, but only in the submicrometer range. Our work points out

  13. Aerosol climate effects and air quality impacts from 1980 to 2030

    International Nuclear Information System (INIS)

    Menon, Surabi; Sednev, Igor; Unger, Nadine; Koch, Dorothy; Shindell, Drew; Francis, Jennifer; Garrett, Tim; Streets, David

    2008-01-01

    We investigate aerosol effects on climate for 1980, 1995 (meant to reflect present day) and 2030 using the NASA Goddard Institute for Space Studies climate model coupled to an on-line aerosol source and transport model with interactive oxidant and aerosol chemistry. Aerosols simulated include sulfates, organic matter (OM), black carbon (BC), sea-salt and dust and, additionally, the amount of tropospheric ozone is calculated, allowing us to estimate both changes to air quality and climate for different time periods and emission amounts. We include both the direct aerosol effect and indirect aerosol effects for liquid-phase clouds. Future changes for the 2030 A1B scenario are examined, focusing on the Arctic and Asia, since changes are pronounced in these regions. Our results for the different time periods include both emission changes and physical climate changes. We find that the aerosol indirect effect (AIE) has a large impact on photochemical processing, decreasing ozone amount and ozone forcing, especially for the future (2030-1995). Ozone forcings increase from 0 to 0.12 W m -2 and the total aerosol forcing decreases from -0.10 to -0.94 W m -2 (AIE decreases from -0.13 to -0.68 W m -2 ) for 1995-1980 versus 2030-1995. Over the Arctic we find that compared to ozone and the direct aerosol effect, the AIE contributes the most to net radiative flux changes. The AIE, calculated for 1995-1980, is positive (1.0 W m -2 ), but the magnitude decreases (-0.3 W m -2 ) considerably for the future scenario. Over Asia, we evaluate the role of biofuel- and transportation-based emissions (for BC and OM) via a scenario (2030A) that includes a projected increase (factor of 2) in biofuel- and transport-based emissions for 2030 A1B over Asia. Projected changes from present day due to the 2030A emissions versus 2030 A1B are a factor of 4 decrease in summertime precipitation in Asia. Our results are sensitive to emissions used. Uncertainty in present-day emissions suggests that

  14. Hypertonic Saline in Treatment of Pulmonary Disease in Cystic Fibrosis

    Directory of Open Access Journals (Sweden)

    Emer P. Reeves

    2012-01-01

    Full Text Available The pathogenesis of lung disease in cystic fibrosis is characterised by decreased airway surface liquid volume and subsequent failure of normal mucociliary clearance. Mucus within the cystic fibrosis airways is enriched in negatively charged matrices composed of DNA released from colonizing bacteria or inflammatory cells, as well as F-actin and elevated concentrations of anionic glycosaminoglycans. Therapies acting against airway mucus in cystic fibrosis include aerosolized hypertonic saline. It has been shown that hypertonic saline possesses mucolytic properties and aids mucociliary clearance by restoring the liquid layer lining the airways. However, recent clinical and bench-top studies are beginning to broaden our view on the beneficial effects of hypertonic saline, which now extend to include anti-infective as well as anti-inflammatory properties. This review aims to discuss the described therapeutic benefits of hypertonic saline and specifically to identify novel models of hypertonic saline action independent of airway hydration.

  15. Carbonyl Emissions in E-cigarette Aerosol: A Systematic Review and Methodological Considerations

    Directory of Open Access Journals (Sweden)

    Konstantinos E. Farsalinos

    2018-01-01

    Full Text Available Carbonyl emissions from tobacco cigarettes represent a substantial health risk contributing to smoking-related morbidity and mortality. As expected, this is an important research topic for tobacco harm reduction products, in an attempt to compare the relative risk of these products compared to tobacco cigarettes. In this study, a systematic review of the literature available on PubMed was performed analyzing the studies evaluating carbonyl emissions from e-cigarettes. A total of 32 studies were identified and presented. We identified a large diversity of methodologies, with substantial discrepancies in puffing patterns, aerosol collection and analytical methods as well as reported units of measurements. Such discrepancies make comparisons difficult, and in some cases the accuracy of the findings cannot be determined. Importantly, control for the generation of dry puffs was not performed in the vast majority of studies, particularly in studies using variable power devices, which could result in testing conditions and reported carbonyl levels that have no clinical relevance or context. Some studies have been replicated, verifying the presence of dry puff conditions. Whenever realistic use conditions were ensured, carbonyl emissions from e-cigarettes were substantially lower than tobacco cigarette smoke, while newer generation (bottom-coil, cotton wick atomizers appeared to emit minimal levels of carbonyls with questionable clinical significance in terms of health risk. However, extremely high levels of carbonyl emissions were reported in some studies, and all these studies need to be replicated because of potentially important health implications.

  16. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    International Nuclear Information System (INIS)

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-01-01

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m 2 between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m 2 depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  17. A study of regional-scale aerosol assimilation using a Stretch-NICAM

    Science.gov (United States)

    Misawa, S.; Dai, T.; Schutgens, N.; Nakajima, T.

    2013-12-01

    Although aerosol is considered to be harmful to human health and it became a social issue, aerosol models and emission inventories include large uncertainties. In recent studies, data assimilation is applied to aerosol simulation to get more accurate aerosol field and emission inventory. Most of these studies, however, are carried out only on global scale, and there are only a few researches about regional scale aerosol assimilation. In this study, we have created and verified an aerosol assimilation system on regional scale, in hopes to reduce an error associated with the aerosol emission inventory. Our aerosol assimilation system has been developed using an atmospheric climate model, NICAM (Non-hydrostaric ICosahedral Atmospheric Model; Satoh et al., 2008) with a stretch grid system and coupled with an aerosol transport model, SPRINTARS (Takemura et al., 2000). Also, this assimilation system is based on local ensemble transform Kalman filter (LETKF). To validate this system, we used a simulated observational data by adding some artificial errors to the surface aerosol fields constructed by Stretch-NICAM-SPRINTARS. We also included a small perturbation in original emission inventory. This assimilation with modified observational data and emission inventory was performed in Kanto-plane region around Tokyo, Japan, and the result indicates the system reducing a relative error of aerosol concentration by 20%. Furthermore, we examined a sensitivity of the aerosol assimilation system by varying the number of total ensemble (5, 10 and 15 ensembles) and local patch (domain) size (radius of 50km, 100km and 200km), both of which are the tuning parameters in LETKF. The result of the assimilation with different ensemble number 5, 10 and 15 shows that the larger the number of ensemble is, the smaller the relative error become. This is consistent with ensemble Kalman filter theory and imply that this assimilation system works properly. Also we found that assimilation system

  18. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state: an aerosol microphysical module for global atmospheric models

    Directory of Open Access Journals (Sweden)

    S. E. Bauer

    2008-10-01

    Full Text Available A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS climate model (ModelE are described. This module, which is based on the quadrature method of moments (QMOM, represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations.

    A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment

  19. Testing Re-entrained Aerosol Kinetic Emissions from Roads : a new approach to infer silt loading on roadways

    Science.gov (United States)

    Kuhns, H.; Etyemezian, V.; Landwehr, D.; MacDougall, C.; Pitchford, M.; Green, M.

    PM 10 and PM 2.5 emissions from roadways are currently estimated using the silt loading on the road surface as a surrogate for the emissions potential of road dust. While the United States Environmental Protection Agency prescribes this method in AP-42, there is considerable cost associated with silt loading measurements; it is feasible to sample only a small portion of a roadway network. A new approach for measuring the concentration of suspendable PM 10 above road surfaces has been developed to obtain a more spatially representative estimate of a road's potential to emit dust. The Testing Re-entrained Aerosols Kinetic Emissions from Roads (TRAKER) system uses real-time aerosol sensors mounted on a vehicle to measure the concentration of dust suspended from the road while the vehicle is in motion. When coupled with a Global Positioning System (GPS) instrument, TRAKER can be used to efficiently survey the changes in suspendable particles due to varying road conditions over a large spatial domain. In a recent study on paved roads in Las Vegas, the TRAKER system was compared with collocated silt loading measurements. The TRAKER system was also used to survey the relative amounts of suspendable road dust on approximately 300 miles of paved roads. The system provides a unique perspective on road dust sources and their spatial distribution. Results of this study indicated that the difference of the PM 10 concentrations measured behind the tire and on the hood is exponentially related to vehicle speed. This was an interesting finding because current AP-42 road dust emissions estimation methods do not include vehicle speed as a factor in the emissions calculations. The experiment also demonstrated that the distribution of suspendable material on roadways is highly variable and that a large number of samples are needed to represent road dust emissions potential on an urban scale for a variety of road and activity conditions.

  20. Light absorbing organic aerosols (brown carbon) over the tropical Indian Ocean: impact of biomass burning emissions

    International Nuclear Information System (INIS)

    Srinivas, Bikkina; Sarin, M M

    2013-01-01

    The first field measurements of light absorbing water-soluble organic carbon (WSOC), referred as brown carbon (BrC), have been made in the marine atmospheric boundary layer (MABL) during the continental outflow to the Bay of Bengal (BoB) and the Arabian Sea (ARS). The absorption signal measured at 365 nm in aqueous extracts of aerosols shows a systematic linear increase with WSOC concentration, suggesting a significant contribution from BrC to the absorption properties of organic aerosols. The mass absorption coefficient (b abs ) of BrC shows an inverse hyperbolic relation with wavelength (from ∼300 to 700 nm), providing an estimate of the Angstrom exponent (α P , range: 3–19; Av: 9 ± 3). The mass absorption efficiency of brown carbon (σ abs−BrC ) in the MABL varies from 0.17 to 0.72 m 2  g −1 (Av: 0.45 ± 0.14 m 2  g −1 ). The α P and σ abs−BrC over the BoB are quite similar to that studied from a sampling site in the Indo-Gangetic Plain (IGP), suggesting the dominant impact of organic aerosols associated with the continental outflow. A comparison of the mass absorption efficiency of BrC and elemental carbon (EC) brings to focus the significant role of light absorbing organic aerosols (from biomass burning emissions) in atmospheric radiative forcing over oceanic regions located downwind of the pollution sources. (letter)

  1. Time-resolved analysis of particle emissions from residential biomass combustion - Emissions of refractory black carbon, PAHs and organic tracers

    Science.gov (United States)

    Nielsen, Ingeborg E.; Eriksson, Axel C.; Lindgren, Robert; Martinsson, Johan; Nyström, Robin; Nordin, Erik Z.; Sadiktsis, Ioannis; Boman, Christoffer; Nøjgaard, Jacob K.; Pagels, Joakim

    2017-09-01

    Time-resolved particle emissions from a conventional wood stove were investigated with aerosol mass spectrometry to provide links between combustion conditions, emission factors, mixing state of refractory black carbon and implications for organic tracer methods. The addition of a new batch of fuel results in low temperature pyrolysis as the fuel heats up, resulting in strong, short-lived, variable emission peaks of organic aerosol-containing markers of anhydrous sugars, such as levoglucosan (fragment at m/z 60). Flaming combustion results in emissions dominated by refractory black carbon co-emitted with minor fractions of organic aerosol and markers of anhydrous sugars. Full cycle emissions are an external mixture of larger organic aerosol-dominated and smaller thinly coated refractory black carbon particles. A very high burn rate results in increased full cycle mass emission factors of 66, 2.7, 2.8 and 1.3 for particulate polycyclic aromatic hydrocarbons, refractory black carbon, total organic aerosol and m/z 60, respectively, compared to nominal burn rate. Polycyclic aromatic hydrocarbons are primarily associated with refractory black carbon-containing particles. We hypothesize that at very high burn rates, the central parts of the combustion zone become air starved, leading to a locally reduced combustion temperature that reduces the conversion rates from polycyclic aromatic hydrocarbons to refractory black carbon. This facilitates a strong increase of polycyclic aromatic hydrocarbons emissions. At nominal burn rates, full cycle emissions based on m/z 60 correlate well with organic aerosol, refractory black carbon and particulate matter. However, at higher burn rates, m/z 60 does not correlate with increased emissions of polycyclic aromatic hydrocarbons, refractory black carbon and organic aerosol in the flaming phase. The new knowledge can be used to advance source apportionment studies, reduce emissions of genotoxic compounds and model the climate impacts of

  2. Diurnal cycling of urban aerosols under different weather regimes

    Science.gov (United States)

    Gregorič, Asta; Drinovec, Luka; Močnik, Griša; Remškar, Maja; Vaupotič, Janja; Stanič, Samo

    2016-04-01

    A one month measurement campaign was performed in summer 2014 in Ljubljana, the capital of Slovenia (population 280,000), aiming to study temporal and spatial distribution of urban aerosols and the mixing state of primary and secondary aerosols. Two background locations were chosen for this purpose, the first one in the city center (urban background - KIS) and the second one in the suburban background (Brezovica). Simultaneous measurements of black carbon (BC) and particle number size distribution of submicron aerosols (PM1) were conducted at both locations. In the summer season emission from traffic related sources is expected to be the main local contribution to BC concentration. Concentrations of aerosol species and gaseous pollutants within the planetary boundary layer are controlled by the balance between emission sources of primary aerosols and gases, production of secondary aerosols, chemical reactions of precursor gases under solar radiation and the rate of dilution by mixing within the planetary boundary layer (PBL) as well as with tropospheric air. Only local emission sources contribute to BC concentration during the stable PBL with low mixing layer height, whereas during the time of fully mixed PBL, regionally transported BC and other aerosols can contribute to the surface measurements. The study describes the diurnal behaviour of the submicron aerosol at the urban and suburban background location under different weather regimes. Particles in three size modes - nucleation (humidity, wind speed and direction), diurnal profile differs for sunny, cloudy and rainy days. Nucleation mode particles were found to be subjected to lower daily variation and only slightly influenced by weather, as opposed to Aitken and accumulation mode particles. The highest correlation between BC and particle number concentration is observed during stable atmospheric conditions in the night and morning hours and is attributed to different particle size modes, depending on the

  3. Wildland fire emissions, carbon, and climate: Emission factors

    Science.gov (United States)

    Shawn Urbanski

    2014-01-01

    While the vast majority of carbon emitted by wildland fires is released as CO2, CO, and CH4, wildland fire smoke is nonetheless a rich and complex mixture of gases and aerosols. Primary emissions include significant amounts of CH4 and aerosol (organic aerosol and black carbon), which are short-lived climate forcers. In addition to CO2 and short-lived climate forcers,...

  4. The impact of bark beetle infestations on monoterpene emissions and secondary organic aerosol formation in western North America

    Directory of Open Access Journals (Sweden)

    A. R. Berg

    2013-03-01

    Full Text Available Over the last decade, extensive beetle outbreaks in western North America have destroyed over 100 000 km2 of forest throughout British Columbia and the western United States. Beetle infestations impact monoterpene emissions through both decreased emissions as trees are killed (mortality effect and increased emissions in trees under attack (attack effect. We use 14 yr of beetle-induced tree mortality data together with beetle-induced monoterpene emission data in the National Center for Atmospheric Research (NCAR Community Earth System Model (CESM to investigate the impact of beetle-induced tree mortality and attack on monoterpene emissions and secondary organic aerosol (SOA formation in western North America. Regionally, beetle infestations may have a significant impact on monoterpene emissions and SOA concentrations, with up to a 4-fold increase in monoterpene emissions and up to a 40% increase in SOA concentrations in some years (in a scenario where the attack effect is based on observed lodgepole pine response. Responses to beetle attack depend on the extent of previous mortality and the number of trees under attack in a given year, which can vary greatly over space and time. Simulated enhancements peak in 2004 (British Columbia and 2008 (US. Responses to beetle attack are shown to be substantially larger (up to a 3-fold localized increase in summertime SOA concentrations in a scenario based on bark-beetle attack in spruce trees. Placed in the context of observations from the IMPROVE network, the changes in SOA concentrations due to beetle attack are in most cases small compared to the large annual and interannual variability in total organic aerosol which is driven by wildfire activity in western North America. This indicates that most beetle-induced SOA changes are not likely detectable in current observation networks; however, these changes may impede efforts to achieve natural visibility conditions in the national parks and wilderness

  5. TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

    Energy Technology Data Exchange (ETDEWEB)

    Annette Rohr

    2005-03-31

    This report documents progress made on the subject project during the period of September 1, 2004 through February 28, 2005. The TERESA Study is designed to investigate the role played by specific emissions sources and components in the induction of adverse health effects by examining the relative toxicity of coal combustion and mobile source (gasoline and/or diesel engine) emissions and their oxidative products. The study involves on-site sampling, dilution, and aging of coal combustion emissions at three coal-fired power plants, as well as mobile source emissions, followed by animal exposures incorporating a number of toxicological endpoints. The DOE-EPRI Cooperative Agreement (henceforth referred to as ''the Agreement'') for which this technical progress report has been prepared covers the performance and analysis of field experiments at the first TERESA plant, located in the Upper Midwest and henceforth referred to as Plant 0, and at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. During this reporting period, all fieldwork at Plant 0 was completed. Stack sampling was conducted in October to determine if there were significant differences between the in-stack PM concentrations and the diluted concentrations used for the animal exposures. Results indicated no significant differences and therefore confidence that the revised stack sampling methodology described in the previous semiannual report is appropriate for use in the Project. Animal exposures to three atmospheric scenarios were carried out. From October 4-7, we conducted exposures to oxidized emissions with the addition of secondary organic aerosol (SOA). Later in October, exposures to the most complex scenario (oxidized, neutralized emissions plus SOA) were repeated to ensure comparability with the results of the June/July exposures where a different stack sampling setup was employed. In November, exposures

  6. MODIS Observation of Aerosols over Southern Africa During SAFARI 2000: Data, Validation, and Estimation of Aerosol Radiative Forcing

    Science.gov (United States)

    Ichoku, Charles; Kaufman, Yoram; Remer, Lorraine; Chu, D. Allen; Mattoo, Shana; Tanre, Didier; Levy, Robert; Li, Rong-Rong; Kleidman, Richard; Lau, William K. M. (Technical Monitor)

    2001-01-01

    Aerosol properties, including optical thickness and size parameters, are retrieved operationally from the MODIS sensor onboard the Terra satellite launched on 18 December 1999. The predominant aerosol type over the Southern African region is smoke, which is generated from biomass burning on land and transported over the southern Atlantic Ocean. The SAFARI-2000 period experienced smoke aerosol emissions from the regular biomass burning activities as well as from the prescribed burns administered on the auspices of the experiment. The MODIS Aerosol Science Team (MAST) formulates and implements strategies for the retrieval of aerosol products from MODIS, as well as for validating and analyzing them in order to estimate aerosol effects in the radiative forcing of climate as accurately as possible. These activities are carried out not only from a global perspective, but also with a focus on specific regions identified as having interesting characteristics, such as the biomass burning phenomenon in southern Africa and the associated smoke aerosol, particulate, and trace gas emissions. Indeed, the SAFARI-2000 aerosol measurements from the ground and from aircraft, along with MODIS, provide excellent data sources for a more intensive validation and a closer study of the aerosol characteristics over Southern Africa. The SAFARI-2000 ground-based measurements of aerosol optical thickness (AOT) from both the automatic Aerosol Robotic Network (AERONET) and handheld Sun photometers have been used to validate MODIS retrievals, based on a sophisticated spatio-temporal technique. The average global monthly distribution of aerosol from MODIS has been combined with other data to calculate the southern African aerosol daily averaged (24 hr) radiative forcing over the ocean for September 2000. It is estimated that on the average, for cloud free conditions over an area of 9 million square kin, this predominantly smoke aerosol exerts a forcing of -30 W/square m C lose to the terrestrial

  7. The European aerosol budget in 2006

    Directory of Open Access Journals (Sweden)

    J. M. J. Aan de Brugh

    2011-02-01

    Full Text Available This paper presents the aerosol budget over Europe in 2006 calculated with the global transport model TM5 coupled to the size-resolved aerosol module M7. Comparison with ground observations indicates that the model reproduces the observed concentrations quite well with an expected slight underestimation of PM10 due to missing emissions (e.g. resuspension. We model that a little less than half of the anthropogenic aerosols emitted in Europe are exported and the rest is removed by deposition. The anthropogenic aerosols are removed mostly by rain (95% and only 5% is removed by dry deposition. For the larger natural aerosols, especially sea salt, a larger fraction is removed by dry processes (sea salt: 70%, mineral dust: 35%. We model transport of aerosols in the jet stream in the higher atmosphere and an import of Sahara dust from the south at high altitudes. Comparison with optical measurements shows that the model reproduces the Ångström parameter very well, which indicates a correct simulation of the aerosol size distribution. However, we underestimate the aerosol optical depth. Because the surface concentrations are close to the observations, the shortage of aerosol in the model is probably at higher altitudes. We show that the discrepancies are mainly caused by an overestimation of wet-removal rates. To match the observations, the wet-removal rates have to be scaled down by a factor of about 5. In that case the modelled ground-level concentrations of sulphate and sea salt increase by 50% (which deteriorates the match, while other components stay roughly the same. Finally, it is shown that in particular events, improved fire emission estimates may significantly improve the ability of the model to simulate the aerosol optical depth. We stress that discrepancies in aerosol models can be adequately analysed if all models would provide (regional aerosol budgets, as presented in the current study.

  8. Uncertainties in modelling the spatial and temporal variations in aerosol concentrations

    NARCIS (Netherlands)

    Meij, de A.

    2009-01-01

    Aerosols play a key role in air quality (health aspects) and climate. In this thesis atmospheric chemistry transport models are used to study the uncertainties in aerosol modelling and to evaluate the effects of emission reduction scenarios on air quality. Uncertainties in: the emissions of gas and

  9. Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

    Science.gov (United States)

    Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

    2015-06-01

    Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

  10. Geophysical applicability of aerosol size distribution measurements using cascade impactors and proton induced X-ray emission

    International Nuclear Information System (INIS)

    Van Grieken, R.E.; Johansson, T.B.; Akselsson, K.R.; Winchester, J.W.; Nelson, J.W.; Chapman, K.R.

    1976-01-01

    Proton Induced X-ray Emission, (PIXE), is capable of high precision analysis for trace element components of aerosol particle size fractions sampled by cascade impactor. A statistical evaluation of data quality has been carried out in order to distinguish between analytical uncertainties in the PIXE procedure, errors caused by cascade impactor performance and by other factors in the sampling procedure, and geophysical causes of differences in composition and particle size distributions of the elements in aerosols. Replicate analyses and simultaneous samplings taken in north Florida and St. Louis have been used for the data evaluation. In addition to the analytical error the sampling procedure contributes an error of approximately 10% to be added quadratically. The resulting precision is sufficient to evaluate the data in geophysical terms. This is illustrated by means of sample sets taken simultaneously in an urban, forest and coastal environment of the same region. (author)

  11. Sea Spray Aerosols

    DEFF Research Database (Denmark)

    Butcher, Andrew Charles

    emissions produced directly from bubble bursting as the result of air entrainment from breaking waves and particles generated from secondary emissions of volatile organic compounds. In the first paper, we study the chemical properties of particles produced from several sea water proxies with the use...... of a cloud condensation nuclei ounter. Proxy solutions with high inorganic salt concentrations and some organics produce sea spray aerosol particles with little change in cloud condensation activity relative to pure salts. Comparison is made between a frit based method for bubble production and a plunging...... a relationship between plunging jet particle ux, oceanic particle ux, and energy dissipation rate in both systems. Previous sea spray aerosol studies dissipate an order of magnitude more energy for the same particle ux production as the open ocean. A scaling factor related to the energy expended in air...

  12. Fingerprinting groundwater salinity sources in the Gulf Coast Aquifer System, USA

    Science.gov (United States)

    Chowdhury, Ali H.; Scanlon, Bridget R.; Reedy, Robert C.; Young, Steve

    2018-02-01

    Understanding groundwater salinity sources in the Gulf Coast Aquifer System (GCAS) is a critical issue due to depletion of fresh groundwater and concerns for potential seawater intrusion. The study objective was to assess sources of groundwater salinity in the GCAS using ˜1,400 chemical analyses and ˜90 isotopic analyses along nine well transects in the Texas Gulf Coast, USA. Salinity increases from northeast (median total dissolved solids (TDS) 340 mg/L) to southwest (median TDS 1,160 mg/L), which inversely correlates with the precipitation distribution pattern (1,370- 600 mm/yr, respectively). Molar Cl/Br ratios (median 540-600), depleted δ2H and δ18O (-24.7‰, -4.5‰) relative to seawater (Cl/Br ˜655 and δ2H, δ18O 0‰, 0‰, respectively), and elevated 36Cl/Cl ratios (˜100), suggest precipitation enriched with marine aerosols as the dominant salinity source. Mass balance estimates suggest that marine aerosols could adequately explain salt loading over the large expanse of the GCAS. Evapotranspiration enrichment to the southwest is supported by elevated chloride concentrations in soil profiles and higher δ18O. Secondary salinity sources include dissolution of salt domes or upwelling brines from geopressured zones along growth faults, mainly near the coast in the northeast. The regional extent and large quantities of brackish water have the potential to support moderate-sized desalination plants in this location. These results have important implications for groundwater management, suggesting a current lack of regional seawater intrusion and a suitable source of relatively low TDS water for desalination.

  13. Nuclear analytical techniques applied to characterization of atmospheric aerosols in Amazon Region

    International Nuclear Information System (INIS)

    Gerab, Fabio; Artaxo, Paulo

    1996-01-01

    This work presents the atmospheric aerosols characterization that exist in different regions of Amazon basin. The biogenic aerosol emission by forest, as well as the atmospheric emissions of particulate materials due to biomass burning, were analyzed. Samples of aerosol particles were collected during three years in two different locations of Amazon region using Stacked Unit Filters. In order to study these samples some analytical nuclear techniques were used. The high concentrations of aerosols as a result of biomass burning process were observed in the period of june-september

  14. The impact of biogenic carbon emissions on aerosol absorption inMexico City

    Energy Technology Data Exchange (ETDEWEB)

    Marley, N; Gaffney, J; Tackett, M J; Sturchio, N; Hearty, L; Martinez, N; Hardy, K D; Machany-Rivera, A; Guilderson, T P; MacMillan, A; Steelman, K

    2009-02-24

    In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbing secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.

  15. Primary marine aerosol emissions from the Mediterranean Sea during pre-bloom and oligotrophic conditions: correlations to seawater chlorophyll a from a mesocosm study

    Science.gov (United States)

    Schwier, A. N.; Rose, C.; Asmi, E.; Ebling, A. M.; Landing, W. M.; Marro, S.; Pedrotti, M.-L.; Sallon, A.; Iuculano, F.; Agusti, S.; Tsiola, A.; Pitta, P.; Louis, J.; Guieu, C.; Gazeau, F.; Sellegri, K.

    2015-07-01

    The effect of ocean acidification and changing water conditions on primary (and secondary) marine aerosol emissions is not well understood on a regional or a global scale. To investigate this effect as well as the indirect effect on aerosol that changing biogeochemical parameters can have, ~ 52 m3 pelagic mesocosms were deployed for several weeks in the Mediterranean Sea during both winter pre-bloom and summer oligotrophic conditions and were subjected to various levels of CO2 to simulate the conditions foreseen in this region for the coming decades. After seawater sampling, primary bubble-bursting aerosol experiments were performed using a plunging water jet system to test both chemical and physical aerosol parameters (10-400 nm). Comparing results obtained during pre-bloom and oligotrophic conditions, we find the same four log-normal modal diameters (18.5 ± 0.6, 37.5 ± 1.4, 91.5 ± 2.0, 260 ± 3.2 nm) describing the aerosol size distribution during both campaigns, yet pre-bloom conditions significantly increased the number fraction of the second (Aitken) mode, with an amplitude correlated to virus-like particles, heterotrophic prokaryotes, TEPs (transparent exopolymeric particles), chlorophyll a and other pigments. Organic fractions determined from kappa closure calculations for the diameter, Dp ~ 50 nm, were much larger during the pre-bloom period (64 %) than during the oligotrophic period (38 %), and the organic fraction decreased as the particle size increased. Combining data from both campaigns together, strong positive correlations were found between the organic fraction of the aerosol and chlorophyll a concentrations, heterotrophic and autotrophic bacteria abundance, and dissolved organic carbon (DOC) concentrations. As a consequence of the changes in the organic fraction and the size distributions between pre-bloom and oligotrophic periods, we find that the ratio of cloud condensation nuclei (CCN) to condensation nuclei (CN) slightly decreased during the

  16. Comprehensive Measurement of Atmospheric Aerosols with a Wide Range Aerosol Spectrometer

    International Nuclear Information System (INIS)

    Keck, L; Pesch, M; Grimm, H

    2011-01-01

    A wide range aerosol spectrometer (WRAS) was used for comprehensive long term measurements of aerosol size distributions. The system combines the results of an optical aerosol spectrometer with the results of a Scanning Mobility Particle Sizer (SMPS) to record essentially the full size range (5 nm - 32 μm) of atmospheric particles in 72 channels. Measurements were carried out over one year (2009) at the Global Atmospheric Watch (GAW)-Station Hohenpeissenberg, Bavaria. Total particle number concentrations obtained from the aerosol size distributions were compared to the total number concentrations measured by a Condensation Particle Counter (CPC). The comparison showed an excellent agreement of the data. The high time resolution of 5 minutes allows the combination of the measured size distributions with meteorological data and correlations to gaseous pollutants (CO, NOx and SO2). A good correlation of particle number and CO concentrations was found for long distance transported small particles, which were probably mainly soot particles. Correlations to NOx were observed for aerosols from local sources such as traffic emissions. The formation of secondary aerosols from gaseous precursors was also observed. Episodes of relatively high concentration of particles in the range of 2-3 μm were probably caused by pollen.

  17. Evaluating Simulated Primary Anthropogenic and Biomass Burning Organic Aerosols during MILAGRO: Implications for Assessing Treatments of Secondary Organic Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Fast, Jerome D.; Aiken, Allison; Allan, James D.; Alexander, M. L.; Campos, Teresa; Canagaratna, Manjula R.; Chapman, Elaine G.; DeCarlo, Peter; de Foy, B.; Gaffney, Jeffrey; de Gouw, Joost A.; Doran, J. C.; Emmons, L.; Hodzic, Alma; Herndon, Scott C.; Huey, L. G.; Jayne, John T.; Jimenez, Jose L.; Kleinman, Lawrence I.; Kuster, W. C.; Marley, Nancy A.; Russell, Lynn M.; Ochoa, Carlos; Onasch, Timothy B.; Pekour, Mikhail S.; Song, Chen; Ulbrich, Ingrid M.; Warneke, Carsten; Welsh-Bon, Daniel; Wiedinmyer, Christine; Worsnop, Douglas R.; Yu, Xiao-Ying; Zaveri, Rahul A.

    2009-08-31

    Simulated primary organic aerosols (POA), as well as other particulates and trace gases, in the vicinity of Mexico City are evaluated using measurements collected during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaigns. Since the emission inventories and dilution will affect predictions of total organic matter and consequently total particulate matter, our objective is to assess the uncertainties in predicted POA before testing and evaluating the performance of secondary organic aerosol (SOA) treatments. Carbon monoxide (CO) is well simulated on most days both over the city and downwind, indicating that transport and mixing processes were usually consistent with the meteorological conditions observed during MILAGRO. Predicted and observed elemental carbon (EC) in the city was similar, but larger errors occurred at remote locations since the CO/EC emission ratios in the national emission inventory were lower than in the metropolitan emission inventory. Components of organic aerosols derived from Positive Matrix Factorization and data from several Aerodyne Aerosol Mass Spectrometer instruments deployed both at ground sites and on research aircraft are used to evaluate the model. Predicted POA was consistently lower than the measured organic matter at the ground sites, which is consistent with the expectation that SOA should be a large fraction of the total organic matter mass. A much better agreement was found when predicted POA was compared with the sum of "primary anthropogenic" and "primary biomass burning" components on days with relatively low biomass burning, suggesting that the overall magnitude of primary organic particulates released was reasonable. The predicted POA was greater than the total observed organic matter when the aircraft flew directly downwind of large fires, suggesting that biomass burning emission estimates from some large fires may be too high. Predicted total observed organic carbon (TOOC) was

  18. Characterization of organic aerosols in Beirut, Lebanon

    International Nuclear Information System (INIS)

    Waked, Antoine

    2012-01-01

    The chemical composition of PM2.5 includes both organic and inorganic compounds. Organic compounds, which constitute a significant fraction of the PM2.5 mass, can be emitted directly as primary aerosol from sources such as fossil-fuel combustion, biomass burning, and natural biogenic emissions, or formed in the atmosphere via chemical reactions leading to secondary organic aerosol (SOA) formation. SOA, which account for 20 - 80 % of total organic aerosol, are currently a major source of uncertainty in air quality modeling. The identification and quantification of the chemical composition of the organic fraction of PM2.5 and its source apportionment are of great interest, especially in the Middle East region where data on organic aerosols are currently lacking. Lebanon, a small developing country in the Middle East region located on the eastern shore of the Mediterranean basin represents a good example for characterizing organic aerosols in this region. To address this issue, the air quality in Beirut (the capital city of Lebanon) was investigated with a focus on organic aerosols. First, an air pollutant emission inventory was developed for Lebanon with a spatial resolution of 5 km x 5 km and for Beirut with a spatial resolution of 1 km x 1 km. The results obtained show that the road transport sector is the major contributor to carbon monoxide (CO), nitrogen oxides (NO x ) and non-methane volatile organic compounds (VOC) emissions, whereas fossil fuel-fired power plants and large industrial plants are the major contributors to sulfur dioxide (SO 2 ) and primary particulate matter (PM) emissions. Then, two intensive 15-day measurement campaigns were conducted at a semi-urban site located in a Beirut suburb to characterize air pollutant concentrations. The first measurement campaign took place in July 2011 and the second in February 2012. Measurements included PM2.5, organic carbon (OC) and elemental carbon (EC) mass concentrations as well as a molecular

  19. Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Shrivastava, Manish [Pacific Northwest National Laboratory, Richland Washington USA; Cappa, Christopher D. [Department of Civil and Environmental Engineering, University of California, Davis California USA; Fan, Jiwen [Pacific Northwest National Laboratory, Richland Washington USA; Goldstein, Allen H. [Department of Environmental Science, Policy and Management and Department of Civil and Environmental Engineering, University of California, Berkeley California USA; Guenther, Alex B. [Department of Earth System Science, University of California, Irvine California USA; Jimenez, Jose L. [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Kuang, Chongai [Brookhaven National Laboratory, Upton New York USA; Laskin, Alexander [Pacific Northwest National Laboratory, Richland Washington USA; Martin, Scot T. [School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge Massachusetts USA; Ng, Nga Lee [School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA; Petaja, Tuukka [Department of Physics, University of Helsinki, Helsinki Finland; Pierce, Jeffrey R. [Department of Atmospheric Science, Colorado State University, Fort Collins Colorado USA; Rasch, Philip J. [Pacific Northwest National Laboratory, Richland Washington USA; Roldin, Pontus [Department of Physics, Lund University, Lund Sweden; Seinfeld, John H. [Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena California USA; Shilling, John [Pacific Northwest National Laboratory, Richland Washington USA; Smith, James N. [Department of Earth System Science, University of California, Irvine California USA; Thornton, Joel A. [Department of Atmospheric Sciences, University of Washington, Seattle Washington USA; Volkamer, Rainer [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Wang, Jian [Brookhaven National Laboratory, Upton New York USA; Worsnop, Douglas R. [Aerodyne Research, Inc., Billerica Massachusetts USA; Zaveri, Rahul A. [Pacific Northwest National Laboratory, Richland Washington USA; Zelenyuk, Alla [Pacific Northwest National Laboratory, Richland Washington USA; Zhang, Qi [Department of Environmental Toxicology, University of California, Davis California USA

    2017-06-01

    Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combination of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol

  20. Seasonal dependence of aerosol processing in urban Philadelphia

    Science.gov (United States)

    Avery, A. M.; Waring, M. S.; DeCarlo, P. F.

    2017-12-01

    Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower

  1. Long-term trends in California mobile source emissions and ambient concentrations of black carbon and organic aerosol.

    Science.gov (United States)

    McDonald, Brian C; Goldstein, Allen H; Harley, Robert A

    2015-04-21

    A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends.

  2. Causes and consequences of decreasing atmospheric organic aerosol in the United States

    Science.gov (United States)

    Ridley, D. A.; Heald, C. L.; Ridley, K. J.; Kroll, J. H.

    2018-01-01

    Exposure to atmospheric particulate matter (PM) exacerbates respiratory and cardiovascular conditions and is a leading source of premature mortality globally. Organic aerosol contributes a significant fraction of PM in the United States. Here, using surface observations between 1990 and 2012, we show that organic carbon has declined dramatically across the entire United States by 25–50%; accounting for more than 30% of the US-wide decline in PM. The decline is in contrast with the increasing organic aerosol due to wildfires and no clear trend in biogenic emissions. By developing a carbonaceous emissions database for the United States, we show that at least two-thirds of the decline in organic aerosol can be explained by changes in anthropogenic emissions, primarily from vehicle emissions and residential fuel burning. We estimate that the decrease in anthropogenic organic aerosol is responsible for averting 180,000 (117,000–389,000) premature deaths between 1990 and 2012. The unexpected decrease in organic aerosol, likely a consequence of the implementation of Clean Air Act Amendments, results in 84,000 (30,000–164,000) more lives saved than anticipated by the EPA between 2000 and 2010.

  3. Simulation of the interannual variations of biogenic emissions of volatile organic compounds in China: Impacts on tropospheric ozone and secondary organic aerosol

    Science.gov (United States)

    Fu, Y.; Liao, H.

    2012-12-01

    We use the MEGAN (Model of emissions of Gases and Aerosols from Nature) module embedded within the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to simulate the interannual variations in biogenic volatile organic compound (BVOC) emissions and concentrations of ozone and secondary organic aerosols (SOA) in China over years 2001-2006. To have better representation of biogenic emissions, we have updated in the model the land cover and leaf area index in China using Moderate Resolution Imaging Spectroradiometer (MODIS) satellite measurements, and we have developed a new classification of vegetation with 21 plant functional types. Estimated annual BVOC emission in China averaged over 2001-2006 is 18.85 Tg C yr-1, in which emissions of isoprene, monoterpenes, and other reactive volatile organic compounds account for 50.9%, 15.0%, and 34.1%, respectively. The simulated BVOC emissions in China have large interannual variations. The values of regionally averaged absolute percent departure from the mean (APDM) of isoprene emissions are in the range of 21-42% in January and 15-28% in July. The APDM values of monoterpene emissions are 14-32% in January and 10-21% in July, which are generally smaller than those of isoprene emissions. Model results indicate that the interannual variations in isoprene emissions are more dependent on variations in meteorological fields, whereas the interannual variations in monoterpene emissions are more sensitive to changes in vegetation parameters. With fixed anthropogenic emissions, as a result of the variations in both meteorological parameters and vegetation, simulated O3 concentrations show interannual variations of 0.8-5 ppbv (or largest APDM values of 4-15%), and simulated SOA shows APDM values of 5-15% in southwestern China in January as well as 10-25% in southeastern and 20-35% in northeastern China in July. On a regional mean basis, the interannual variations in BVOCs alone can lead to 2

  4. Impacts of East Asian Sulfate Aerosols on Local and Remote Climate

    Science.gov (United States)

    Bartlett, R. E.; Bollasina, M. A.

    2017-12-01

    Anthropogenic aerosols exert significant climate forcing, which increases with emissions following trends of growing population and industry. Globally, aerosols cause a net cooling, counteracting greenhouse gas warming; however, regional impacts vary since emissions are spatially and temporally heterogeneous. While European and North American emissions have decreased in recent decades, Asian, particularly East Asian, emissions continued to rise into the 21st century. In addition to links between Asian anthropogenic aerosols and significant local climate impacts - for example, changes to the Asian monsoon system - studies have also shown influences on remote climate. Sulfate aerosols are particularly important for East Asia, remaining at constant levels higher than column burdens of other aerosol species. If a concerted effort - as laid out by government policies aiming to improve air quality - is made, the effects of anthropogenic aerosols (due to their short atmospheric lifetime) could be quickly reversed. Thus, it is vital to understand the climate impact aerosols have had up to now to aid in determining what will happen in the future. We use transient climate modelling experiments with the Community Earth System Model to investigate the impacts of East Asian sulfate aerosols in the present day compared to 1950 (i.e. before rapid industrialisation in this region), focusing on dynamical mechanisms leading to the occurrence of such impacts, and how their influence can spread to remote regions. We find, in addition to significant monsoon impacts, noticeable shifts in large-scale circulation features such as the ITCZ and the Pacific Walker cell. Through diabatic heating responses, changes to upper-level atmospheric dynamics are evident, leading to downstream effects on surface climate - for example, surface cooling over Europe. Understanding of these impacts is vital when considering how the good intentions of air quality improvement might inadvertently have

  5. Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

    Science.gov (United States)

    Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary...

  6. PREP-CHEM-SRC – 1.0: a preprocessor of trace gas and aerosol emission fields for regional and global atmospheric chemistry models

    Directory of Open Access Journals (Sweden)

    S. R. Freitas

    2011-05-01

    Full Text Available The preprocessor PREP-CHEM-SRC presented in the paper is a comprehensive tool aiming at preparing emission fields of trace gases and aerosols for use in atmospheric-chemistry transport models. The considered emissions are from the most recent databases of urban/industrial, biogenic, biomass burning, volcanic, biofuel use and burning from agricultural waste sources. For biomass burning, emissions can be also estimated directly from satellite fire detections using a fire emission model included in the tool. The preprocessor provides emission fields interpolated onto the transport model grid. Several map projections can be chosen. The inclusion of these emissions in transport models is also presented. The preprocessor is coded using Fortran90 and C and is driven by a namelist allowing the user to choose the type of emissions and the databases.

  7. Primary marine aerosol emissions from the Mediterranean Sea during pre-bloom and oligotrophic conditions: correlations to seawater chlorophyll a from a mesocosm study

    OpenAIRE

    Schwier , A. N.; Rose , C.; Asmi , E.; Ebling , A. M.; Landing , W. M.; Marro , S.; Pedrotti , M.-L.; Sallon , A.; Iuculano , F.; Agusti , S.; Tsiola , A.; Pitta , P.; Louis , J.; Guieu , C.; Gazeau , F.

    2015-01-01

    The effect of ocean acidification and changing water conditions on primary (and secondary) marine aerosol emissions is not well understood on a regional or a global scale. To investigate this effect as well as the indirect effect on aerosol that changing biogeochemical parameters can have, ~ 52 m3 pelagic mesocosms were deployed for several weeks in the Mediterranean Sea during both winter pre-bloom and summer oligotrophic conditions and were subjected to various levels of C...

  8. Proton-Induced X-Ray Emission Analysis of Crematorium Emissions

    Science.gov (United States)

    Ali, Salina; Nadareski, Benjamin; Yoskowitz, Joshua; Labrake, Scott; Vineyard, Michael

    2014-09-01

    There has been considerable debate in recent years about possible mercury emissions from crematoria due to amalgam tooth restorations. We have performed a proton-induced X-ray emission (PIXE) analysis of aerosol and soil samples taken near the Vale Cemetery Crematorium in Schenectady, NY, to address this concern. The aerosol samples were collected on the roof of the crematorium using a nine-stage, cascade impactor that separates the particulate matter by aerodynamic diameter and deposits it onto thin Kapton foils. The soil samples were collected at several different distances from the crematorium and compressed into pellets with a hydraulic press. The Kapton foils containing the aerosol samples and the soil pellets were bombarded with 2.2-MeV protons from the 1.1-MV tandem Pelletron accelerator in the Union College Ion-Beam Analysis Laboratory. We measured significant concentrations of sulfur, phosphorus, potassium, calcium, and iron, but essentially no mercury in the aerosol samples. The lower limit of detection for airborne mercury in this experiment was approximately 0.2 ng / m3. The PIXE analysis of the soil samples showed the presence of elements commonly found in soil (Si, K, Ca, Ti, Mn, Fe), but no trace of mercury. There has been considerable debate in recent years about possible mercury emissions from crematoria due to amalgam tooth restorations. We have performed a proton-induced X-ray emission (PIXE) analysis of aerosol and soil samples taken near the Vale Cemetery Crematorium in Schenectady, NY, to address this concern. The aerosol samples were collected on the roof of the crematorium using a nine-stage, cascade impactor that separates the particulate matter by aerodynamic diameter and deposits it onto thin Kapton foils. The soil samples were collected at several different distances from the crematorium and compressed into pellets with a hydraulic press. The Kapton foils containing the aerosol samples and the soil pellets were bombarded with 2.2-Me

  9. Global aerosol transport and consequences for the radiation budget

    International Nuclear Information System (INIS)

    Newiger, M.; Grassl, H.; Schussel, P.; Rehkopf, J.

    1984-01-01

    Man's activities may influence global climate by changing the atmospheric composition and surface characteristics and by waste heat. Most prominent within this discussion is the increase or decrease of radiatively active trace gases like CO/sub 2/, N/sub 2/O, O/sub 3/, and others. The general opinion is converging towards a greenhouse effect as a combined action of all trace gases, whose exact magnitude is uncertain mainly because of the unknown reaction of water cycle. The aim of our global 2-D (resolving latitude and height) aerosol transport model is the calculation of aerosol particle number density profiles as a function of latitude for present natural plus anthropogenic emissions. The aerosol transport model uses prescribed meridonal circulation, diffusivity factors and cloud climatology for January as well as July. All these latitude and height dependent input parameters were taken from well known sources. The fixed climatology excludes the feedback of aerosol particle parameter changes on mean circulation. However, the radiative parameters of six clouds types are modified, although they possess by adoption of the Telegadas and London (1954) cloud climatology prescribed amount and height. The inclusion of the feedback on mean circulation seems premature at present. Adding particles either accounting for natural emissions or natural anthropogenic emission and removing particles by all known sinks outside and within clouds gives us - for the stationary state - vertical profiles of aerosol number density in three sizes classes as a function of latitude. These profiles in turn are input for radiation flux calculations in clear and cloudy areas in order to assess net flux changes caused by the present aerosol load in comparison to a scenario without anthropogenic emissions. The net flux changes finally are compared to those calculated for increased CO/sub 2/ levels

  10. A multi-model evaluation of aerosols over South Asia: common problems and possible causes

    Science.gov (United States)

    Pan, X.; Chin, M.; Gautam, R.; Bian, H.; Kim, D.; Colarco, P. R.; Diehl, T. L.; Takemura, T.; Pozzoli, L.; Tsigaridis, K.; Bauer, S.; Bellouin, N.

    2015-05-01

    Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, water cycle and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions. In this study, the spatio-temporal aerosol distributions over South Asia from seven global aerosol models are evaluated against aerosol retrievals from NASA satellite sensors and ground-based measurements for the period of 2000-2007. Overall, substantial underestimations of aerosol loading over South Asia are found systematically in most model simulations. Averaged over the entire South Asia, the annual mean aerosol optical depth (AOD) is underestimated by a range 15 to 44% across models compared to MISR (Multi-angle Imaging SpectroRadiometer), which is the lowest bound among various satellite AOD retrievals (from MISR, SeaWiFS (Sea-Viewing Wide Field-of-View Sensor), MODIS (Moderate Resolution Imaging Spectroradiometer) Aqua and Terra). In particular during the post-monsoon and wintertime periods (i.e., October-January), when agricultural waste burning and anthropogenic emissions dominate, models fail to capture AOD and aerosol absorption optical depth (AAOD) over the Indo-Gangetic Plain (IGP) compared to ground-based Aerosol Robotic Network (AERONET) sunphotometer measurements. The underestimations of aerosol loading in models generally occur in the lower troposphere (below 2 km) based on the comparisons of aerosol extinction profiles calculated by the models with those from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data. Furthermore, surface concentrations of all aerosol components (sulfate, nitrate, organic aerosol (OA) and black carbon (BC)) from the models are found much lower than in situ measurements in winter. Several possible causes for these common problems of underestimating aerosols in models during the post-monsoon and wintertime periods are identified: the aerosol hygroscopic growth and formation of

  11. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  12. Modeling aerosol suspension from soils and oceans as sources of micropollutants to air.

    Science.gov (United States)

    Qureshi, Asif; MacLeod, Matthew; Hungerbühler, Konrad

    2009-10-01

    Soil and marine aerosol suspension are two physical mass transfer processes that are not usually included in models describing fate and transport of environmental pollutants. Here, we review the literature on soil and marine aerosol suspension and estimate aerosol suspension mass transfer velocities for inclusion in multimedia models, as a global average and on a 1 x 1 scale. The yearly, global average mass transfer velocity for soil aerosol suspension is estimated to be 6 x 10(-10)mh(-1), approximately an order of magnitude smaller than marine aerosol suspension, which is estimated to be 8 x 10(-9)mh(-1). Monthly averages of these velocities can be as high as 10(-7)mh(-1) and 10(-5)mh(-1) for soil and marine aerosol suspension, respectively, depending on location. We use a unit-world multimedia model to analyze the relevance of these two suspension processes as a mechanism that enhances long-range atmospheric transport of pollutants. This is done by monitoring a metric of long-range transport potential, phi-one thousand (phi1000), that denotes the fraction of modeled emissions to air, water or soil in a source region that reaches a distance of 1000 km in air. We find that when the yearly, globally averaged mass transfer velocity is used, marine aerosol suspension increases phi1000 only fractionally for both emissions to air and water. However, enrichment of substances in marine aerosols, or speciation between ionic and neutral forms in ocean water may increase the influence of this surface-to-air transfer process. Soil aerosol suspension can be the dominant process for soil-to-air transfer in an emission-to-soil scenario for certain substances that have a high affinity to soil. When a suspension mass transfer velocity near the maximum limit is used, soil suspension remains important if the emissions are made to soil, and marine aerosol suspension becomes important regardless of if emissions are made to air or water compartments. We recommend that multimedia models

  13. Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Srivastava, A.K. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India); Ram, K. [Institute of Environment and Sustainable Development, Banaras Hindu University, Varanasi (India); Singh, Sachchidanand, E-mail: ssingh@nplindia.org [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Kumar, Sanjeev [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Tiwari, S. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India)

    2015-01-01

    The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm{sup −2}) and high values of corresponding heating rate (0.80 ± 0.14 Kday{sup −1}) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm{sup −2} and from − 3 to − 50 Wm{sup −2} at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm{sup −2} resulting in a heating rate of 0.1–1.8 Kday{sup −1}. - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed

  14. Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

    International Nuclear Information System (INIS)

    Srivastava, A.K.; Ram, K.; Singh, Sachchidanand; Kumar, Sanjeev; Tiwari, S.

    2015-01-01

    The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm −2 ) and high values of corresponding heating rate (0.80 ± 0.14 Kday −1 ) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm −2 and from − 3 to − 50 Wm −2 at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm −2 resulting in a heating rate of 0.1–1.8 Kday −1 . - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed over the station in the

  15. Receptor models for source apportionment of remote aerosols in Brazil

    International Nuclear Information System (INIS)

    Artaxo Netto, P.E.

    1985-11-01

    The PIXE (particle induced X-ray emission), and PESA (proton elastic scattering analysis) method were used in conjunction with receptor models for source apportionment of remote aerosols in Brazil. The PIXE used in the determination of concentration for elements with Z >- 11, has a detection limit of about 1 ng/m 3 . The concentrations of carbon, nitrogen and oxygen in the fine fraction of Amazon Basin aerosols was measured by PESA. We sampled in Jureia (SP), Fernando de Noronha, Arembepe (BA), Firminopolis (GO), Itaberai (GO) and Amazon Basin. For collecting the airbone particles we used cascade impactors, stacked filter units, and streaker samplers. Three receptor models were used: chemical mass balance, stepwise multiple regression analysis and principal factor analysis. The elemental and gravimetric concentrations were explained by the models within the experimental errors. Three sources of aerosol were quantitatively distinguished: marine aerosol, soil dust and aerosols related to forests. The emission of aerosols by vegetation is very clear for all the sampling sites. In Amazon Basin and Jureia it is the major source, responsible for 60 to 80% of airborne concentrations. (Author) [pt

  16. Data assimilation of CALIPSO aerosol observations

    Directory of Open Access Journals (Sweden)

    T. T. Sekiyama

    2010-01-01

    Full Text Available We have developed an advanced data assimilation system for a global aerosol model with a four-dimensional ensemble Kalman filter in which the Level 1B data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO were successfully assimilated for the first time, to the best of the authors' knowledge. A one-month data assimilation cycle experiment for dust, sulfate, and sea-salt aerosols was performed in May 2007. The results were validated via two independent observations: 1 the ground-based lidar network in East Asia, managed by the National Institute for Environmental Studies of Japan, and 2 weather reports of aeolian dust events in Japan. Detailed four-dimensional structures of aerosol outflows from source regions over oceans and continents for various particle types and sizes were well reproduced. The intensity of dust emission at each grid point was also corrected by this data assimilation system. These results are valuable for the comprehensive analysis of aerosol behavior as well as aerosol forecasting.

  17. Black carbon in aerosol during BIBLE B

    Science.gov (United States)

    Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

    2003-02-01

    The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

  18. Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

    Science.gov (United States)

    da Silva, Arlindo

    2010-01-01

    A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

  19. Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

    Directory of Open Access Journals (Sweden)

    B. Sič

    2015-02-01

    Full Text Available This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI, the ground (AERONET, EMEP, and a model inter-comparison project (AeroCom are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10 and a better correlation (from 0.06 to 0.32 in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16, and a negative MNMB in

  20. Improving Aerosol Simulation over South Asia for Climate and Air Quality Studies

    Science.gov (United States)

    Pan, Xiaohua; Chin, Mian; Bian, Huisheng; Gautam, Ritesh

    2014-01-01

    Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. However, it has been proved quite challenging to adequately represent the aerosol spatial distribution and magnitude over this critical region in global models (Pan et al. 2014), with the surface concentrations, aerosol optical depth (AOD), and absorbing AOD (AAOD) significantly underestimated, especially in October-January when the agricultural waste burning and anthropogenic aerosol dominate over dust aerosol. In this study, we aim to investigate the causes for such discrepancy in winter by conducting sets of model experiments with NASA's GEOS-5 in terms of (1) spatial resolution, (2) emission amount, and (3) meteorological fields.

  1. Aerosol Emissions from Great Lakes Harmful Algal Blooms

    Energy Technology Data Exchange (ETDEWEB)

    May, Nathaniel W. [Department; Olson, Nicole E. [Department; Panas, Mark [Department; Axson, Jessica L. [Department; Tirella, Peter S. [Department; Kirpes, Rachel M. [Department; Craig, Rebecca L. [Department; Gunsch, Matthew J. [Department; China, Swarup [William; Laskin, Alexander [William; Ault, Andrew P. [Department; Department; Pratt, Kerri A. [Department; Department

    2017-12-20

    In freshwater lakes, harmful algal blooms (HABs) of Cyanobacteria (blue-green algae) produce toxins that impact human health. However, little is known about the chemical species present in lake spray aerosol (LSA) produced from wave-breaking in freshwater HABs. In this study, a laboratory LSA generator produced aerosols from freshwater samples collected from Lake Michigan and Lake Erie during HAB and non-bloom conditions. Particles were analyzed for size and chemical composition by single particle mass spectrometry, electron microscopy, and fluorescence microscopy, with three distinct types of LSA identified with varying levels of organic carbon and biological material associated with calcium salts. LSA autofluorescence increases with blue-green algae concentration, showing that organic molecules of biological origin are incorporated in LSA from HABs. The number fraction of LSA with biological mass spectral markers also increases with particle diameter (greater than 0.5 μm), showing that HABs have size-dependent impacts on aerosol composition. The highest number fraction of LSA enriched in organic carbon were observed in particles less than 0.5 μm in diameter. Understanding the transfer of organic and biogenic material from freshwater to the atmosphere via LSA particles is crucial for determining health and climate effects due to HABs.

  2. How important is organic aerosol hygroscopicity to aerosol indirect forcing?

    International Nuclear Information System (INIS)

    Liu Xiaohong; Wang Jian

    2010-01-01

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR community atmospheric model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (represented by a single parameter 'κ' ) of POA and SOA. Our model simulation indicates that in the present-day (PD) condition changing the 'κ' value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S = 0.1% by 40-80% over the POA source regions, while changing the 'κ' value of SOA by ± 50% (from 0.14 to 0.07 and 0.21) changes the CCN concentration within 40%. There are disproportionally larger changes in CCN concentration in the pre-industrial (PI) condition. Due to the stronger impact of organics hygroscopicity on CCN and cloud droplet number concentration at PI condition, global annual mean anthropogenic aerosol indirect forcing (AIF) between PD and PI conditions reduces with the increase of the hygroscopicity of organics. Global annual mean AIF varies by 0.4 W m -2 in the sensitivity runs with the control run of - 1.3 W m -2 , highlighting the need for improved understanding of organics hygroscopicity and its representation in global models.

  3. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    Directory of Open Access Journals (Sweden)

    D. E. Young

    2016-05-01

    Full Text Available The San Joaquin Valley (SJV in California experiences persistent air-quality problems associated with elevated particulate matter (PM concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ campaign. The average submicron aerosol (PM1 concentration was 31.0 µg m−3 and the total mass was dominated by organic aerosols (OA, 55 %, followed by ammonium nitrate (35 %. High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C, hydrogen-to-carbon (H / C, and nitrogen-to-carbon (N / C ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09 associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19 associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60 most likely

  4. Atmospheric emitted radiance interferometer (AERI): Status and the aerosol explanation for extra window region emissions

    Energy Technology Data Exchange (ETDEWEB)

    Revercomb, H.E.; Knuteson, R.O.; Best, F.A.; Dirkx, T.P. [Univ. of Wisconsin, Madison, WI (United States)] [and others

    1996-04-01

    High spectral resolution observations of downwelling emission from 3 to 19 microns have been made by the Atmospheric Emitted Radiance Interferometer (AERI) Prototype at the Southern Great Plains (SGP) Cloud and Radiative Testbed (CART) site for over two years. The spectral data set from AERI provides a basis for improving clear sky radiative transfer; determining the radiative impact of clouds, including the derivation of cloud radiative properties; defining the influences of aerosols in the window regions; and retrieving boundary layer state properties, including temperature, water vapor, and other trace gases. The data stream of radiometrically and spectrally calibrated radiances is routinely provided by Pacific Northwest Laboratory (PNL) to those science teams requesting it, and further information on the instrument and data characteristics is available in the ARM Science Team proceedings for 1993 and 1994 and in several conference publications. This paper describes the AERI status, calibration, field experiment wit a new AERI-01 and schedule, window region emissions, and future AERI plans.

  5. Secondary organic aerosol from sesquiterpene and monoterpene emissions in the United States.

    Science.gov (United States)

    Sakulyanontvittaya, Tanarit; Guenther, Alex; Helmig, Detlev; Milford, Jana; Wiedinmyer, Christine

    2008-12-01

    Emissions of volatile organic compounds (VOC) from vegetation are believed to be a major source of secondary organic aerosol (SOA), which in turn comprises a large fraction of fine particulate matter in many areas. Sesquiterpenes are a class of biogenic VOC with high chemical reactivity and SOA yields. Sesquiterpenes have only recently been quantified in emissions from a wide variety of plants. In this study, a new sesquiterpene emission inventory is used to provide input to the Models-3 Community Multiscale Air Quality (CMAQ) model. CMAQ is used to estimate the contribution of sesquiterpenes and monoterpenes to SOA concentrations over the contiguous United States. The gas-particle partitioning module of CMAQ was modified to include condensable products of sesquiterpene oxidation and to update values of the enthalpy of vaporization. The resulting model predicts July monthly average surface concentrations of total SOA in the eastern U.S. ranging from about 0.2-0.8 microg m(-3). This is roughly double the amount of SOA produced in this region when sesquiterpenes are not included. Even with sesquiterpenes included, however, the model significantly underpredicts surface concentrations of particle-phase organic matter compared to observed values. Treating all SOA as capable of undergoing polymerization increases predicted monthly average surface concentrations in July to 0.4-1.2 microg m(-3), in closer agreement with observations. Using the original enthalpy of vaporization value in CMAQ in place of the values estimated from the recent literature results in predicted SOA concentrations of about 0.3-1.3 microg m(-3).

  6. Estimation of the aerosol optical thickness distribution in the Northeast Asian forest fire episode in May 2003: Possible missing emissions

    Science.gov (United States)

    In, Hee-Jin; Kim, Yong Pyo

    2010-11-01

    During the study of the enhancement of aerosol optical thickness (AOT) which was derived by Community Multi-scale Air Quality (CMAQ) model for an active forest fire episode in Northeast Asia for May 2003 (In et al., 2009), it was found that CMAQ underestimated and overestimated AOT sporadically compared to the multiple satellite observations. Based on the AERONET surface AOT observation result, the WMO Global Telecommunications System (GTS) SYNOP system smoke/fire reports, and surface aerosol concentration data in Korea, it was found that these errors were resulted from missing of biomass burning emissions and coarse aerosols originating from soil. An inconsistency between surface observed and CMAQ estimate AOT and MODIS hot spot detects was found, which suggests that accuracy of MODIS fire products needs to be assessed in East Russian, China, and Korea in order to utilize them for national scale fire management in the region. The implement of origin and transport process of wind blown dust in current CMAQ is necessary to extend CMAQ capability in Northeast Asia.

  7. A characterization of Arctic aerosols on the basis of aerosol optical depth and black carbon measurements

    Directory of Open Access Journals (Sweden)

    R. S. Stone

    2014-06-01

    Full Text Available Abstract Aerosols, transported from distant source regions, influence the Arctic surface radiation budget. When deposited on snow and ice, carbonaceous particles can reduce the surface albedo, which accelerates melting, leading to a temperature-albedo feedback that amplifies Arctic warming. Black carbon (BC, in particular, has been implicated as a major warming agent at high latitudes. BC and co-emitted aerosols in the atmosphere, however, attenuate sunlight and radiatively cool the surface. Warming by soot deposition and cooling by atmospheric aerosols are referred to as “darkening” and “dimming” effects, respectively. In this study, climatologies of spectral aerosol optical depth AOD (2001–2011 and Equivalent BC (EBC (1989–2011 from three Arctic observatories and from a number of aircraft campaigns are used to characterize Arctic aerosols. Since the 1980s, concentrations of BC in the Arctic have decreased by more than 50% at ground stations where in situ observations are made. AOD has increased slightly during the past decade, with variations attributed to changing emission inventories and source strengths of natural aerosols, including biomass smoke and volcanic aerosol, further influenced by deposition rates and airflow patterns.

  8. Climate forcing by anthropogenic aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Charlson, R J; Schwartz, S E; Hales, J M; Cess, R D; Coakley, Jr, J A; Hansen, J E; Hofmann, D J [University of Washington, Seattle, WA (USA). Inst. for Environmental Studies, Dept. of Atmospheric Sciences

    1992-01-24

    Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of short wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square metre, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes. 73 refs., 4 figs., 2 tabs.

  9. Climate forcing by anthropogenic aerosols.

    Science.gov (United States)

    Charlson, R J; Schwartz, S E; Hales, J M; Cess, R D; Coakley, J A; Hansen, J E; Hofmann, D J

    1992-01-24

    Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of shortwavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

  10. The Spatial and Temporal Distributions of Absorbing Aerosols over East Asia

    Directory of Open Access Journals (Sweden)

    Litai Kang

    2017-10-01

    Full Text Available Absorbing aerosols can strongly absorb solar radiation and have a profound impact on the global and regional climate. Black carbon (BC, organic carbon (OC and dust are three major types of absorbing aerosols. In order to deepen the overall understanding of absorbing aerosols over East Asia and provide a basis for further investigation of its role in enhanced warming in drylands, the spatial-temporal distribution of absorbing aerosols over East Asia for the period of 2005–2016 was investigated based on the Ozone Monitoring Instrument (OMI satellite retrievals. Overall, high values of Aerosol Absorption Optical Depth (AAOD mainly distribute near dust sources as well as BC and OC sources. AAOD reaches its maximum during spring over East Asia as a result of dust activity and biomass burning. Single-scattering albedo (SSA is comparatively high (>0.96 in the most part of East Asia in the summer, indicating the dominance of aerosol scattering. Hyper-arid regions have the highest Aerosol Optical Depth (AOD and AAOD among the five climatic regions, with springtime values up to 0.72 and 0.04, respectively. Humid and sub-humid regions have relatively high AOD and AAOD during the spring and winter and the highest SSA during the summer. AAOD in some areas shows significant upward trends, which is likely due to the increase of BC and OC emission. SSA shows overall downward trends, indicating the enhancement of the aerosol absorption. Analysis of emission inventory and dust index data shows that BC and OC emissions mainly come from the humid regions, while dust sources mainly distribute in drylands.

  11. Black carbon reduction will weaken the aerosol net cooling effect

    Science.gov (United States)

    Wang, Z. L.; Zhang, H.; Zhang, X. Y.

    2014-12-01

    Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in a short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate coupled model BCC_AGCM2.0.1_CUACE/Aero, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with present-day conditions if the BC emission is reduced exclusively to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial for the mitigation of global warming. However, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 relative to present-day conditions if emissions of BC and co-emitted sulfur dioxide and organic carbon are simultaneously reduced as the most close conditions to the actual situation to the level projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

  12. Emission factor ratios, SOA mass yields, and the impact of vehicular emissions on SOA formation

    Science.gov (United States)

    Ensberg, J. J.; Hayes, P. L.; Jimenez, J. L.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Holloway, J. S.; Gordon, T. D.; Jathar, S.; Robinson, A. L.; Seinfeld, J. H.

    2014-03-01

    The underprediction of ambient secondary organic aerosol (SOA) levels by current atmospheric models in urban areas is well established, yet the cause of this underprediction remains elusive. Likewise, the relative contribution of emissions from gasoline- and diesel-fueled vehicles to the formation of SOA is generally unresolved. We investigate the source of these two discrepancies using data from the 2010 CalNex experiment carried out in the Los Angeles Basin (Ryerson et al., 2013). Specifically, we use gas-phase organic mass (GPOM) and CO emission factors in conjunction with measured enhancements in oxygenated organic aerosol (OOA) relative to CO to quantify the significant lack of closure between expected and observed organic aerosol concentrations attributable to fossil-fuel emissions. Two possible conclusions emerge from the analysis to yield consistency with the ambient data: (1) vehicular emissions are not a dominant source of anthropogenic fossil SOA in the Los Angeles Basin, or (2) the ambient SOA mass yields used to determine the SOA formation potential of vehicular emissions are substantially higher than those derived from laboratory chamber studies.

  13. Qualitative Analysis of E-Liquid Emissions as a Function of Flavor Additives Using Two Aerosol Capture Methods.

    Science.gov (United States)

    Eddingsaas, Nathan; Pagano, Todd; Cummings, Cody; Rahman, Irfan; Robinson, Risa; Hensel, Edward

    2018-02-13

    This work investigates emissions sampling methods employed for qualitative identification of compounds in e-liquids and their resultant aerosols to assess what capture methods may be sufficient to identify harmful and potentially harmful constituents present. Three popular e-liquid flavors (cinnamon, mango, vanilla) were analyzed using qualitative gas chromatography-mass spectrometry (GC-MS) in the un-puffed state. Each liquid was also machine-puffed under realistic-use flow rate conditions and emissions were captured using two techniques: filter pads and methanol impingers. GC-MS analysis was conducted on the emissions captured using both techniques from all three e-liquids. The e-liquid GC-MS analysis resulted in positive identification of 13 compounds from the cinnamon flavor e-liquid, 31 from mango, and 19 from vanilla, including a number of compounds observed in all e-liquid experiments. Nineteen compounds were observed in emissions which were not present in the un-puffed e-liquid. Qualitative GC-MS analysis of the emissions samples identify compounds observed in all three samples: e-liquid, impinge, and filter pads, and each subset thereof. A limited number of compounds were observed in emissions captured with impingers, but were not observed in emissions captured using filter pads; a larger number of compounds were observed on emissions collected from the filter pads, but not those captured with impingers. It is demonstrated that sampling methods have different sampling efficiencies and some compounds might be missed using only one method. It is recommended to investigate filter pads, impingers, thermal desorption tubes, and solvent extraction resins to establish robust sampling methods for emissions testing of e-cigarette emissions.

  14. Dynamic-chemistry-aerosol modelling interaction: the ESCOMPTE 2001 experiment; Modelisation de l'interaction dynamique- chimie - aerosol: campagne ESCOMPTE 2001

    Energy Technology Data Exchange (ETDEWEB)

    Cousin, F

    2004-09-01

    After most pollution studies independently devoted to gases and aerosols, there now appears an urgent need to consider their interactions. In this view, an aerosol module has been implemented in the Meso-NH-C model to simulate two IOPs documented during the ESCOMPTE campaign which took place in the Marseille/Fos-Berre region in June-July 2001. First, modelled dynamic parameters (winds, temperatures, boundary layer thickness) and gaseous chemistry have been validated with measurements issued from the exhaustive ESCOMPTE database. Sensitivity analysis have also been performed using different gaseous emission inventories at various resolution. These simulations have illustrated the deep impact of both synoptic and local dynamics on observed ozone concentrations on June 24 (IOP2b) in the ESCOMPTE domain. Afterwards, the ORISAM aerosol module has been introduced into the Meso-NH-C model. Dynamics, gaseous chemistry and aerosol processes have thus been coupled on-line. The particulate pollution episode on June 24 (IOP2b) has been characterised through a satisfactory comparison, specially from sub-micron particles, between modelling and measurements at different representative stations in the domain. This study, with validation of the particulate emission inventory has also highlighted the need for future improvements, such as further characterisation of organic and inorganic aerosol species and consideration of coarse particles. Aerosol impact on gaseous chemistry has been preliminary approached in view of future development and modification to be given to the Meso-NH-C model. (author)

  15. On the Specification of Smoke Injection Heights for Aerosol Forecasting

    Science.gov (United States)

    da Silva, A.; Schaefer, C.; Randles, C. A.

    2014-12-01

    The proper forecasting of biomass burning (BB) aerosols in global or regional transport models requires not only the specification of emission rates with sufficient temporal resolution but also the injection layers of such emissions. While current near realtime biomass burning inventories such as GFAS, QFED, FINN, GBBEP and FLAMBE provide such emission rates, it is left for each modeling system to come up with its own scheme for distributing these emissions in the vertical. A number of operational aerosol forecasting models deposits BB emissions in the near surface model layers, relying on the model's parameterization of turbulent and convective transport to determine the vertical mass distribution of BB aerosols. Despite their simplicity such schemes have been relatively successful reproducing the vertical structure of BB aerosols, except for those large fires that produce enough buoyancy to puncture the PBL and deposit the smoke at higher layers. Plume Rise models such as the so-called 'Freitas model', parameterize this sub-grid buoyancy effect, but require the specification of fire size and heat fluxes, none of which is readily available in near real-time from current remotely-sensed products. In this talk we will introduce a bayesian algorithm for estimating file size and heat fluxes from MODIS brightness temperatures. For small to moderate fires the Freitas model driven by these heat flux estimates produces plume tops that are highly correlated with the GEOS-5 model estimate of PBL height. Comparison to MINX plume height estimates from MISR indicates moderate skill of this scheme predicting the injection height of large fires. As an alternative, we make use of OMPS UV aerosol index data in combination with estimates of Overshooting Convective Tops (from MODIS and Geo-stationary satellites) to detect PyCu events and specify the BB emission vertical mass distribution in such cases. We will present a discussion of case studies during the SEAC4RS field campaign in

  16. Environment, Health and Climate: Impact of African aerosols

    Science.gov (United States)

    Liousse, C.; Doumbia, T.; Assamoi, E.; Galy-Lacaux, C.; Baeza, A.; Penner, J. E.; Val, S.; Cachier, H.; Xu, L.; Criqui, P.

    2012-12-01

    Fossil fuel and biofuel emissions of particles in Africa are expected to significantly increase in the near future, particularly due to rapid growth of African cities. In addition to biomass burning emissions prevailing in these areas, air quality degradation is then expected with important consequences on population health and climatic/radiative impact. In our group, we are constructing a new integrated methodology to study the relations between emissions, air quality and their impacts. This approach includes: (1) African combustion emission characterizations; (2) joint experimental determination of aerosol chemistry from ultrafine to coarse fractions and health issues (toxicology and epidemiology). (3) integrated environmental, health and radiative modeling. In this work, we show some results illustrating our first estimates of African anthropogenic emission impacts: - a new African anthropogenic emission inventory adapted to regional specificities on traffic, biofuel and industrial emissions has been constructed for the years 2005 and 2030. Biomass burning inventories were also improved in the frame of AMMA (African Monsoon) program. - carbonaceous aerosol radiative impact in Africa has been modeled with TM5 model and Penner et al. (2011) radiative code for these inventories for 2005 and 2030 and for two scenarios of emissions : a reference scenario, with no further emission controls beyond those achieved in 2003 and a ccc* scenario including planned policies in Kyoto protocol and regulations as applied to African emission specificities. In this study we will show that enhanced heating is expected with the ccc* scenarios emissions in which the OC fraction is relatively lower than in the reference scenario. - results of short term POLCA intensive campaigns in Bamako and Dakar in terms of aerosol chemical characterization linked to specific emissions sources and their inflammatory impacts on the respiratory tract through in vitro studies. In this study, organic

  17. Anthropogenic influence on the distribution of tropospheric sulphate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Langner, J; Rodhe, H; Crutzen, P J; Zimmermann, P [Swedish Meteorological and Hydrological Institute, Norrkoeping (Sweden)

    1992-10-22

    Human activities have increased global emissions of sulphur gases by about a factor of three during the past century, leading to increased sulphate aerosol concentrations, mainly in the Northern Hemisphere. Sulphate aerosols can affect the climate directly, by increasing the backscattering of solar radiation in cloud-free air, and indirectly, by providing additional cloud condensation nuclei. Here a global transport-chemistry model is used to estimate the changes in the distribution of tropospheric sulphate aerosol and deposition of non-seasalt sulphur that have occurred since pre-industrial times. The increase in sulphate aerosol concentration is small over the Southern Hemisphere oceans, but reaches a factor of 100 over northern Europe in winter. Calculations indicate, however, that at most 6% of the anthropogenic sulphur emissions is available for the formation of new aerosol particles. This is because about one-half of the sulphur dioxide is deposited on the Earth's surface, and most of the remainder is oxidized in cloud droplets so that the sulphate becomes associated with pre-existing particles. Even so, the rate of formation of new sulphate particles may have doubled since pre-industrial times. 18 refs., 3 figs.

  18. Background aerosol over the Himalayas and Tibetan Plateau: observed characteristics of aerosol mass loading

    Science.gov (United States)

    Liu, Bin; Cong, Zhiyuan; Wang, Yuesi; Xin, Jinyuan; Wan, Xin; Pan, Yuepeng; Liu, Zirui; Wang, Yonghong; Zhang, Guoshuai; Wang, Zhongyan; Wang, Yongjie; Kang, Shichang

    2017-01-01

    To investigate the atmospheric aerosols of the Himalayas and Tibetan Plateau (HTP), an observation network was established within the region's various ecosystems, including at the Ngari, Qomolangma (QOMS), Nam Co, and Southeastern Tibetan (SET) stations. In this paper we illustrate aerosol mass loadings by integrating in situ measurements with satellite and ground-based remote sensing datasets for the 2011-2013 period, on both local and large scales. Mass concentrations of these surface atmospheric aerosols were relatively low and varied with land cover, showing a general tendency of Ngari and QOMS (barren sites) > Nam Co (grassland site) > SET (forest site). Daily averages of online PM2.5 (particulates with aerodynamic diameters below 2.5 µm) at these sites were sequentially 18.2 ± 8.9, 14.5 ± 7.4, 11.9 ± 4.9 and 11.7 ± 4.7 µg m-3. Correspondingly, the ratios of PM2.5 to total suspended particles (TSP) were 27.4 ± 6.65, 22.3 ± 10.9, 37.3 ± 11.1 and 54.4 ± 6.72 %. Bimodal mass distributions of size-segregated particles were found at all sites, with a relatively small peak in accumulation mode and a more notable peak in coarse mode. Diurnal variations in fine-aerosol masses generally displayed a bi-peak pattern at the QOMS, Nam Co and SET stations and a single-peak pattern at the Ngari station, controlled by the effects of local geomorphology, mountain-valley breeze circulation and aerosol emissions. Dust aerosol content in PM2.1 samples gave fractions of 26 % at the Ngari station and 29 % at the QOMS station, or ˜ 2-3 times that of reported results at human-influenced sites. Furthermore, observed evidence confirmed the existence of the aerodynamic conditions necessary for the uplift of fine particles from a barren land surface. Combining surface aerosol data and atmospheric-column aerosol optical properties, the TSP mass and aerosol optical depth (AOD) of the Multi-angle Imaging Spectroradiometer (MISR) generally decreased as land cover changed from

  19. Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

    Science.gov (United States)

    Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

    2015-12-01

    The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

  20. Program GICC, final report (March 2005), inventory of carbonaceous aerosol particles from 1860 to 2100 or which carbonaceous aerosol for a significant climatic regional/global impact?; Programme GICC, RAPPORT DEFINITIF (Mars 2005), inventaire d'emissions d'aerosol carbone de 1860 a 2100 ou quelles emissions d'aerosol carbone pour un impact climatique regional/global significatif?

    Energy Technology Data Exchange (ETDEWEB)

    Cachier, H.; Guinot, B. [Laboratoire des Sciences du Climat et de l' Environnment, UMR CEA/CNRS 1572 - CEA Saclay, 91 - Gif sur Yvette (France); Criqui, P.; Mima, S. [IEPE, 38 - Grenoble (France); Brignon, J.M. [INERIS, 60 - Verneuil-en-Halatte (France); Penner, J. [Michigan Univ., Ann Arbor, MI (United States); Carmichael, G. [Iowa Univ., Iowa City, IA (United States); Gadi, R. [National Physical Lab., New Delhi (India); Denier Van der Gon, H. [TNO Hollande (Netherlands); Gregoire, J.M. [JRC, Ispra (Italy); Liousse, C.; Michel, C.; Guillaume, B.; Junker, C

    2007-07-01

    The aim of our program is to determine past, present and future emission inventories of carbonaceous particles from 1860 to 2100 for fossil fuel and biofuel sources. Emission inventories for savannah and forest fires have been developed by using burnt area products given by satellite for Asia and Africa. The strong collaboration with the different groups attending this GICC program has allowed to develop the following results. 1- With the improvement of algorithms and new choices for emission factors, emission inventories for black carbon (BC), primary organic carbon (OCp) and total organic carbon (OCtot) have been constructed for the period 1950 to 1997 for fossil fuel and biofuel sources. With these new development, biofuel sources have been seen to be significant, especially in the developing countries. 2- Past inventories have been developed for fossil fuel and biofuel sources from 1860 to 1997 by taking into account the evolution of fuel consumption, fuel use and emission factors. 3- Savannah and forest fire inventories have been constructed based on burnt area products, for Africa (1981-1991, 2000) and Asia (2000-2001). These results show the importance of using real time data instead of statistics. 4-Future emission inventory of black carbon by fossil fuel sources has been constructed for 2100 following the IPCC scenario A2 (catastrophic case) and B1 (perfect world). 5-Characterization of biofuel emissions has been realized by organizing an experiment in a combustion chamber where indian and chinese biofuels (fuelwood, agricultural wastes, dung-cake etc..). were burnt, reproducing the burning methods used in these countries. 6-Finally, the differences between the existing inventories of carbonaceous aerosols has been explained. (A.L.B.)

  1. Application of Recent Advances in Forward Modeling of Emissions from Boreal and Temperate Wildfires to Real-time Forecasting of Aerosol and Trace Gas Concentrations

    Science.gov (United States)

    Hyer, E. J.; Reid, J. S.; Kasischke, E. S.; Allen, D. J.

    2005-12-01

    The magnitude of trace gas and aerosol emissions from wildfires is a scientific problem with important implications for atmospheric composition, and is also integral to understanding carbon cycling in terrestrial ecosystems. Recent ecological research on modeling wildfire emissions has integrated theoretical advances derived from ecological fieldwork with improved spatial and temporal databases to produce "post facto" estimates of emissions with high spatial and temporal resolution. These advances have been shown to improve agreement with atmospheric observations at coarse scales, but can in principle be applied to applications, such as forecasting, at finer scales. However, several of the approaches employed in these forward models are incompatible with the requirements of real-time forecasting, requiring modification of data inputs and calculation methods. Because of the differences in data inputs used for real-time and "post-facto" emissions modeling, the key uncertainties in the forward problem are not necessarily the same for these two applications. However, adaptation of these advances in forward modeling to forecasting applications has the potential to improve air quality forecasts, and also to provide a large body of experimental data which can be used to constrain crucial uncertainties in current conceptual models of wildfire emissions. This talk describes a forward modeling method developed at the University of Maryland and its application to the Fire Locating and Modeling of Burning Emissions (FLAMBE) system at the Naval Research Laboratory. Methods for applying the outputs of the NRL aerosol forecasting system to the inverse problem of constraining emissions will also be discussed. The system described can use the feedback supplied by atmospheric observations to improve the emissions source description in the forecasting model, and can also be used for hypothesis testing regarding fire behavior and data inputs.

  2. Modelisation of soluble aerosols behaviour in the atmosphere of a PWR nuclear reactor in case of accident

    International Nuclear Information System (INIS)

    Abbas, A.F.

    1984-07-01

    After a short description of soluble aerosols accidental production in a PWR, a calculation model is given for physical properties of a gaz and steam mixture in a given atmosphere. Then the equilibrium of a saline drop with steam is studied. From the MASON equation, a calculation model is given for kinetic of volume variation of a saline drop and also a sensitivity study showing the little influence of the boundary layer on the drop surface, of the drop settling and of the thermodynamic conditions of the containment. As a numerical application, this condensation/evaporation model, and a simplified one with faster numerical resolution, is introduced in the AEROSOLS codes of the CEA-DEMT. The AEROSOLS/A2 suppose a log-normal distribution of the suspended particles in the containment. This application shows the very large sensitivity of the condensation depending on the moisture ratio inside the reactor building, and its primary importance on the behaviour of the aerosols. It is also shown that the simplified model gives a very little difference compared with the detailed model, and that the computation time is much more lower [fr

  3. The role of aerosols in cloud drop parameterizations and its applications in global climate models

    Energy Technology Data Exchange (ETDEWEB)

    Chuang, C.C.; Penner, J.E. [Lawrence Livermore National Lab., CA (United States)

    1996-04-01

    The characteristics of the cloud drop size distribution near cloud base are initially determined by aerosols that serve as cloud condensation nuclei and the updraft velocity. We have developed parameterizations relating cloud drop number concentration to aerosol number and sulfate mass concentrations and used them in a coupled global aerosol/general circulation model (GCM) to estimate the indirect aerosol forcing. The global aerosol model made use of our detailed emissions inventories for the amount of particulate matter from biomass burning sources and from fossil fuel sources as well as emissions inventories of the gas-phase anthropogenic SO{sub 2}. This work is aimed at validating the coupled model with the Atmospheric Radiation Measurement (ARM) Program measurements and assessing the possible magnitude of the aerosol-induced cloud effects on climate.

  4. PIXE analysis of atmospheric aerosol and hydrometeor particles

    International Nuclear Information System (INIS)

    Groeneveld, K.O.; Hofmann, D.; Georgii, H.W.

    1993-01-01

    Atmospheric aerosol and hydrometeor particles act decisively on our weather, climate and thereby on all living conditions on Earth. Particle induced X-ray emission (PIXE) analysis has been demonstrated to be an extremely valuable tool for quantitative and qualitative elemental analysis of aerosol particles and hydrometeors. Reliability and detection limits of PIXE are determined, including comparison with other techniques. Aerosol particles are collected on a global scale in ground stations, or by ships and by planes. Correlation between wind direction and elemental composition of atmospheric aerosols, elemental particle size distributions of the tropospheric aerosol, aerosol elemental composition in particle size fractions in the case of long range transport, transport pathways of pollution aerosol, and trace element content precipitation are discussed. Hydrometeors were studied in the form of rain, snow, fog, dew and frost. The time dependence of the melting process of snow was studied in detail, in particular the washout phenomena of impurity ions. (orig.)

  5. Changes in microbial diversity in industrial wastewater evaporation ponds following artificial salination.

    Science.gov (United States)

    Ben-Dov, Eitan; Shapiro, Orr H; Gruber, Ronen; Brenner, Asher; Kushmaro, Ariel

    2008-11-01

    The salinity of industrial wastewater evaporation ponds was artificially increased from 3-7% to 12-16% (w/v), in an attempt to reduce the activity of sulfate-reducing bacteria (SRB) and subsequent emission of H2S. To investigate the changes in bacterial diversity in general, and SRB in particular, following this salination, two sets of universal primers targeting the 16S rRNA gene and the functional apsA [adenosine-5'-phosphosulfate (APS) reductase alpha-subunit] gene of SRB were used. Phylogenetic analysis indicated that Proteobacteria was the most dominant phylum both before and after salination (with 52% and 68%, respectively), whereas Firmicutes was the second most dominant phylum before (39%) and after (19%) salination. Sequences belonging to Bacteroidetes, Spirochaetes and Actinobacteria were also found. Several groups of SRB from Proteobacteria and Firmicutes were also found to inhabit this saline environment. Comparison of bacterial diversity before and after salination of the ponds revealed both a shift in community composition and an increase in microbial diversity following salination. The share of SRB in the 16S rRNA gene was reduced following salination, consistent with the reduction of H2S emissions. However, the community composition, as shown by apsA gene analysis, was not markedly affected.

  6. Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

    Directory of Open Access Journals (Sweden)

    W. T. Morgan

    2010-09-01

    substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

  7. Aerosol Transport Over Equatorial Africa

    Science.gov (United States)

    Gatebe, C. K.; Tyson, P. D.; Annegarn, H. J.; Kinyua, A. M.; Piketh, S.; King, M.; Helas, G.

    1999-01-01

    Long-range and inter-hemispheric transport of atmospheric aerosols over equatorial Africa has received little attention so far. Most aerosol studies in the region have focussed on emissions from rain forest and savanna (both natural and biomass burning) and were carried out in the framework of programs such as DECAFE (Dynamique et Chimie Atmospherique en Foret Equatoriale) and FOS (Fires of Savanna). Considering the importance of this topic, aerosols samples were measured in different seasons at 4420 meters on Mt Kenya and on the equator. The study is based on continuous aerosol sampling on a two stage (fine and coarse) streaker sampler and elemental analysis by Particle Induced X-ray Emission. Continuous samples were collected for two seasons coinciding with late austral winter and early austral spring of 1997 and austral summer of 1998. Source area identification is by trajectory analysis and sources types by statistical techniques. Major meridional transports of material are observed with fine-fraction silicon (31 to 68 %) in aeolian dust and anthropogenic sulfur (9 to 18 %) being the major constituents of the total aerosol loading for the two seasons. Marine aerosol chlorine (4 to 6 %), potassium (3 to 5 %) and iron (1 to 2 %) make up the important components of the total material transport over Kenya. Minimum sulfur fluxes are associated with recirculation of sulfur-free air over equatorial Africa, while maximum sulfur concentrations are observed following passage over the industrial heartland of South Africa or transport over the Zambian/Congo Copperbelt. Chlorine is advected from the ocean and is accompanied by aeolian dust recirculating back to land from mid-oceanic regions. Biomass burning products are transported from the horn of Africa. Mineral dust from the Sahara is transported towards the Far East and then transported back within equatorial easterlies to Mt Kenya. This was observed during austral summer and coincided with the dying phase of 1997/98 El

  8. Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

    Directory of Open Access Journals (Sweden)

    C. J. Hennigan

    2011-08-01

    Full Text Available Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III. We investigated emissions from 12 different fuels commonly burned in North American wildfires. The experiments feature atmospheric and plume aerosol and oxidant concentrations; aging times ranged from 3 to 4.5 h. OA production, expressed as a mass enhancement ratio (ratio of OA to primary OA (POA mass, was highly variable. OA mass enhancement ratios ranged from 2.9 in experiments where secondary OA (SOA production nearly tripled the POA concentration to 0.7 in experiments where photo-oxidation resulted in a 30 % loss of the OA mass. The campaign-average OA mass enhancement ratio was 1.7 ± 0.7 (mean ± 1σ; therefore, on average, there was substantial SOA production. In every experiment, the OA was chemically transformed. Even in experiments with net loss of OA mass, the OA became increasingly oxygenated and less volatile with aging, indicating that photo-oxidation transformed the POA emissions. Levoglucosan concentrations were also substantially reduced with photo-oxidation. The transformations of POA were extensive; using levoglucosan as a tracer for POA, unreacted POA only contributed 17 % of the campaign-average OA mass after 3.5 h of exposure to typical atmospheric hydroxyl radical (OH levels. Heterogeneous reactions with OH could account for less than half of this transformation, implying that the coupled gas-particle partitioning and reaction of semi-volatile vapors is an important and potentially dominant mechanism for POA processing. Overall, the results illustrate that biomass burning emissions are subject to extensive chemical processing in the atmosphere, and the timescale for these transformations is rapid.

  9. OH-initiated Aging of Biomass Burning Aerosol during FIREX

    Science.gov (United States)

    Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

    2017-12-01

    Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

  10. Modelling African aerosol using updated fossil fuel and biofuel emission inventories for 2005 and 2030

    Science.gov (United States)

    Liousse, C.; Penner, J. E.; Assamoi, E.; Xu, L.; Criqui, P.; Mima, S.; Guillaume, B.; Rosset, R.

    2010-12-01

    A regional fossil fuel and biofuel emission inventory for particulates has been developed for Africa at a resolution of 0.25° x 0.25° for the year 2005. The original database of Junker and Liousse (2008) was used after modification for updated regional fuel consumption and emission factors. Consumption data were corrected after direct inquiries conducted in Africa, including a new emitter category (i.e. two-wheel vehicles including “zemidjans”) and a new activity sector (i.e. power plants) since both were not considered in the previous emission inventory. Emission factors were measured during the 2005 AMMA campaign (Assamoi and Liousse, 2010) and combustion chamber experiments. Two prospective inventories for 2030 are derived based on this new regional inventory and two energy consumption forecasts by the Prospective Outlook on Long-term Energy Systems (POLES) model (Criqui, 2001). The first is a reference scenario, where no emission controls beyond those achieved in 2003 are taken into account, and the second is for a "clean" scenario where possible and planned policies for emission control are assumed to be effective. BC and OCp emission budgets for these new inventories will be discussed and compared to the previous global dataset. These new inventories along with the most recent open biomass burning inventory (Liousse et al., 2010) have been tested in the ORISAM-TM5 global chemistry-climate model with a focus over Africa at a 1° x 1° resolution. Global simulations for BC and primary OC for the years 2005 and 2030 are carried out and the modelled particulate concentrations for 2005 are compared to available measurements in Africa. Finally, BC and OC radiative properties (aerosol optical depths and single scattering albedo) are calculated and the direct radiative forcing is estimated using an off line model (Wang and Penner, 2009). Results of sensitivity tests driven with different emission scenarios will be presented.

  11. Nuclear analytical techniques applied to the large scale measurements of atmospheric aerosols in the amazon region

    International Nuclear Information System (INIS)

    Gerab, Fabio

    1996-03-01

    This work presents the characterization of the atmosphere aerosol collected in different places of the Amazon Basin. We studied both the biogenic emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burning during the dry season. The samples were collected during a three year period at two different locations in the Amazon, namely the Alta Floresta (MT) and Serra do Navio (AP) regions, using stacked unit filters. These regions represent two different atmospheric compositions: the aerosol is dominated by the forest natural biogenic emission at Serra do Navio, while at Alta Floresta it presents an important contribution from the man-made burning during the dry season. At Alta Floresta we took samples in gold in order to characterize mercury emission to the atmosphere related to the gold prospection activity in Amazon. Airplanes were used for aerosol sampling during the 1992 and 1993 dry seasons to characterize the atmospheric aerosol contents from man-made burning in large Amazonian areas. The samples were analyzed using several nuclear analytic techniques: Particle Induced X-ray Emission for the quantitative analysis of trace elements with atomic number above 11; Particle Induced Gamma-ray Emission for the quantitative analysis of Na; and Proton Microprobe was used for the characterization of individual particles of the aerosol. Reflectancy technique was used in the black carbon quantification, gravimetric analysis to determine the total atmospheric aerosol concentration and Cold Vapor Atomic Absorption Spectroscopy for quantitative analysis of mercury in the particulate from the Alta Floresta gold shops. Ionic chromatography was used to quantify ionic contents of aerosols from the fine mode particulate samples from Serra do Navio. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. (author)

  12. A Systematic Exploration of the Local and Remote Climate Effects of Anthropogenic Aerosol Emissions from Key Regions

    Science.gov (United States)

    Voulgarakis, A.; Kasoar, M.; Shawki, D.; Lamarque, J. F.; Shindell, D. T.; Faluvegi, G.; Bellouin, N.; Collins, W.; Tsigaridis, K.

    2016-12-01

    The radiative forcing of short-lived pollutants such as aerosols and tropospheric ozone is highly inhomogeneous and can therefore affect regional temperature, circulation and precipitation in a much more complicated way than the forcing of well-mixed greenhouse gases. Such effects have only recently started to be examined thoroughly and systematically from a global point of view, to understand regional interactions. Here, after outlining some key past work in this area, results from recent simulations with the UK Met Office's HadGEM3 global composition-climate model will be presented in which anthropogenic emissions of sulfur dioxide (SO2) and black carbon in key regions (East Asia, South Asia, Europe, the US, and the northern mid-latitudes as a whole) have been removed. The linkages between emissions, concentrations, radiative forcing, temperature and precipitation responses will be discussed. A particular emphasis will be placed on non-local effects, i.e. how emissions over a certain region can affect other areas remotely. Finally, we will contrast our results with those from similar experiments pursued using the NASA GISS-E2 and the NCAR CESM1 models for US and East Asian SO2 emissions, and will discuss the large differences in the models' behaviour.

  13. Extremely large anthropogenic-aerosol contribution to total aerosol load over the Bay of Bengal during winter season

    Directory of Open Access Journals (Sweden)

    D. G. Kaskaoutis

    2011-07-01

    Full Text Available Ship-borne observations of spectral aerosol optical depth (AOD have been carried out over the entire Bay of Bengal (BoB as part of the W-ICARB cruise campaign during the period 27 December 2008–30 January 2009. The results reveal a pronounced temporal and spatial variability in the optical characteristics of aerosols mainly due to anthropogenic emissions and their dispersion controlled by local meteorology. The highest aerosol amount, with mean AOD500>0.4, being even above 1.0 on specific days, is found close to the coastal regions in the western and northern parts of BoB. In these regions the Ångström exponent is also found to be high (~1.2–1.25 indicating transport of strong anthropogenic emissions from continental regions, while very high AOD500 (0.39±0.07 and α380–870 values (1.27±0.09 are found over the eastern BoB. Except from the large α380–870 values, an indication of strong fine-mode dominance is also observed from the AOD curvature, which is negative in the vast majority of the cases, suggesting dominance of an anthropogenic-pollution aerosol type. On the other hand, clean maritime conditions are rather rare over the region, while the aerosol types are further examined through a classification scheme based on the relationship between α and dα. It was found that even for the same α values the fine-mode dominance is larger for higher AODs showing the strong continental influence over the marine environment of BoB. Furthermore, there is also an evidence of aerosol-size growth under more turbid conditions indicative of coagulation and/or humidification over specific BoB regions. The results obtained using OPAC model show significant fraction of soot aerosols (~6 %–8 % over the eastern and northwestern BoB, while coarse-mode sea salt particles are found to dominate in the southern parts of BoB.

  14. Lung delivery of aerosolized dextran.

    Science.gov (United States)

    Finlay, W H; Lange, C F; King, M; Speert, D P

    2000-01-01

    The ability of nebulizers to deliver dextran (nominal molecular mass, 4,000 g/mol) to the lung as an inhaled aerosol is evaluated by in vitro experimental methods and mathematical models. Dextran in isotonic saline was aerosolized by four nebulizer types (Pari LC STAR, Hudson T-Updraft II, Acorn II, and Sonix 2000) at dextran concentrations phase Doppler anemometry, filter collection, osmometry, and gravimetry. Mathematical models were used to estimate amounts of the characterized aerosols depositing in the different regions of lung models, and mathematical models of mucous thickness were then developed to estimate initial concentrations of the depositing dextran in the mucus of each conducting airway generation. Models of three subjects (4 yr old, 8 yr old, and adult) were used. The high viscosity of the dextran solutions tested (up to seven times that of water) negatively impacts nebulization, and results in poor performance with most delivery systems tested. Our results suggest that airway mucosal dextran concentrations associated with efficacy in previous animal and in vitro models are achievable with reasonable delivery times (

  15. Black carbon aerosols and the third polar ice cap

    Energy Technology Data Exchange (ETDEWEB)

    Menon, Surabi; Koch, Dorothy; Beig, Gufran; Sahu, Saroj; Fasullo, John; Orlikowski, Daniel

    2010-04-15

    Recent thinning of glaciers over the Himalayas (sometimes referred to as the third polar region) have raised concern on future water supplies since these glaciers supply water to large river systems that support millions of people inhabiting the surrounding areas. Black carbon (BC) aerosols, released from incomplete combustion, have been increasingly implicated as causing large changes in the hydrology and radiative forcing over Asia and its deposition on snow is thought to increase snow melt. In India BC emissions from biofuel combustion is highly prevalent and compared to other regions, BC aerosol amounts are high. Here, we quantify the impact of BC aerosols on snow cover and precipitation from 1990 to 2010 over the Indian subcontinental region using two different BC emission inventories. New estimates indicate that Indian BC emissions from coal and biofuel are large and transport is expected to expand rapidly in coming years. We show that over the Himalayas, from 1990 to 2000, simulated snow/ice cover decreases by {approx}0.9% due to aerosols. The contribution of the enhanced Indian BC to this decline is {approx}36%, similar to that simulated for 2000 to 2010. Spatial patterns of modeled changes in snow cover and precipitation are similar to observations (from 1990 to 2000), and are mainly obtained with the newer BC estimates.

  16. Physical and chemical characterization of residential oil boiler emissions.

    Science.gov (United States)

    Hays, Michael D; Beck, Lee; Barfield, Pamela; Lavrich, Richard J; Dong, Yuanji; Vander Wal, Randy L

    2008-04-01

    The toxicity of emissions from the combustion of home heating oil coupled with the regional proximity and seasonal use of residential oil boilers (ROB) is an important public health concern. Yet scant physical and chemical information about the emissions from this source is available for climate and air quality modeling and for improving our understanding of aerosol-related human health effects. The gas- and particle-phase emissions from an active ROB firing distillate fuel oil (commonly known as diesel fuel) were evaluated to address this deficiency. Ion chromatography of impactor samples showed that the ultrafine ROB aerosol emissions were approximately 45% (w/w) sulfate. Gas chromatography-mass spectrometry detected various n-alkanes at trace levels, sometimes in accumulation mode particles, and out of phase with the size distributions of aerosol mass and sulfate. The carbonaceous matter in the ROB aerosol was primarily light-adsorbing elemental carbon. Gas chromatography-atomic emission spectroscopy measured a previously unrecognized organosulfur compound group in the ROB aerosol emissions. High-resolution transmission electron microscopy of ROB soot indicated the presence of a highly ordered primary particle nanostructure embedded in larger aggregates. Organic gas emissions were measured using EPA Methods TO-15 and TO-11A. The ROB emitted volatile oxygenates (8 mg/(kg of oil burned)) and olefins (5 mg/(kg of oil burned)) mostly unrelated to the base fuel composition. In the final analysis, the ROB tested was a source of numerous hazardous air pollutants as defined in the Clean Air Act Amendments. Approximations conducted using emissions data from the ROB tests show relatively low contributions to a regional-level anthropogenic emissions inventory for volitile organic compounds, PM2.5, and SO2 mass.

  17. Transport of Aerosols: Regional and Global Implications for Climate, Weather, and Air Quality

    Science.gov (United States)

    Chin, Mian; Diehl, Thomas; Yu, Hongbin; Bian, Huisheng; Remer, Lorraine; Kahn, Ralph

    2008-01-01

    Long-range transport of atmospheric aerosols can have a significant impact on global climate, regional weather, and local air quality. In this study, we use a global model GOCART together with satellite data and ground-based measurements to assess the emission and transport of pollution, dust, biomass burning, and volcanic aerosols and their implications. In particular, we will show the impact of emissions and long-range transport of aerosols from major pollution and dust source regions to (1) the surface air quality, (2) the atmospheric heating rates, and (3) surface radiation change near the source and downwind regions.

  18. Self-charging of 198Au-labeled monodisperse gold aerosols studied with a miniature electrical mobility spectrometer

    International Nuclear Information System (INIS)

    Yeh, H.C.; Newton, G.J.; Raabe, O.G.; Boor, D.R.

    1976-01-01

    Knowledge of the electrostatic character of an aerosol may be essential in assessing its potential inhalation hazard. In inhalation studies with radioactive aerosols, the aerosol charge state may change in the course of transport due to the emission of α, β or γ radiations. This paper describes an experimental study of the self-charging of 198 Au-labeled aerosols of monodisperse gold spheres by β emission. A miniature aerosol electrical mobility spectrometer, suitable for use in inhalation studies with radioactive aerosols, was developed and used in this study. This device is relatively inexpensive, easy to manufacture and its contamination by radioactive material has been minimized. Using polystyrene latex spheres, ranging in diameter from 0.176 to 1.18 μm, the spectrometer was calibrated with flow rates ranging from 400 to 4800 ml/min. Experiments with two sizes of 198 Au-labeled monodisperse gold aerosols were performed. Results indicate that the radioactivity of an aerosol can cause self-charging and affect the charge distribution. (author)

  19. Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

    Energy Technology Data Exchange (ETDEWEB)

    McMeeking, Gavin R.; Kreidenweis, Sonia M.; Baker, Stephen; Carrico, Christian M.; Chow, Judith C.; Collett, Jr., Jeffrey L.; Hao, Wei Min; Holden, Amanda S.; Kirchstetter, Thomas W.; Malm, William C.; Moosmuller, Hans; Sullivan, Amy P.; Wold, Cyle E.

    2009-05-15

    We characterized the gas- and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly-burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern US (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO{sub 2}, CO, CH{sub 4}, C{sub 2-4} hydrocarbons, NH{sub 3}, SO{sub 2}, NO, NO{sub 2}, HNO{sub 3} and particle-phase organic carbon (OC), elemental carbon (EC), SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, Cl{sup -}, Na{sup +}, K{sup +}, and NH{sub 4}{sup +} generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming- and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed EF for total fine particulate matter. Our measurements often spanned a larger range of MCE than prior studies, and thus help to improve estimates for individual fuels of the variation of emissions with combustion conditions.

  20. Soil salinity decreases global soil organic carbon stocks.

    Science.gov (United States)

    Setia, Raj; Gottschalk, Pia; Smith, Pete; Marschner, Petra; Baldock, Jeff; Setia, Deepika; Smith, Jo

    2013-11-01

    Saline soils cover 3.1% (397 million hectare) of the total land area of the world. The stock of soil organic carbon (SOC) reflects the balance between carbon (C) inputs from plants, and losses through decomposition, leaching and erosion. Soil salinity decreases plant productivity and hence C inputs to the soil, but also microbial activity and therefore SOC decomposition rates. Using a modified Rothamsted Carbon model (RothC) with a newly introduced salinity decomposition rate modifier and a plant input modifier we estimate that, historically, world soils that are currently saline have lost an average of 3.47 tSOC ha(-1) since they became saline. With the extent of saline soils predicted to increase in the future, our modelling suggests that world soils may lose 6.8 Pg SOC due to salinity by the year 2100. Our findings suggest that current models overestimate future global SOC stocks and underestimate net CO2 emissions from the soil-plant system by not taking salinity effects into account. From the perspective of enhancing soil C stocks, however, given the lower SOC decomposition rate in saline soils, salt tolerant plants could be used to sequester C in salt-affected areas. Copyright © 2012 Elsevier B.V. All rights reserved.

  1. The effect of sea ice loss on sea salt aerosol concentrations and the radiative balance in the Arctic

    Directory of Open Access Journals (Sweden)

    H. Struthers

    2011-04-01

    Full Text Available Understanding Arctic climate change requires knowledge of both the external and the local drivers of Arctic climate as well as local feedbacks within the system. An Arctic feedback mechanism relating changes in sea ice extent to an alteration of the emission of sea salt aerosol and the consequent change in radiative balance is examined. A set of idealized climate model simulations were performed to quantify the radiative effects of changes in sea salt aerosol emissions induced by prescribed changes in sea ice extent. The model was forced using sea ice concentrations consistent with present day conditions and projections of sea ice extent for 2100. Sea salt aerosol emissions increase in response to a decrease in sea ice, the model results showing an annual average increase in number emission over the polar cap (70–90° N of 86 × 106 m−2 s−1 (mass emission increase of 23 μg m−2 s−1. This in turn leads to an increase in the natural aerosol optical depth of approximately 23%. In response to changes in aerosol optical depth, the natural component of the aerosol direct forcing over the Arctic polar cap is estimated to be between −0.2 and −0.4 W m−2 for the summer months, which results in a negative feedback on the system. The model predicts that the change in first indirect aerosol effect (cloud albedo effect is approximately a factor of ten greater than the change in direct aerosol forcing although this result is highly uncertain due to the crude representation of Arctic clouds and aerosol-cloud interactions in the model. This study shows that both the natural aerosol direct and first indirect effects are strongly dependent on the surface albedo, highlighting the strong coupling between sea ice, aerosols, Arctic clouds and their radiative effects.

  2. Potential climatic effects of anthropogenic aerosols

    International Nuclear Information System (INIS)

    Pueschel, R.F.

    1993-01-01

    Aerosols act as part of the climate system through their influence on solar and terrestrial radiation. The effect of anthropogenic aerosols on the reduction of visibility is explored in this chapter. Elemental carbon has been identified as the most effective visibility-reducing species. Most of the visibility reduction is due to particles with diameter smaller than 2.5 μm. Studies indicate that sulfate is also a very important aerosol species that results in low visibility and high turbidity. Radiative properties such as aerosol single-scattering albedo values and absorption-to-backscatter ratios purported to produce warming or cooling effects of aerosols are discussed. It is concluded that aerosol clouds have a tendency to cool when they are over a low-albedo surface and have a tendency to warm when they are over high-albedo surfaces such as snow. Anthropogenic aerosols have a tendency to warm the earth's atmospheric system, based on calculations and assumed aerosol optical properties. However, this effect is somewhat offset by the absorption and re-emission into space of infrared terrestrial radiation. The net effect depends on the ratio of the absorption coefficients in the visible and infrared and also on the surface albedo. The effects on infrared radiation are documented for two anthropogenic aerosol sources in the United States, the Denver metropolitan area and power plant plumes in New Mexico, through calculations and measurements. Measured cooling rates within an aerosol plume are not sufficient to offset the warming rate due to absorption of short-wave radiation. Research indicates that anthropogenic aerosols can possibly cause local-scale warming of the atmosphere, but global-scale climatic effects remain an open question

  3. Salinization and Saline Environments

    Science.gov (United States)

    Vengosh, A.

    2003-12-01

    One of the most conspicuous phenomena of water-quality degradation, particularly in arid and semi-arid zones, is salinization of water and soil resources. Salinization is a long-term phenomenon, and during the last century many aquifers and river basins have become unsuitable for human consumption owing to high levels of salinity. Future exploitation of thousands of wells in the Middle East and in many other water-scarce regions in the world depends, to a large extent, on the degree and rate of salinization. Moreover, every year a large fraction of agricultural land is salinized and becomes unusable.Salinization is a global environmental phenomenon that affects many different aspects of our life (Williams, 2001a, b): changing the chemical composition of natural water resources (lakes, rivers, and groundwater), degrading the quality of water supply to the domestic and agriculture sectors, contribution to loss of biodiversity, taxonomic replacement by halotolerant species ( Williams, 2001a, b), loss of fertile soil, collapse of agricultural and fishery industries, changing of local climatic conditions, and creating severe health problems (e.g., the Aral Basin). The damage due to salinity in the Colorado River Basin alone, for example, ranges between 500 and 750 million per year and could exceed 1 billion per year if the salinity in the Imperial Dam increases from 700 mg L-1 to 900 mg L-1 (Bureau of Reclamation, 2003, USA). In Australia, accelerating soil salinization has become a massive environmental and economic disaster. Western Australia is "losing an area equal to one football oval an hour" due to spreading salinity ( Murphy, 1999). The annual cost for dryland salinity in Australia is estimated as AU700 million for lost land and AU$130 million for lost production ( Williams et al., 2002). In short, the salinization process has become pervasive.Salinity in water is usually defined by the chloride content (mg L-1) or total dissolved solids content (TDS, mg L-1or g

  4. The Impact of Pre-Industrial Land Use Change on Atmospheric Composition and Aerosol Radiative Forcing.

    Science.gov (United States)

    Hamilton, D. S.; Carslaw, K. S.; Spracklen, D. V.; Folberth, G.; Kaplan, J. O.; Pringle, K.; Scott, C.

    2015-12-01

    Anthropogenic land use change (LUC) has had a major impact on the climate by altering the amount of carbon stored in vegetation, changing surface albedo and modifying the levels of both biogenic and pyrogenic emissions. While previous studies of LUC have largely focused on the first two components, there has recently been a recognition that changes to aerosol and related pre-cursor gas emissions from LUC are equally important. Furthermore, it has also recently been recognised that the pre-industrial (PI) to present day (PD) radiative forcing (RF) of climate from aerosol cloud interactions (ACI) due to anthropogenic emissions is highly sensitive to the amount of natural aerosol that was present in the PI. This suggests that anthropogenic RF from ACI may be highly sensitive to land-use in the PI. There are currently two commonly used baseline reference years for the PI; 1750 and 1860. Rapid LUC occurred between 1750 and 1860, with large reductions in natural vegetation cover in Eastern Northern America, Europe, Central Russia, India and Eastern China as well as lower reductions in parts of Brazil and Africa. This LUC will have led to significant changes in biogenic and fire emissions with implications for natural aerosol concentrations and PI-to-PD RF. The focus of this study is therefore to quantify the impact of LUC between 1750 and 1860 on aerosol concentrations and PI-to-PD RF calculations from ACI. We use the UK Met Office HadGEM3-UKCA coupled-chemistry-climate model to calculate the impacts of anthropogenic emissions and anthropogenic LUC on aerosol size distributions in both 1750 and 1860. We prescribe LUC using the KK10 historical dataset of land cover change. Monoterpene emissions are coupled directly to the prescribed LUC through the JULES land surface scheme in HadGEM3. Fire emissions from LUC were calculated offline using the fire module LPJ-LMfire in the Lund-Potsdam-Jena dynamic global vegetation model. To separate out the impacts of LUC from

  5. Interannual variation in the fine-mode MODIS aerosol optical depth and its relationship to the changes in sulfur dioxide emissions in China between 2000 and 2010

    Directory of Open Access Journals (Sweden)

    S. Itahashi

    2012-03-01

    Full Text Available Anthropogenic SO2 emissions increased alongside economic development in China at a rate of 12.7% yr−1 from 2000 to 2005. However, under new Chinese government policy, SO2 emissions declined by 3.9% yr−1 between 2005 and 2009. Between 2000 and 2010, we found that the variability in the fine-mode (submicron aerosol optical depth (AOD over the oceans adjacent to East Asia increased by 3–8% yr−1 to a peak around 2005–2006 and subsequently decreased by 2–7% yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS on board NASA's Terra satellite and simulations by a chemical transport model. This trend is consistent with ground-based observations of aerosol particles at a mountainous background observation site in central Japan. These fluctuations in SO2 emission intensity and fine-mode AOD are thought to reflect the widespread installation of fuel-gas desulfurization (FGD devices in power plants in China, because aerosol sulfate is a major determinant of the fine-mode AOD in East Asia. Using a chemical transport model, we confirmed that the contribution of particulate sulfate to the fine-mode AOD is more than 70% of the annual mean and that the abovementioned fluctuation in fine-mode AOD is caused mainly by changes in SO2 emission rather than by other factors such as varying meteorological conditions in East Asia. A strong correlation was also found between satellite-retrieved SO2 vertical column density and bottom-up SO2 emissions, both of which were also consistent with observed fine-mode AOD trends. We propose a simplified approach for evaluating changes in SO2 emissions in China, combining the use of modeled sensitivity coefficients that describe the variation of fine-mode AOD with changes in SO2 emissions and satellite retrieval. Satellite measurements of fine-mode AOD

  6. MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

    Science.gov (United States)

    Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

    2017-01-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  7. Origins and composition of fine atmospheric carbonaceous aerosol in the Sierra Nevada Mountains, California

    Directory of Open Access Journals (Sweden)

    D. R. Worton

    2011-10-01

    Full Text Available In this paper we report chemically resolved measurements of organic aerosol (OA and related tracers during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX at the Blodgett Forest Research Station, California from 15 August–10 October 2007. OA contributed the majority of the mass to the fine atmospheric particles and was predominately oxygenated (OOA. The highest concentrations of OA were during sporadic wildfire influence when aged plumes were impacting the site. In situ measurements of particle phase molecular markers were dominated by secondary compounds and along with gas phase compounds could be categorized into six factors or sources: (1 aged biomass burning emissions and oxidized urban emissions, (2 oxidized urban emissions (3 oxidation products of monoterpene emissions, (4 monoterpene emissions, (5 anthropogenic emissions and (6 local methyl chavicol emissions and oxidation products. There were multiple biogenic components that contributed to OA at this site whose contributions varied diurnally, seasonally and in response to changing meteorological conditions, e.g. temperature and precipitation events. Concentrations of isoprene oxidation products were larger when temperatures were higher during the first half of the campaign (15 August–12 September due to more substantial emissions of isoprene and enhanced photochemistry. The oxidation of methyl chavicol, an oxygenated terpene emitted by ponderosa pine trees, contributed similarly to OA throughout the campaign. In contrast, the abundances of monoterpene oxidation products in the particle phase were greater during the cooler conditions in the latter half of the campaign (13 September–10 October, even though emissions of the precursors were lower, although the mechanism is not known. OA was correlated with the anthropogenic tracers 2-propyl nitrate and carbon monoxide (CO, consistent with previous observations, while being comprised of mostly non-fossil carbon

  8. TEM Study of SAFARI-2000 Aerosols

    Science.gov (United States)

    Buseck, Peter R.

    2004-01-01

    The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from biomass smoke plume s in southern Africa and from air masses in the region that are affec ted by the smoke. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and ele ctron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to study aerosol particles from several smoke and haz e samples and from a set of cloud samples.

  9. Biological Particle Emissions From a South-East Asian Tropical Rainforest Using a Real- Time Dual Channel UV Fluorescence Bio-Aerosol Spectrometer

    Science.gov (United States)

    Gabey, A.; Coe, H.; Gallagher, M.; McFiggans, G.; Kaye, P.; Stanley, W.; Foot, V.

    2008-12-01

    Primary biogenic aerosols (PBA) contribute typically up to half of coarse mode particulate loading in tropical regions (e.g. Elbert et al. 2007). PBA contribute to the spread of genetic material and hence biodiversity within the biosphere either directly by transport of the organisms or their reproductive components. This spread via various vectors contributes to disease both animal and plant. Many studies have suggested PBA might be important for initiation of cloud formation and subsequent precipitation evolution by acting as cloud condensation nuclei (CCN) or possibly as ice nuclei (IN). This link is inferred from laboratory studies demonstrating the high activation efficiency of PBA at warm temperatures, coupled with observations that biological particles are ubiquitous in the atmosphere. Despite more than two hundred years of research, e.g. Ehrenberg (1830), information on the abundance, composition and more importantly the sources and heterogeneity of PBA on global scales are still poorly understood. The first realistic estimates of global average emission rates of PBA based on observations (mainly in Amazonia) and budget calculations, were provided by Elbert et al. (2007). They demonstrate that fungi, which have evolved many passive and active spore dispersal mechanisms, contribute a major fraction of the observed PBA and coarse particulate mass (particles with diameters between 1-10 μ m) in many, but in particular, tropical regions. Two major classes of fungal spores are commonly identified, these being AAM and ABM, Acomycota and Basidiomycota respectively (we will adopt the nomenclature used by Elbert et al. 2007, in this study). These species discharge their spores via wet spore active discharge mechanisms. Elbert et al. (2007) estimate a global average spore emission rate for ABM of ~17-50 Tg yr-1. This is consistent with observed typical concentrations of ABS which range from ~103 to 104 m- 3; and ~0.1-1 μ g m-3 by mass. The global average abundance

  10. Biomass Burning Emissions of Black Carbon from African Sources

    Science.gov (United States)

    Aiken, A. C.; Leone, O.; Nitschke, K. L.; Dubey, M. K.; Carrico, C.; Springston, S. R.; Sedlacek, A. J., III; Watson, T. B.; Kuang, C.; Uin, J.; McMeeking, G. R.; DeMott, P. J.; Kreidenweis, S. M.; Robinson, A. L.; Yokelson, R. J.; Zuidema, P.

    2016-12-01

    Biomass burning (BB) emissions are a large source of carbon to the atmosphere via particles and gas phase species. Carbonaceous aerosols are emitted along with gas-phase carbon monoxide (CO) and carbon dioxide (CO2) that can be used to determine particulate emission ratios and modified combustion efficiencies. Black carbon (BC) aerosols are potentially underestimated in global models and are considered to be one of the most important global warming factors behind CO2. Half or more BC in the atmosphere is from BB, estimated at 6-9 Tg/yr (IPCC, 5AR) and contributing up to 0.6 W/m2 atmospheric warming (Bond et al., 2013). With a potential rise in drought and extreme events in the future due to climate change, these numbers are expected to increase. For this reason, we focus on BC and organic carbon aerosol species that are emitted from forest fires and compare their emission ratios, physical and optical properties to those from controlled laboratory studies of single-source BB fuels to understand BB carbonaceous aerosols in the atmosphere. We investigate BC in concentrated BB plumes as sampled from the new U.S. DOE ARM Program campaign, Layered Atlantic Smoke Interactions with Clouds (LASIC). The ARM Aerosol Mobile Facility 1 (AMF1) and Mobile Aerosol Observing System (MAOS) are currently located on Ascension Island in the South Atlantic Ocean, located midway between Angola and Brazil. The location was chosen for sampling maximum aerosol outflow from Africa. The far-field aged BC from LASIC is compared to BC from indoor generation from single-source fuels, e.g. African grass, sampled during Fire Lab At Missoula Experiments IV (FLAME-IV). BC is measured with a single-particle soot photometer (SP2) alongside numerous supporting instrumentation, e.g. particle counters, CO and CO2 detectors, aerosol scattering and absorption measurements, etc. FLAME-IV includes both direct emissions and well-mixed aerosol samples that have undergone dilution, cooling, and condensation. BC

  11. Modeling of pollution aerosols in Ile-de-France; Modelisation des aerosols de pollution en Ile-de-France

    Energy Technology Data Exchange (ETDEWEB)

    Hodzic, A

    2005-10-15

    The modeling of aerosols is a major stake in the understanding of the emission processes and evolution of particulates in the atmosphere. However, the parameterizations used in today's aerosol models still comprise many uncertainties. This work has been motivated by the need of better identifying the weaknesses of aerosols modeling tools and by the necessity of having new validation methods for a 3D evaluation of models. The studies have been carried out using the CHIMERE chemistry-transport model, which allows to simulate the concentrations and physico-chemical characteristics of pollution aerosols at the European scale and in Ile-de-France region. The validation approach used is based on the complementarity of the measurements performed on the ground by monitoring networks with those acquired during the ESQUIF campaign (study and simulation of air quality in Ile-de-France), with lidar and photometric measurements and with satellite observations. The comparison between the observations and the simulations has permitted to identify and reduce the modeling errors, and to characterize the aerosol properties in the vicinity of an urban area. (J.S.)

  12. Modeling of pollution aerosols in Ile-de-France; Modelisation des aerosols de pollution en Ile-de-France

    Energy Technology Data Exchange (ETDEWEB)

    Hodzic, A

    2005-10-15

    The modeling of aerosols is a major stake in the understanding of the emission processes and evolution of particulates in the atmosphere. However, the parameterizations used in today's aerosol models still comprise many uncertainties. This work has been motivated by the need of better identifying the weaknesses of aerosols modeling tools and by the necessity of having new validation methods for a 3D evaluation of models. The studies have been carried out using the CHIMERE chemistry-transport model, which allows to simulate the concentrations and physico-chemical characteristics of pollution aerosols at the European scale and in Ile-de-France region. The validation approach used is based on the complementarity of the measurements performed on the ground by monitoring networks with those acquired during the ESQUIF campaign (study and simulation of air quality in Ile-de-France), with lidar and photometric measurements and with satellite observations. The comparison between the observations and the simulations has permitted to identify and reduce the modeling errors, and to characterize the aerosol properties in the vicinity of an urban area. (J.S.)

  13. Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

    Science.gov (United States)

    Russell, L. M.

    2017-12-01

    Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

  14. Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

    Science.gov (United States)

    Slowik, J. G.; Stroud, C.; Bottenheim, J. W.; Brickell, P. C.; Chang, R. Y.-W.; Liggio, J.; Makar, P. A.; Martin, R. V.; Moran, M. D.; Shantz, N. C.; Sjostedt, S. J.; van Donkelaar, A.; Vlasenko, A.; Wiebe, H. A.; Xia, A. G.; Zhang, J.; Leaitch, W. R.; Abbatt, J. P. D.

    2010-03-01

    Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

  15. Aerosol numerical modelling at local scale

    International Nuclear Information System (INIS)

    Albriet, Bastien

    2007-01-01

    At local scale and in urban areas, an important part of particulate pollution is due to traffic. It contributes largely to the high number concentrations observed. Two aerosol sources are mainly linked to traffic. Primary emission of soot particles and secondary nanoparticle formation by nucleation. The emissions and mechanisms leading to the formation of such bimodal distribution are still badly understood nowadays. In this thesis, we try to provide an answer to this problematic by numerical modelling. The Modal Aerosol Model MAM is used, coupled with two 3D-codes: a CFD (Mercure Saturne) and a CTM (Polair3D). A sensitivity analysis is performed, at the border of a road but also in the first meters of an exhaust plume, to identify the role of each process involved and the sensitivity of different parameters used in the modelling. (author) [fr

  16. Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

    Science.gov (United States)

    Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

    2015-08-01

    The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging

  17. Comparison of Gasoline Direct-Injection (GDI) and Port Fuel Injection (PFI) Vehicle Emissions: Emission Certification Standards, Cold-Start, Secondary Organic Aerosol Formation Potential, and Potential Climate Impacts.

    Science.gov (United States)

    Saliba, Georges; Saleh, Rawad; Zhao, Yunliang; Presto, Albert A; Lambe, Andrew T; Frodin, Bruce; Sardar, Satya; Maldonado, Hector; Maddox, Christine; May, Andrew A; Drozd, Greg T; Goldstein, Allen H; Russell, Lynn M; Hagen, Fabian; Robinson, Allen L

    2017-06-06

    Recent increases in the Corporate Average Fuel Economy standards have led to widespread adoption of vehicles equipped with gasoline direct-injection (GDI) engines. Changes in engine technologies can alter emissions. To quantify these effects, we measured gas- and particle-phase emissions from 82 light-duty gasoline vehicles recruited from the California in-use fleet tested on a chassis dynamometer using the cold-start unified cycle. The fleet included 15 GDI vehicles, including 8 GDIs certified to the most-stringent emissions standard, superultra-low-emission vehicles (SULEV). We quantified the effects of engine technology, emission certification standards, and cold-start on emissions. For vehicles certified to the same emissions standard, there is no statistical difference of regulated gas-phase pollutant emissions between PFIs and GDIs. However, GDIs had, on average, a factor of 2 higher particulate matter (PM) mass emissions than PFIs due to higher elemental carbon (EC) emissions. SULEV certified GDIs have a factor of 2 lower PM mass emissions than GDIs certified as ultralow-emission vehicles (3.0 ± 1.1 versus 6.3 ± 1.1 mg/mi), suggesting improvements in engine design and calibration. Comprehensive organic speciation revealed no statistically significant differences in the composition of the volatile organic compounds emissions between PFI and GDIs, including benzene, toluene, ethylbenzene, and xylenes (BTEX). Therefore, the secondary organic aerosol and ozone formation potential of the exhaust does not depend on engine technology. Cold-start contributes a larger fraction of the total unified cycle emissions for vehicles meeting more-stringent emission standards. Organic gas emissions were the most sensitive to cold-start compared to the other pollutants tested here. There were no statistically significant differences in the effects of cold-start on GDIs and PFIs. For our test fleet, the measured 14.5% decrease in CO 2 emissions from GDIs was much greater than

  18. Dynamic-chemistry-aerosol modelling interaction: the ESCOMPTE 2001 experiment

    International Nuclear Information System (INIS)

    Cousin, F.

    2004-09-01

    After most pollution studies independently devoted to gases and aerosols, there now appears an urgent need to consider their interactions. In this view, an aerosol module has been implemented in the Meso-NH-C model to simulate two IOPs documented during the ESCOMPTE campaign which took place in the Marseille/Fos-Berre region in June-July 2001. First, modelled dynamic parameters (winds, temperatures, boundary layer thickness) and gaseous chemistry have been validated with measurements issued from the exhaustive ESCOMPTE database. Sensitivity analysis have also been performed using different gaseous emission inventories at various resolution. These simulations have illustrated the deep impact of both synoptic and local dynamics on observed ozone concentrations on June 24 (IOP2b) in the ESCOMPTE domain. Afterwards, the ORISAM aerosol module has been introduced into the Meso-NH-C model. Dynamics, gaseous chemistry and aerosol processes have thus been coupled on-line. The particulate pollution episode on June 24 (IOP2b) has been characterised through a satisfactory comparison, specially from sub-micron particles, between modelling and measurements at different representative stations in the domain. This study, with validation of the particulate emission inventory has also highlighted the need for future improvements, such as further characterisation of organic and inorganic aerosol species and consideration of coarse particles. Aerosol impact on gaseous chemistry has been preliminary approached in view of future development and modification to be given to the Meso-NH-C model. (author)

  19. Organic aerosol formation in citronella candle plumes

    OpenAIRE

    Bothe, Melanie; Donahue, Neil McPherson

    2010-01-01

    Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In rep...

  20. Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone

    Science.gov (United States)

    Yu, Pengfei; Rosenlof, Karen H.; Liu, Shang; Telg, Hagen; Thornberry, Troy D.; Rollins, Andrew W.; Portmann, Robert W.; Bai, Zhixuan; Ray, Eric A.; Duan, Yunjun; Pan, Laura L.; Toon, Owen B.; Bian, Jianchun; Gao, Ru-Shan

    2017-07-01

    An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (˜15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (˜35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.

  1. Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

    Directory of Open Access Journals (Sweden)

    N. Meskhidze

    2011-11-01

    Full Text Available Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR's Community Atmosphere Model (CAM5 with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7. Emissions of marine primary organic aerosols (POA, phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA and methane sulfonate (MS are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr−1, for the Gantt et al. (2011 and Vignati et al. (2010 emission parameterizations, respectively. Marine sources of SOA and particulate MS (containing both sulfur and carbon atoms contribute an additional 0.2 and 5.1 Tg yr−1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m−3, with values up to 400 ng m−3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2, both Gantt et al. (2011 and Vignati et al. (2010 formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011 parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN. The largest increases (up to 20% in CCN (at a supersaturation (S of 0.2% number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming

  2. Assessment of Atmospheric heavy metal deposition in North Egypt aerosols using neutron activation analysis and optical emission inductively coupled plasma

    International Nuclear Information System (INIS)

    El-Araby, E.H.; Abd El-Wahab, M.; Diab, H.M.; El-Desouky, T.M.; Mohsen, M.

    2011-01-01

    The aim of the present study is to assess the current level of atmospheric heavy metal pollution of aerosols in different cities of North Egypt using the neutron activation analysis and optical emission inductively coupled plasma techniques. The results revealed that the highest concentrations of particulate matter PM 10 and total suspended particulate matter were close to industrial areas. From the results of the enrichment factor calculations, the most significant elements of anthropogenic origin are Ba, Sb, Ce and Zn. - Highlights: → Average concentration of Cd using OE-ICP is below detection limit for all the samples. → Maximum average concentration of Pb in PM10 and TSP is 5425 and 570.3, respectively. → Concentration of 20 elements in PM 10 and TSP aerosols are determined using the NAA. → EF revealed that Pb, Ba, Br, Ce, Hf, La Sb and Zn are of anthropogenic origin.

  3. Simulation of the anthropogenic aerosols over South Asia and their effects on Indian summer monsoon

    Energy Technology Data Exchange (ETDEWEB)

    Ji, Zhenming [Institute of Tibetan Plateau Research, Chinese Academy of Sciences, Key Laboratory of Tibetan Environment Changes and Land Surface Processes, Beijing (China); National Climate Center, Beijing (China); Graduate University of Chinese Academy of Sciences, Beijing (China); Kang, Shichang [Institute of Tibetan Plateau Research, Chinese Academy of Sciences, Key Laboratory of Tibetan Environment Changes and Land Surface Processes, Beijing (China); Chinese Academy of Sciences, State Key Laboratory of Cryospheric Science, Lanzhou (China); Zhang, Dongfeng [Shanxi Meteorological Bureau, Taiyuan (China); Zhu, Chunzi [Nanjing University of Information Science Technology, College of Atmospheric Science, Nanjing (China); Wu, Jia; Xu, Ying [National Climate Center, Beijing (China)

    2011-05-15

    A regional climate model coupled with a chemistry-aerosol model is employed to simulate the anthropogenic aerosols including sulfate, black carbon and organic carbon and their direct effect on climate over South Asia. The model is driven by the NCAR/NCEP re-analysis data. Multi-year simulations with half, normal and double emission fluxes are conducted. Results show that the model performs well in reproducing present climate over the region. Simulations of the aerosol optical depth and surface concentration of aerosols are also reasonable although to a less extent. The negative radiative forcing is found at the top of atmosphere and largely depended on emission concentration. Surface air temperature decreases by 0.1-0.5 C both in pre-monsoon and monsoon seasons. The range and intensity of cooling areas enlarge while aerosol emission increases. Changes in precipitation are between -25 and 25%. Different diversifications of rainfall are showed with three emission scenarios. The changes of precipitation are consistent with varieties of monsoon onset dates in pre-monsoon season. In the regions of increasing precipitation, monsoon onset is advanced and vice versa. In northeast India and Myanmar, aerosols lead the India summer monsoon onset advancing 1-2 pentads, and delaying by 1-2 pentads in central and southeast India. These changes are mainly caused by the anomaly of local Hadley circulations and enhancive precipitation. Tibetan Plateau played a crucial role in the circulation changes. (orig.)

  4. A new nebulization device with exchangeable aerosol generation mode as a useful tool to investigate sample introduction processes in inductively coupled plasma atomic emission spectrometry

    International Nuclear Information System (INIS)

    Grotti, Marco; Lagomarsino, Cristina; Frache, Roberto

    2004-01-01

    A new sample introduction device has been designed in order to differentiate between the effects of the aerosol production and its following desolvation on analytical performances of an inductively coupled plasma optical spectrometer. This research tool allows to easily switch between the pneumatic and ultrasonic aerosol generation mode and to use a joint desolvation chamber. In this way, a real comparison between aerosol production systems may be attained and the influence of aerosol generation process on analytical figures clearly distinguished from that of the desolvation process. In this work, the separate effects of the aerosol generation and desolvation processes on analytical sensitivity and tolerance towards matrix effects have been investigated. Concerning sensitivity, it was found that both the processes play an important role in determining emission intensities, being the increase in sensitivity due to desolvation higher than that due to the improved aerosol generation efficiency. Concerning the matrix effects, a predominant role of the desolvation system was found, while the influence of the aerosol generation mode was much less important. For nitric acid, the decreasing effect was mitigated by the presence of a desolvation system, due to partial removal of the acid. On the contrary, the depressive effect of sulfuric acid was enhanced by the presence of a desolvation system, due to degradation of the solvent removal efficiency and to further decrease in the analyte transport rate caused by clustering phenomena. Concerning the interferences due to sodium and calcium, a depressive effect was observed, which is enhanced by desolvation

  5. Hydrochemical measures and salinity studies in Inhanhuns' waters, Ceara State, Brazil

    International Nuclear Information System (INIS)

    Lima, Carlos Henrique; Santiago, Marlucia Freitas; Mendes Filho, Josue; Frischkorn, Horst

    1996-08-01

    The Inhamuns region is one of the most arid in Ceara Waters exhibit very high salinity. Here we evaluate measurements of chemical parameters (electrical conductivity, EC, and major ions) and δ 18 O for waters from wells, springs and surface reservoirs. Results show that springs, with EC of up to nearly 5000 μS/cm, are fed by pluvial water, exchange through dams can be excluded. Electrical conductivity is well correlated with Na + Mg ++ and Cl - for waters of various origins, whereas Ca ++ correlates reasonably only for wells. We conclude that aerosol deposition is a major source of salt, Enrichment through evaporation constitutes the most important process for surface water salination. Dissolution of chlorite-silicates is the cause for the magnesian character of underground water. (author)

  6. Potential of secondary aerosol formation from Chinese gasoline engine exhaust.

    Science.gov (United States)

    Du, Zhuofei; Hu, Min; Peng, Jianfei; Guo, Song; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Qin, Yanhong; Niu, He; Li, Mengren; Yang, Yudong; Lu, Sihua; Wu, Yusheng; Shao, Min; Shuai, Shijin

    2018-04-01

    Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds (VOCs). However, little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4-5hr simulation, which was estimated to represent more than 10days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol (SOA) production was 426±85mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China. Copyright © 2017. Published by Elsevier B.V.

  7. Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    U. Lohmann

    2007-07-01

    Full Text Available The double-moment cloud microphysics scheme from ECHAM4 that predicts both the mass mixing ratios and number concentrations of cloud droplets and ice crystals has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass, number concentrations and mixing state. The simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and −35° C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient.

    The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to −1.9 W m−2 in ECHAM5, when a relative humidity dependent cloud cover scheme and aerosol emissions representative for the years 1750 and 2000 from the AeroCom emission inventory are used. The contribution of the cloud albedo effect amounts to −0.7 W m−2. The total anthropogenic aerosol effect is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed because the cloud lifetime effect increases.

  8. GHG AND AEROSOL EMISSION FROM FIRE PIXEL DURING CROP RESIDUE BURNING UNDER RICE AND WHEAT CROPPING SYSTEMS IN NORTH-WEST INDIA

    Directory of Open Access Journals (Sweden)

    P. Acharya

    2016-10-01

    Full Text Available Emission of smoke and aerosol from open field burning of crop residue is a long-standing subject matter of atmospheric pollution. In this study, we proposed a new approach of estimating fuel load in the fire pixels and corresponding emissions of selected GHGs and aerosols i.e. CO2, CO, NO2, SO2, and total particulate matter (TPM due to burning of crop residue under rice and wheat cropping systems in Punjab in north-west India from 2002 to 2012. In contrasts to the conventional method that uses RPR ratio to estimate the biomass, fuel load in the fire pixels was estimated as a function of enhanced vegetation index (EVI. MODIS fire products were used to detect the fire pixels during harvesting seasons of rice and wheat. Based on the field measurements, fuel load in the fire pixels were modelled as a function of average EVI using second order polynomial regression. Average EVI for rice and wheat crops that were extracted through Fourier transformation were computed from MODIS time series 16 day EVI composites. About 23 % of net shown area (NSA during rice and 11 % during wheat harvesting seasons are affected by field burning. The computed average fuel loads are 11.32 t/ha (±17.4 during rice and 10.89 t/ha (±8.7 during wheat harvesting seasons. Calculated average total emissions of CO2, CO, NO2, SO2 and TPM were 8108.41, 657.85, 8.10, 4.10, and 133.21 Gg during rice straw burning and 6896.85, 625.09, 1.42, 1.77, and 57.55 Gg during wheat burning. Comparison of estimated values shows better agreement with the previous concurrent estimations. The method, however, shows its efficiency parallel to the conventional method of estimation of fuel load and related pollutant emissions.

  9. A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

    Science.gov (United States)

    Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

    2010-01-01

    Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

  10. Relationship between trace gases and aerosols from biomass burning in Southeast Asia using satellite and emission data

    Science.gov (United States)

    Azuma, Yoshimi; Nakamura, Maya; Kuji, Makoto

    2012-11-01

    Southeast Asia is one of the biggest regions of biomass burning with forest fires and slash-and-burn farming. From the fire events, a large amount of air pollutants are emitted such as carbon monoxide (CO), nitrogen oxide (NOx) and aerosol (black carbon; BC). Biomass burning generally causes not only local, but also transboundary air pollution, and influences the atmospheric environment in the world accordingly. However, impact of air pollutants' emissions from large-scale fire in Southeast Asia is not well investigated compared to other regions such as South America and Africa. In this study, characteristics of the atmospheric environment were investigated with correlative analyses among several satellite data (MOPITT, OMI, and MODIS) and emission inventory (GFEDv3) in Southeast Asia from October 2004 to June 2008 on a monthly basis. As a result, it is suggested that the transboundary air pollution from the biomass burning regions occurred over Southeast Asia, which caused specifically higher air pollutants' concentration at Hanoi, Vietnam in spring dry season.

  11. Secondary Aerosol Formation over the ESCOMPTE Area: Results from airborne Aerosol and Trace Gas Measurements

    Science.gov (United States)

    van Dingenen, R.; Martins-Dos Santos, S.; Putaud, J. P.; Allet, C.; Bretton, E.; Perros, P.

    2003-04-01

    From June 10th to July 14th 2001, the ESCOMPTE campaign took place in the Marseille-Berre area in Southern France. The goal of the campaign was to produce a high quality 3-D data base from emissions, transport and air composition measurements during urban photochemical pollution episodes at the meso-scale. The CAATER AEROPLUM project was embedded within this international field campaign. AEROPLUM aimed at mapping size distributions of aerosols and photo-oxidants in the mixed layer over the ESCOMPTE domain, using the ARAT Fokker 27 as measurement platform. Aircraft sub-micrometer aerosol measurements are validated during overpasses against ground-based measurements, carried out with similar instrumentation. We will present and discuss data during periods of seabreeze, transporting coastal industrial and urban pollution land-inwards. This leads to intense photochemical activity, evidenced by elevated O_3 concentrations and aerosol levels.

  12. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    Science.gov (United States)

    Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

    2015-12-01

    The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi-volatile oxygenated OA (SV-OOA; 16 % of total OA; O / C = 0.63) and low volatility oxygenated OA (LV-OOA; 24 % of total OA; O / C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a~previous wintertime campaign (winter 2010), most notably that PM1 concentrations were nearly three times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 to 12:00 PST. This is an indication that nighttime chemistry might also be

  13. On the Link Between Ocean Biota Emissions, Aerosol, and Maritime Clouds: Airborne, Ground, and Satellite Measurements Off the Coast of California

    Science.gov (United States)

    2009-10-14

    Simpson, 1948; Lovelock et al., 1972; Andreae, 1990; Leck et al., 1990). Facchini et al. (2008a) have also shown that biogenic emissions are a...fastigiata, Dimethyl-2- carboxy-ethylsulphonium hydroxide and its salts, J. Chem. Soc., 3, 1591-1597. Charlson, R. J., Lovelock , J. E., Andreae...aerosols for pristine Arctic clouds, Tellus, 57B, 261-268. Lovelock , J. E., Maggs, R. J., and R. A. Rasmussen (1972). Atmospheric dimethyl sulfide and

  14. Evaluation of aerosol distributions in the GISS-TOMAS global aerosol microphysics model with remote sensing observations

    Directory of Open Access Journals (Sweden)

    Y. H. Lee

    2010-03-01

    Full Text Available The Aerosol Optical Depth (AOD and Angstrom Coefficient (AC predictions in the GISS-TOMAS model of global aerosol microphysics are evaluated against remote sensing data from MODIS, MISR, and AERONET. The model AOD agrees well (within a factor of two over polluted continental (or high sulfate, dusty, and moderate sea-salt regions but less well over the equatorial, high sea-salt, and biomass burning regions. Underprediction of sea-salt in the equatorial region is likely due to GCM meteorology (low wind speeds and high precipitation. For the Southern Ocean, overprediction of AOD is very likely due to high sea-salt emissions and perhaps aerosol water uptake in the model. However, uncertainties in cloud screening at high latitudes make it difficult to evaluate the model AOD there with the satellite-based AOD. AOD in biomass burning regions is underpredicted, a tendency found in other global models but more severely here. Using measurements from the LBA-SMOCC 2002 campaign, the surface-level OC concentration in the model are found to be underpredicted severely during the dry season while much less severely for EC concentration, suggesting the low AOD in the model is due to underpredictions in OM mass. The potential for errors in emissions and wet deposition to contribute to this bias is discussed.

  15. 2-D model of global aerosol transport

    Energy Technology Data Exchange (ETDEWEB)

    Rehkopf, J; Newiger, M; Grassl, H

    1984-01-01

    The distribution of aerosol particles in the troposphere is described. Starting with long term mean seasonal flow and diffusivities as well as temperature, cloud distribution (six cloud classes), relative humidity and OH radical concentration, the steady state concentration of aerosol particles and SO/sub 2/ are calculated in a two-dimensional global (height and latitude) model. The following sources and sinks for particles are handled: direct emission, gas-to-particle conversion from SO/sub 2/, coagulation, rainout, washout, gravitational settling, and dry deposition. The sinks considered for sulphur emissions are dry deposition, washout, rainout, gasphase oxidation, and aqueous phase oxidation. Model tests with the water vapour cycle show a good agreement between measured and calculated zonal mean precipitation distribution. The steady state concentration distribution for natural emissions reached after 10 weeks model time, may be described by a mean exponent ..cap alpha.. = 3.2 near the surface assuming a modified Junge distribution and an increased value, ..cap alpha.. = 3.7, for the combined natural and man-made emission. The maximum ground level concentrations are 2000 and 10,000 particules cm/sup -3/ for natural and natural plus man-made emissions, respectively. The resulting distribution of sulphur dioxide agrees satisfactorily with measurements given by several authors. 37 references, 4 figures.

  16. Herbivory by an Outbreaking Moth Increases Emissions of Biogenic Volatiles and Leads to Enhanced Secondary Organic Aerosol Formation Capacity.

    Science.gov (United States)

    Yli-Pirilä, Pasi; Copolovici, Lucian; Kännaste, Astrid; Noe, Steffen; Blande, James D; Mikkonen, Santtu; Klemola, Tero; Pulkkinen, Juha; Virtanen, Annele; Laaksonen, Ari; Joutsensaari, Jorma; Niinemets, Ülo; Holopainen, Jarmo K

    2016-11-01

    In addition to climate warming, greater herbivore pressure is anticipated to enhance the emissions of climate-relevant biogenic volatile organic compounds (VOCs) from boreal and subarctic forests and promote the formation of secondary aerosols (SOA) in the atmosphere. We evaluated the effects of Epirrita autumnata, an outbreaking geometrid moth, feeding and larval density on herbivore-induced VOC emissions from mountain birch in laboratory experiments and assessed the impact of these emissions on SOA formation via ozonolysis in chamber experiments. The results show that herbivore-induced VOC emissions were strongly dependent on larval density. Compared to controls without larval feeding, clear new particle formation by nucleation in the reaction chamber was observed, and the SOA mass loadings in the insect-infested samples were significantly higher (up to 150-fold). To our knowledge, this study provides the first controlled documentation of SOA formation from direct VOC emission of deciduous trees damaged by known defoliating herbivores and suggests that chewing damage on mountain birch foliage could significantly increase reactive VOC emissions that can importantly contribute to SOA formation in subarctic forests. Additional feeding experiments on related silver birch confirmed the SOA results. Thus, herbivory-driven volatiles are likely to play a major role in future biosphere-vegetation feedbacks such as sun-screening under daily 24 h sunshine in the subarctic.

  17. The background aerosol in the lower stratosphere and the tropospheric aerosol in the Alps. Final report; Das Hintergrundaerosol der unteren Stratosphaere und das troposphaerische Aerosol der Alpen. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Jaeger, H.; Trickl, T.

    2001-06-04

    As a contribution to the German Aerosol-Lidar Network lidar backscatter measurements have been carried out at Garmisch-Partenkirchen in a wide range of the atmosphere from next to the ground to altitudes beyond 30 km. The investigations, on one hand, were devoted to establishing a climatology of the aerosol extinction coefficient for the northern Alps and to prolonging the long-term measurement series of the stratospheric aerosol. On the other hand, aerosol was used as a tracer of polluted air masses in atmospheric transport studies (orographically induced vertical transport, advection of Saharan dust, as well as aerosol advection from the North american boundary layer and from large-scale wild fire in the United States and Canada). These transport processes given the seasonal cycle of the aerosol throughout the troposphere. In the free troposphere a pronounced spring-time aerosol maximum was found. The stratospheric aerosol concentration had decayed to a background-type level during the reporting period. As a consequence, the influence of smaller aerosol contributions could be distinguished such as the eruption of the volcano Shishaldin (Alaska) and aircraft emissions. (orig.) [German] Im Rahmen des deutschen Aerosollidarnetzes wurden in Garmisch-Partenkirchen Lidar-Rueckstreumessungen in einem weiten Bereich der Atmosphaere von Bodennaehe bis in ueber 30 km Hoehe durchgefuehrt. Die Arbeiten dienten zum einen der Erstellung einer Klimatologie des Aerosol-Extinktionskoeffizienten fuer die Nordalpen sowie der Verlaengerung der seit 1976 erstellten Langzeitmessreihe des stratosphaerischen Aerosols. Zum anderen fanden atmosphaerische Transportstudien statt, bei denen das Aerosol als 'Tracer' fuer Luftverschmutzung verwendet wurde (orographisch induzierter Vertikaltransport, Advektion von Saharastaub und Aerosoladvektion aus der nordamerikanischen Genzschicht und von grossflaechigen Waldbraenden in den U.S.A. und Kanada). Diese Transportprozesse bestimmen den

  18. Secondary organic aerosol importance in the future atmosphere

    International Nuclear Information System (INIS)

    Tsigaridis, K.; Kanakidou, M.

    2007-01-01

    In order to investigate the secondary organic aerosol (SOA) response to changes in biogenic volatile organic compounds (VOC) emissions in the future atmosphere and how important will SOA be relative to the major anthropogenic aerosol component (sulfate), the global three-dimensional chemistry/transport model TM3 has been used. Emission estimates of biogenic VOC (BVOC) and anthropogenic gases and particles from the literature for the year 2100 have been adopted. According to our present-day model simulations, isoprene oxidation produces 4.6 Tg SOA yr -1 , that is less than half of the 12.2 Tg SOA yr -1 formed by the oxidation of other BVOC. In the future, nitrate radicals and ozone become more important than nowadays, but remain minor oxidants for both isoprene and aromatics. SOA produced by isoprene is estimated to almost triple, whereas the production from other BVOC more than triples. The calculated future SOA burden change, from 0.8 Tg at present to 2.0 Tg in the future, is driven by changes in emissions, oxidant levels and pre-existing particles. The non-linearity in SOA formation and the involved chemical and physical feedbacks prohibit the quantitative attribution of the computed changes to the above-mentioned individual factors. In 2100, SOA burden is calculated to exceed that of sulfate, indicating that SOA might become more important than nowadays. These results critically depend on the biogenic emissions and thus are subject to the high uncertainty associated with these emissions estimated due to the insufficient knowledge on plant response to carbon dioxide changes. Nevertheless, they clearly indicate that the change in oxidants and primary aerosol caused by human activities can contribute as much as the change in BVOC emissions to the increase of the biogenic SOA production in the future atmosphere. (authors)

  19. Aerosol Optical Properties in Southeast Asia From AERONET Observations

    Science.gov (United States)

    Eck, T. F.; Holben, B. N.; Boonjawat, J.; Le, H. V.; Schafer, J. S.; Reid, J. S.; Dubovik, O.; Smirnov, A.

    2003-12-01

    There is little published data available on measured optical properties of aerosols in the Southeast Asian region. The AERONET project and collaborators commenced monitoring of aerosol optical properties in February 2003 at four sites in Thailand and two sites in Viet Nam to measure the primarily anthropogenic aerosols generated by biomass burning and fossil fuel combustion/ industrial emissions. Automatic sun/sky radiometers at each site measured spectral aerosol optical depth in 7 wavelengths from 340 to 1020 nm and combined with directional radiances in the almucantar, retrievals were made of spectral single scattering albedo and aerosol size distributions. Angstrom exponents, size distributions and spectral single scattering albedo of primarily biomass burning aerosols at rural sites are compared to measurements made at AERONET sites in other major biomass burning regions in tropical southern Africa, South America, and in boreal forest regions. Additionally, the aerosol single scattering albedo and size distributions measured in Bangkok, Thailand are compared with those measured at other urban sites globally. The influences of aerosols originating from other regions outside of Southeast Asia are analyzed using trajectory analyses. Specifically, cases of aerosol transport and mixing from Southern China and from India are presented.

  20. Effects of emission reductions on organic aerosol in the southeastern United States

    Directory of Open Access Journals (Sweden)

    C. L. Blanchard

    2016-01-01

    Full Text Available Long-term (1999 to 2013 data from the Southeastern Aerosol Research and Characterization (SEARCH network are used to show that anthropogenic emission reductions led to important decreases in fine-particle organic aerosol (OA concentrations in the southeastern US On average, 45 % (range 25 to 63 % of the 1999 to 2013 mean organic carbon (OC concentrations are attributed to combustion processes, including fossil fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC, carbon monoxide (CO, and nitrogen oxides (NOx. The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 µg m−3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 µg m−3 (68 % of total OC to 1.4 ± 0.1 µg m−3 (60 % of total OC between 1999 and 2013 at the urban Atlanta, Georgia, site (JST and from 2.9 ± 0.4 µg m−3 (39 % of total OC to 0.7 ± 0.1 µg m−3 (30 % of total OC between 2001 and 2013 at the urban Birmingham, Alabama (BHM, site. The urban OC declines coincide with reductions of motor vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 µg m−3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 µg m−3 in 2001 to 0.2 ± 0.03 µg m−3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass burning tracer indicate that biomass burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4 ranging from 0.3 to 1.0 µg m−3 on average, representing  ∼  25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC identified with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4

  1. General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI – integrating aerosol research from nano to global scales

    Directory of Open Access Journals (Sweden)

    D. Simpson

    2011-12-01

    Full Text Available In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI. EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b comprehensive aerosol measurements in four developing countries, (c a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

  2. Equilibrium climate response of the East Asian summer monsoon to forcing of anthropogenic aerosol species

    Science.gov (United States)

    Wang, Zhili; Wang, Qiuyan; Zhang, Hua

    2017-12-01

    We used an online aerosol-climate model to study the equilibrium climate response of the East Asian summer monsoon (EASM) to increases in anthropogenic emissions of sulfate, organic carbon, and black carbon aerosols from 1850 to 2000. Our results show that each of these aerosol species has a different effect on the EASM as a result of changes in the local sea-land thermal contrast and atmospheric circulation. The increased emission of sulfate aerosol leads to a decrease in the thermal contrast between the land and ocean, a southward shift of the East Asian subtropical jet, and significant northerly wind anomalies at 850 hPa over eastern China and the ambient oceans, markedly dampening the EASM. An increase in organic carbon aerosol results in pronounced surface cooling and the formation of an anomalous anticyclone over the oceans north of 30°N. These effects cause a slight increase in the sea-land thermal contrast and southerly flow anomalies to the west of the anticyclonic center, strengthening the northern EASM. An increase in organic carbon emission decreases the sea-land thermal contrast over southern China, which weakens the southern EASM. The response of the summer 850-hPa winds and rainfall over the East Asian monsoon region to an increase in black carbon emission is generally consistent with the response to an increase in organic carbon. The increase in black carbon emission leads to a strengthening of the northern EASM north of 35°N and a slight weakening of the southern EASM south of 35°N. The simulated response of the EASM to the increase in black carbon emission is unchanged when the emission of black carbon is scaled up by five times its year 2000 levels, although the intensities of the response is enhanced. The increase in sulfate emission primarily weakens the EASM, whereas the increases in black carbon and organic carbon emissions mitigate weakening of the northern EASM.

  3. Stratospheric Aerosol Measurements

    Science.gov (United States)

    Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

    1998-01-01

    Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

  4. Fractional iron solubility of aerosol particles enhanced by biomass burning and ship emission in Shanghai, East China.

    Science.gov (United States)

    Fu, H B; Shang, G F; Lin, J; Hu, Y J; Hu, Q Q; Guo, L; Zhang, Y C; Chen, J M

    2014-05-15

    In terms of understanding Fe mobilization from aerosol particles in East China, the PM2.5 particles were collected in spring at Shanghai. Combined with the backtrajectory analysis, the PM2.5/PM10 and Ca/Al ratios, a serious dust-storm episode (DSE) during the sampling was identified. The single-particle analysis showed that the major iron-bearing class is the aluminosilicate dust during DSE, while the Fe-bearing aerosols are dominated by coal fly ash, followed by a minority of iron oxides during the non-dust storm days (NDS). Chemical analyses of samples showed that the fractional Fe solubility (%FeS) is much higher during NDS than that during DSE, and a strong inverse relationship of R(2)=0.967 between %FeS and total atmospheric iron loading were found, suggested that total Fe (FeT) is not controlling soluble Fe (FeS) during the sampling. Furthermore, no relationship between FeS and any of acidic species was established, suggesting that acidic process on aerosol surfaces are not involved in the trend of iron solubility. It was thus proposed that the source-dependent composition of aerosol particles is a primary determinant for %FeS. Specially, the Al/Fe ratio is poorly correlated (R(2)=0.113) with %FeS, while the apparent relationship between %FeS and the calculated KBB(+)/Fe ratio (R(2)=0.888) and the V/Fe ratio (R(2)=0.736) were observed, reflecting that %FeS could be controlled by both biomass burning and oil ash from ship emission, rather than mineral particles and coal fly ash, although the latter two are the main contributors to the atmospheric Fe loading during the sampling. Such information can be useful improving our understanding on iron solubility on East China, which may further correlate with iron bioavailability to the ocean, as well as human health effects associated with exposure to fine Fe-rich particles in densely populated metropolis in China. Copyright © 2014 Elsevier B.V. All rights reserved.

  5. Seasonal variation of marine organic aerosols in the North Pacific Ocean

    Science.gov (United States)

    Fu, P.; Kawamura, K.

    2017-12-01

    Atmospheric aerosols were collected in the marine boundary layer during five marine cruises in the northern Pacific Ocean from October 1996 to July 1997. Organic molecular compositions of the marine aerosols were measured using gas chromatography/mass spectrometry (GC/MS). Higher concentrations of levoglucosan and its isomers, the biomass-burning tracers, were observed in the coastal regions than those in the central north Pacific. Seasonal trends of biomass burning tracers were found to be higher in fall-winter-spring than in summer, suggesting an enhanced influence of continental aerosols to the marine atmosphere during cold seasons when the westerlies prevail. However, the atmospheric levels of secondary organic aerosol (SOA) tracers from the photooxidation of isoprene and monoterpenes were higher in warm seasons than cold seasons, which are in accordance with the enhanced emissions of biogenic volatile organic compounds (BVOCs) in summer. Stable C isotope ratios of total carbon (δ13CTC) in the marine aerosols ranged from -28.5‰ to -23.6‰ (mean -26.4‰), suggesting an important input of terrestrial/continental aerosol particles. Stable N isotope ratios (2.6‰ to 12.9‰, mean 7.1‰) were found to be higher in the coastal regions than those in the open oceans, suggesting an enhanced emission of marine aerosols in the open oceans. The fluorescence properties of the water-soluble organic carbon (WSOC) in the marine aerosols conform the importance of marine emitted organics in the open ocean, especially during the high biological activity periods.

  6. Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

    Science.gov (United States)

    Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

    2014-09-15

    The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic

  7. Study of aerosol sample interaction with dc plasma in the presence of oscillating magnetic field

    International Nuclear Information System (INIS)

    Stoiljkovic, M.M.; Pavlovic, M.S.; Savovic, J.; Kuzmanovic, M.; Marinkovic, M.

    2005-01-01

    Oscillating magnetic field was used to study the efficiency of the aerosol sample introduction into the dc plasma. At atmospheric plasmas, the effect of magnetic field is reduced to Lorentz forces on the current carrying plasma, which produces motion of the plasma. The motion velocity of dc plasma caused by oscillating magnetic field was correlated to spectral emission enhancement of analytes introduced as aerosols. Emission enhancement is the consequence of the reduced barrier to introduction of analyte species and aerosol particles into the hot plasma region. Two hypotheses described in the literature for the origin of the barrier are considered: (i) barrier induced by temperature field is based upon the thermophoretic forces on the aerosol particles when their radius is comparable to the molecular free path in the surrounding gas and (ii) barrier induced by radial electric field, recently described, that originates from gradients of charged particles in radial direction. Correlation between ionization energy of the analyte atoms with experimental emission enhancement obtained by the use of oscillating magnetic field indicates that mechanism (ii) based upon the radial electric field is predominant. The ultimate emission enhancement and possible analytical advantage is discussed

  8. Modification of combustion aerosols in the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Weingartner, E [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

    1996-07-01

    Combustion aerosols particles are released on large scale into the atmosphere in the industrialized regions as well as in the tropics (by wood fires). The particles are subjected to various aging processes which depend on the size, morphology, and chemical composition of the particles. The interaction of combustion particles with sunlight and humidity as well as adsorption and desorption of volatile material to or from the particles considerably changes their physical and chemical properties and thus their residence time in the atmosphere. This is of importance because combustion particles are known to have a variety of health effects on people. Moreover, atmospheric aerosol particles have an influence on climate, directly through the reflection and absorption of solar radiation and indirectly through modifying the optical properties and lifetime of clouds. In a first step, a field experiment was carried out to study the sources and characteristics of combustion aerosols that are emitted from vehicles in a road tunnel. It was found that most of the fine particles were tail pipe emissions of diesel powered vehicles. The calculation shows that on an average these vehicles emit about 300 mg fine particulate matter per driven kilometer. This emission factor is at least 100 times higher than the mean emission factor estimated for gasoline powered vehicles. Furthermore, it is found that during their residence time in the tunnel, the particles undergo significant changes: The particles change towards a more compact structure. The conclusion is reached that this is mainly due to adsorption of volatile material from the gas phase to the particle surface. In the atmosphere, the life cycle as well as the radiative and chemical properties of an aerosol particle is strongly dependent on its response to humidity. Therefore the hygroscopic behavior of combustion particles emitted from single sources (i.e. from a gasoline and a diesel engine) were studied in laboratory experiments.

  9. Fission product vapour - aerosol interactions in the containment: simulant fuel studies

    International Nuclear Information System (INIS)

    Beard, A.M.; Benson, C.G.; Bowsher, B.R.

    1988-12-01

    Experiments have been conducted in the Falcon facility to study the interaction of fission product vapours released from simulant fuel samples with control rod aerosols. The aerosols generated from both the control rod and fuel sample were chemically distinct and had different deposition characteristics. Extensive interaction was observed between the fission product vapours and the control rod aerosol. The two dominant mechanisms were condensation of the vapours onto the aerosol, and chemical reactions between the two components; sorption phenomena were believed to be only of secondary importance. The interaction of fission product vapours and reactor materials aerosols could have a major impact on the transport characteristics of the radioactive emission from a degrading core. (author)

  10. Micrometeorological flux measurements of aerosol and gases above Beijing

    Science.gov (United States)

    Nemitz, Eiko; Langford, Ben; Mullinger, Neil; Cowan, Nicholas; Coyle, Mhairi; Acton, William Joe; Lee, James; Fu, Pingqing

    2017-04-01

    Air pollution is estimated to cause 1.6 million premature deaths in China every year and in the winter 2016/17 Beijing had to issue health alerts and put in place ad hoc limitations on industrial and vehicular activity. Much of this pollution is attributed to emissions from industrial processes and in particular coal combustion. By contrast, the diffuse pollutant sources within the city are less well understood. This includes, e.g., emissions from the Beijing traffic fleet, the sewage system, food preparation, solid fuel combustion in the streets and small industrial processes. Within the framework of a major UK-Chinese collaboration to study air pollution and its impact on human health in Beijing, we therefore measured fluxes of a large range of pollutants from a height of 102 m on the 325 m meteorological tower at the Institute of Atmospheric Physics. Several instruments were mounted at 102 m: fluxes of CO2 and H2O were measured with an infrared gas analyser (LiCOR 7500) and fluxes of ozone with a combination of a relative fast-response ozone analyser (ROFI) and a 2B absolute O3 instrument. Total particle number fluxes were measured with a condensation particle counter (TSI CPC 3785), and size-segregated fluxes over the size range 0.06 to 20 μm with a combination of an optical Ultrafine High Sensitivity Aerosol Spectrometer (UHSAS) and an Aerodynamic Particle Sizer Spectrometer (TSI APS3321). Ammonia (NH3) fluxes were measured for the first time above the urban environment using an Aerodyne compact quantum cascade laser (QCL). In addition, composition resolved aerosol fluxes were measured with an Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS), operated in a measurement container at the bottom of the tower, which subsampled from a 120 m long copper tube (15 mm OD). The analysis so far suggests that, due to often low wind speeds, fluxes were at times de-coupled from the surface. Fluxes normalised by CO2, a tracer for the amount of fossil fuel consumed, should be

  11. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

    Science.gov (United States)

    Gantt, B.; Kelly, J. T.; Bash, J. O.

    2015-11-01

    Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

  12. Improved Near Real Time WRF-Chem Volcanic Emission Prediction and Impacts of Ash Aerosol on Weather.

    Science.gov (United States)

    Stuefer, M.; Webley, P. W.; Hirtl, M.

    2017-12-01

    We use the numerical Weather Research Forecasting (WRF) model with online Chemistry (WRF-Chem) to investigate the regional effects of volcanic aerosol on weather. A lot of observational data have become available since the Icelandic eruption of Eyjafjallajökull in spring 2010. The observed plume characteristics and meteorological data have been exploited for volcanic WRF-Chem case studies. We concluded that the Eyjafjallajökull ash plume resulted in significant direct aerosol effects altering the state of the atmosphere over large parts of Europe. The WRF-Chem model runs show near surface temperature differences up to 3ºC, altered vertical stability, changed pressure- and wind fields within the atmosphere loaded with ash aerosol. The modeled results have been evaluated with lidar network data, and ground and balloon based observations all over Europe. Besides case studies, we use WRF-Chem to build an improved volcanic ash decision support system that NOAA can use within the Volcanic Ash Advisory Center (VAAC) system. Realistic eruption source parameter (ESP) estimates are a main challenge in predicting volcanic emission dispersion in near real time. We implemented historic ESP into the WRF-Chem preprocessing routine, which can be used as a first estimate to assess a volcanic plume once eruption activity is reported. In a second step, a range of varying plume heights has been associated with the different ash variables within WRF-Chem, resulting in an assembly of different plume scenarios within one WRF-Chem model run. Once there is plume information available from ground or satellite observations, the forecaster has the option to select the corresponding ash variable that best matches the observations. In addition we added an automatic domain generation tool to create near real time WRF-Chem model runs anywhere on the globe by reducing computing expenses at the same time.

  13. TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

    Energy Technology Data Exchange (ETDEWEB)

    Annette C. Rohr; Petros Koutrakis; John Godleski

    2011-03-31

    Determining the health impacts of different sources and components of fine particulate matter (PM2.5) is an important scientific goal, because PM is a complex mixture of both inorganic and organic constituents that likely differ in their potential to cause adverse health outcomes. The TERESA (Toxicological Evaluation of Realistic Emissions of Source Aerosols) study focused on two PM sources - coal-fired power plants and mobile sources - and sought to investigate the toxicological effects of exposure to realistic emissions from these sources. The DOE-EPRI Cooperative Agreement covered the performance and analysis of field experiments at three power plants. The mobile source component consisted of experiments conducted at a traffic tunnel in Boston; these activities were funded through the Harvard-EPA Particulate Matter Research Center and will be reported separately in the peer-reviewed literature. TERESA attempted to delineate health effects of primary particles, secondary (aged) particles, and mixtures of these with common atmospheric constituents. The study involved withdrawal of emissions directly from power plant stacks, followed by aging and atmospheric transformation of emissions in a mobile laboratory in a manner that simulated downwind power plant plume processing. Secondary organic aerosol (SOA) derived from the biogenic volatile organic compound {alpha}-pinene was added in some experiments, and in others ammonia was added to neutralize strong acidity. Specifically, four scenarios were studied at each plant: primary particles (P); secondary (oxidized) particles (PO); oxidized particles + secondary organic aerosol (SOA) (POS); and oxidized and neutralized particles + SOA (PONS). Extensive exposure characterization was carried out, including gas-phase and particulate species. Male Sprague Dawley rats were exposed for 6 hours to filtered air or different atmospheric mixtures. Toxicological endpoints included (1) breathing pattern; (2) bronchoalveolar lavage

  14. Assimilation of Polder aerosol optical thickness into LMD2-Inca model in order to study aerosol-climate interactions; Etude des interactions entre aerosols et climat: assimilation des observations spatiales de Polder dans LMDz-Inca

    Energy Technology Data Exchange (ETDEWEB)

    Generoso, S.

    2004-12-15

    Aerosols influence the Earth radiative budget both through their direct (scattering and absorption of solar radiation) and indirect (impacts on cloud microphysics) effects. The anthropogenic perturbation due to aerosol emissions is of the same order of magnitude than the one due to greenhouse gases, but less well known. To improve our knowledge, we need to better know aerosol spatial and temporal distributions. Indeed, aerosol modeling still suffers from large uncertainties in sources and transport, while satellite observations are incomplete (no detection in the presence of clouds, no information on the vertical distribution or on the chemical nature). Moreover, field campaigns are localized in space and time. This study aims to reduce uncertainties in aerosol distributions, developing assimilation of satellite data into a chemical transport model. The basic idea is to combine information obtained from spatial observation (optical thickness) and modeling studies (aerosol types, vertical distribution). In this study, we assimilate data from the POLDER space-borne instrument into the LMDz-INCA model. The results show the advantage of merging information from different sources. In many regions, the method reduces uncertainties on aerosol distribution (reduction of RMS error). An application of the method to the study of aerosol impact on cloud microphysics is shown. (author)

  15. Origins of aerosol chlorine during winter over north central Colorado, USA

    Science.gov (United States)

    Jordan, C. E.; Pszenny, A. A. P.; Keene, W. C.; Cooper, O. R.; Deegan, B.; Maben, J.; Routhier, M.; Sander, R.; Young, A. H.

    2015-01-01

    The Nitrogen, Aerosol Composition, and Halogens on a Tall Tower campaign (February-March 2011) near Boulder, Colorado, investigated nighttime ClNO2 production and processing. Virtually all particulate Cl was in the form of ionic Cl-. The size distributions of Cl- and Na+ were similar, with most of the mass in the supermicrometer size fraction, suggesting primary sources for both. Median Cl- concentrations were about half those of Na+ and Ca2+ for particle diameters centered at 1.4 and 2.5 µm. To investigate potential sources of Na+ and Cl-, four cases were studied that featured the prevalence of Na+ and Cl- and different transport pathways based on FLEXible PARTicle dispersion model (FLEXPART) retroplumes. Estimates of supermicrometer Na+ particle lifetime against deposition indicate that long-range transport of marine aerosols could account for the observed Na+. However, measured molar ratios of Ca2+ to Na+ (0.143-0.588) compared to seawater (0.022) indicate significant contributions from crustal sources to the supermicrometer aerosol composition during these four case studies. Further, low molar ratios of Mg2+ to Na+ (0.007-0.098) relative to seawater (0.114) suggest that some of the Na+, and presumably associated Cl-, originated from non-sea-salt sources. The heterogeneous chemical composition of saline soils throughout the western U.S., along with the nonlinearity of wind-driven soil deflation as a function of various surface soil properties, precludes a quantitative apportionment of soil, marine, and anthropogenic sources to the observed coarse-fraction aerosol. Nonetheless, results suggest that deflation of saline soils was a potentially important source of particulate Cl- that sustained atmospheric ClNO2 production and associated impacts on oxidation processes over northern Colorado.

  16. Chemical composition and sources of atmospheric aerosols at Djougou (Benin)

    Science.gov (United States)

    Ouafo-Leumbe, Marie-Roumy; Galy-Lacaux, Corinne; Liousse, Catherine; Pont, Veronique; Akpo, Aristide; Doumbia, Thierno; Gardrat, Eric; Zouiten, Cyril; Sigha-Nkamdjou, Luc; Ekodeck, Georges Emmanuel

    2017-06-01

    In the framework of the INDAAF (International Network to study Deposition and Atmospheric chemistry in AFrica) program, atmospheric aerosols were collected in PM2.5 and PM10 size fractions at Djougou, Benin, in the West Africa, from November, 2005 to October, 2009. Particulate carbon, ionic species, and trace metals were analyzed. Weekly PM2.5 and PM10 total mass concentrations varied between 0.7 and 47.3 µg m-3 and 1.4-148.3 µg m-3, respectively. We grouped the aerosol chemical compounds into four classes: dust, particulate organic matter (POM), elemental carbon (EC), and ions. We studied the annual variation of each class to determine their contribution in the total aerosol mass concentration and finally to investigate their potential emission sources. On an annual basis, the species presented a well-marked seasonality, with the peak of mass concentration for both sizes registered in dry season, 67 ± 2 to 86 ± 9 versus 14 ± 9 to 34 ± 5% in wet season. These values emphasized the seasonality of the emissions and the relative weak interannual standard deviation indicates the low variability of the seasonality. At the seasonal scale, major contributions to the aerosol chemistry in the dry season are: dust (26-59%), POM (30-59%), EC (5-9%), and ions (3-5%), suggesting a predominance of Sahelian and Saharan dust emissions and biomass burning source in this season. In the wet season, POM is predominant, followed by dust, EC, and ions. These results point out the contribution of surrounded biofuel combustion used for cooking and biogenic emissions during the wet season.

  17. A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2008-02-01

    Full Text Available With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic matter in the marine aerosol is prescribed for each aerosol mode with varying organic mass and mixing state, and with a geographical distribution and seasonality similar to the oceanic emission of dimethyl sulfide. Measurements of aerosol mass, aerosol chemical composition and cloud drop effective radius are used to assess the representativity of the model initializations. Good agreement with the measurements is obtained when organic matter is added to the Aitken, accumulation and coarse modes simultaneously. Representing marine organics in the model leads to higher cloud drop number concentrations and thus smaller cloud drop effective radii, and this improves the agreement with measurements. The mixing state of the organics and the other aerosol matter, i.e. internal or external depending on the formation process of aerosol organics, is an important factor for this. We estimate that globally about 75 Tg C yr−1 of organic matter from marine origin enters the aerosol phase, with comparable contributions from primary emissions and secondary organic aerosol formation.

  18. Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

    Science.gov (United States)

    Zhang, Xinghua; Xu, Jianzhong; Kang, Shichang; Liu, Yanmei; Zhang, Qi

    2018-04-01

    An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m-3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (˜ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

  19. Aerosols at the poles: an AeroCom Phase II multi-model evaluation

    Directory of Open Access Journals (Sweden)

    M. Sand

    2017-10-01

    Full Text Available Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC from fossil fuel and biomass burning, sulfate, organic aerosols (OAs, dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs, we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt and spring (dust, whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N. The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE associated with BC and OA from fossil fuel and biofuel (FF, sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m−2, dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity

  20. Particle characterization at rural, suburban and urban aerosol sampling sites in Hungary

    International Nuclear Information System (INIS)

    Borbely-Kiss, I.; Koltay, E.; Szabo, G.; Meszaros, E.; Molnar, A.; Bozo, L.

    1994-01-01

    The study of atmospheric aerosols originating from natural and anthropogenic processes is of basic importance for a detailed understanding of the physics and chemistry of the atmosphere. Particle Induced X-ray Emission (PIXE) technique has been used by the authors for studying regularly the elemental composition of rural, suburban, and urban aerosols collected at six sampling sites in Hungary. Observed data presented in terms of concentrations and regional signature values and evaluated wind sector partition and in transport modelling revealed the natural/anthropogenic contribution to the moderate air pollution here. Dry deposition velocities have been deduced for elements V, Cr, Mn, Co, Ni, Cu, Zn, Cd, and Pb. Model calculations based on annual emission data and observed elemental concentrations resulted in total dry and wet deposition masses of the above elements to the territory of the country. At the same time, deduced budget data for the emission and deposition of the constituents indicated whether the country represents a net source or a sink for the above mentioned elements in the regional aerosol transport between neighbouring countries. Evidences have been found for intrusion events of Saharan aerosol to the atmosphere of Hungary. Part of the data collected recently will be evaluated in the frame-work of an international co-ordinated research programme. (author)

  1. Research Spotlight: Satellites monitor air pollutant emissions in China

    Science.gov (United States)

    Tretkoff, Ernie

    A new satellite study verifies that Chinese emission control efforts did reduce power plant emissions of sulfur dioxide (SO2), a harmful gas that causes acid rain and can form sulfate aerosols; these aerosols play an important role in the climate system by affecting clouds and precipitation patterns and altering the amount of sunlight that is reflected away from Earth.

  2. Remote Sensing of Salinity: The Dielectric Constant of Sea Water

    Science.gov (United States)

    LeVine, David M.; Lang, R.; Utku, C.; Tarkocin, Y.

    2011-01-01

    Global monitoring of sea surface salinity from space requires an accurate model for the dielectric constant of sea water as a function of salinity and temperature to characterize the emissivity of the surface. Measurements are being made at 1.413 GHz, the center frequency of the Aquarius radiometers, using a resonant cavity and the perturbation method. The cavity is operated in a transmission mode and immersed in a liquid bath to control temperature. Multiple measurements are made at each temperature and salinity. Error budgets indicate a relative accuracy for both real and imaginary parts of the dielectric constant of about 1%.

  3. Simultaneous PIXE and PIGE analyses of aerosol samples collected in urban areas

    International Nuclear Information System (INIS)

    Boni, C.; Caruso, E.; Cereda, E.; Marcazzan, G.M.; Redaelli, P.; Bacci, P.

    1988-01-01

    The paper concerns the simultaneous PIXE (Particle Induced X-ray Emission) and PIGE (Proton Induced Gamma-ray Emission) analyses of aerosol samples collected in urban areas. The results show that PIGE can detect Li, F, Na, Al, and Si in fly ashes and F, Na, Al and Si in atmospheric aerosol. The PIXE-PIGE technique has also been applied to 80 samples of atmospheric particular matter collected above Milan during the winter and summer months of 1986/7, and the average values of concentrations and enrichment factors are given for the detected elements. (U.K.)

  4. Distributions and climate effects of atmospheric aerosols from the preindustrial era to 2100 along Representative Concentration Pathways (RCPs simulated using the global aerosol model SPRINTARS

    Directory of Open Access Journals (Sweden)

    T. Takemura

    2012-12-01

    Full Text Available Global distributions and associated climate effects of atmospheric aerosols were simulated using a global aerosol climate model, SPRINTARS, from 1850 to the present day and projected forward to 2100. Aerosol emission inventories used by the Coupled Model Intercomparison Project Phase 5 (CMIP5 were applied to this study. Scenarios based on the Representative Concentration Pathways (RCPs were used for the future projection. Aerosol loading in the atmosphere has already peaked and is now reducing in Europe and North America. However, in Asia where rapid economic growth is ongoing, aerosol loading is estimated to reach a maximum in the first half of this century. Atmospheric aerosols originating from the burning of biomass have maintained high loadings throughout the 21st century in Africa, according to the RCPs. Evolution of the adjusted forcing by direct and indirect aerosol effects over time generally correspond to the aerosol loading. The probable future pathways of global mean forcing differ based on the aerosol direct effect for different RCPs. Because aerosol forcing will be close to the preindustrial level by the end of the 21st century for all RCPs despite the continuous increases in greenhouse gases, global warming will be accelerated with reduced aerosol negative forcing.

  5. Effects of aerosol/cloud interactions on the global radiation budget

    International Nuclear Information System (INIS)

    Chuang, C.C.; Penner, J.E.

    1994-01-01

    Aerosols may modify the microphysics of clouds by acting as cloud condensation nuclei (CCN), thereby enhancing the cloud reflectivity. Aerosols may also alter precipitation development by affecting the mean droplet size, thereby influencing cloud lifetimes and modifying the hydrological cycle. Clouds have a major effect on climate, but aerosol/cloud interactions have not been accounted for in past climate model simulations. However, the worldwide steady rise of global pollutants and emissions makes it imperative to investigate how atmospheric aerosols affect clouds and the global radiation budget. In this paper, the authors examine the relationship between aerosol and cloud drop size distributions by using a detailed micro-physical model. They parameterize the cloud nucleation process in terms of local aerosol characteristics and updraft velocity for use in a coupled climate/chemistry model to predict the magnitude of aerosol cloud forcing. Their simulations indicate that aerosol/cloud interactions may result in important increases in reflected solar radiation, which would mask locally the radiative forcing from increased greenhouse gases. This work is aimed at improving the assessment of the effects of anthropogenic aerosols on cloud optical properties and the global radiation budget

  6. Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2011-12-01

    Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O3, NOx and NOy concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

  7. Geochemical, Sulfur Isotopic Characteristics and Source Contributions of Size-Aggregated Aerosols Collected in Baring Head, New Zealand.

    Science.gov (United States)

    Li, J.; Michalski, G. M.; Davy, P.; Harvey, M.; Wilkins, B. P.; Katzman, T. L.

    2017-12-01

    Sulfate aerosols are critical to the climate, human health, and the hydrological cycle in the atmosphere, yet the sources of sulfate in aerosols are not completely understood. In this work, we evaluated the sources of sulfate in size-aggregated aerosols from the Southern Pacific Ocean and the land of New Zealand using geochemical and isotopic analyses. Aerosols were collected at Baring Head, New Zealand between 6/30/15 to 8/4/16 using two collectors, one only collects Southern Pacific Ocean derived aerosols (open-ocean collector), the other collects aerosols from both the ocean and the land (all-direction collector). Each collector is equipped with two filters to sample size-aggregated aerosols (fine aerosols: NSS-SO42-, 70%), while coarse aerosols are dominated by sea-salt sulfate. However, some NSS-SO42- was also observed in coarse aerosols collected in summer, suggesting the presence of accumulation mode NSS-SO42- aerosols, which is possibly due to high summer biogenic DMS flux. The sources of sulfur in NSS-SO42- could be further determined by their d34S values. DMS emission is likely the sole sulfur source in the open-ocean collector as it shows constant DMS-like d34S signatures (15-18‰) throughout the year. Meanwhile, the d34S of NSS-SO42- in the all-direction collector display a seasonal trend: summer time d34S values are higher and DMS-like (15-18‰), indicating DMS emission is the dominant sulfur source; winter time d34S values are lower ( 6-12‰), therefore the sulfur is likely sourced from both DMS emission and terrestrial S input with low d34S values, such as volcanic activities, fossil fuel and wood burning.

  8. Regional radiative impacts of mixed dust and carbonaceous aerosols over West Africa

    Science.gov (United States)

    Malavelle, Florent; Pont, Véronique; Solmon, Fabien; Mallet, Marc; Léon, Jean-François; Liousse, Catherine; Johnson, Ben

    2010-05-01

    Africa is a major source of aerosols at global scale. Two types of aerosols dominate the regional background: biomass burning aerosols as results of combustion of the vegetation and mineral dust aerosols related to erosion of arid soils by wind. These important burdens of aerosols are known to have each one a strong impact on the regional radiative budget. Whereas recent modelling efforts show significant impacts at climatic timescale on West African Monsoon due to the radiative effects of dust aerosols (see Solmon et al 2008 in GRL and references therein), biomass burning radiative effects in this region stand still poorly documented. What about West Africa, during the dry season (december-february) when both biomass burning and dust aerosols are encountered in the atmospheric background ? In that frame, we use ICTP Regional Climate Model versions 3 in order to estimate the radiative forcing due to the external mixing of mineral dust and carbonaceous aerosols from biomass burning, BioFuel and Fossil Fuel combustion during the dry season. Emissions of biomass burning aerosols are taken from new inventories based on SPOT vegetation burnt area products. Optical properties of carboneaceous aerosols are updated thanks to chemical sampling at Djougou during AMMA SOP-0. This presentation focuses on the model efficiency to correctly reproduce the main features concerning aerosols observed during AMMA-SOP0/DABEX field campaigns. It refers to (i) a strong stratification of dust and smoke layers, and (ii) a marked seasonal cycle of aerosol mixture optical properties. Those features are key parameters for modelling the direct and semi direct effects of aerosols over West Africa. Results of simulations indicate that the particular low value of single scattering albedo (SSA) for biomass burning aerosols (~0.81 at 550nm) involves important diabatic heating in the atmosphere. Values of aerosol heating rates are estimated and compared with aircraft measurement from DABEX

  9. Identification of secondary aerosol precursors emitted by an aircraft turbofan

    Science.gov (United States)

    Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

    2018-05-01

    Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

  10. Characterization of aerosols produced by surgical procedures

    Energy Technology Data Exchange (ETDEWEB)

    Yeh, H.C.; Muggenburg, B.A.; Lundgren, D.L.; Guilmette, R.A.; Snipes, M.B.; Jones, R.K. [Inhalation Toxicology Research Institute, Albuquerque, NM (United States); Turner, R.S. [Lovelace Health Systems, Albuquerque, NM (United States)

    1994-07-01

    In many surgeries, especially orthopedic procedures, power tools such as saws and drills are used. These tools may produce aerosolized blood and other biological material from bone and soft tissues. Surgical lasers and electrocautery tools can also produce aerosols when tissues are vaporized and condensed. Studies have been reported in the literature concerning production of aerosols during surgery, and some of these aerosols may contain infectious material. Garden et al. (1988) reported the presence of papilloma virus DNA in the fumes produced from laser surgery, but the infectivity of the aerosol was not assessed. Moon and Nininger (1989) measured the size distribution and production rate of emissions from laser surgery and found that particles were generally less than 0.5 {mu}m diameter. More recently there has been concern expressed over the production of aerosolized blood during surgical procedures that require power tools. In an in vitro study, the production of an aerosol containing the human immunodeficiency virus (HIV) was reported when power tools were used to cut tissues with blood infected with HIV. Another study measured the size distribution of blood aerosols produced by surgical power tools and found blood-containing particles in a number of size ranges. Health care workers are anxious and concerned about whether surgically produced aerosols are inspirable and can contain viable pathogens such as HIV. Other pathogens such as hepatitis B virus (HBV) are also of concern. The Occupational Safety and Health funded a project at the National Institute for Inhalation Toxicology Research Institute to assess the extent of aerosolization of blood and other tissues during surgical procedures. This document reports details of the experimental and sampling approach, methods, analyses, and results on potential production of blood-associated aerosols from surgical procedures in the laboratory and in the hospital surgical suite.

  11. An algorithm for hyperspectral remote sensing of aerosols: 2. Information content analysis for aerosol parameters and principal components of surface spectra

    Science.gov (United States)

    Hou, Weizhen; Wang, Jun; Xu, Xiaoguang; Reid, Jeffrey S.

    2017-05-01

    This paper describes the second part of a series of investigation to develop algorithms for simultaneous retrieval of aerosol parameters and surface reflectance from the future hyperspectral and geostationary satellite sensors such as Tropospheric Emissions: Monitoring of POllution (TEMPO). The information content in these hyperspectral measurements is analyzed for 6 principal components (PCs) of surface spectra and a total of 14 aerosol parameters that describe the columnar aerosol volume Vtotal, fine-mode aerosol volume fraction, and the size distribution and wavelength-dependent index of refraction in both coarse and fine mode aerosols. Forward simulations of atmospheric radiative transfer are conducted for 5 surface types (green vegetation, bare soil, rangeland, concrete and mixed surface case) and a wide range of aerosol mixtures. It is shown that the PCs of surface spectra in the atmospheric window channel could be derived from the top-of-the-atmosphere reflectance in the conditions of low aerosol optical depth (AOD ≤ 0.2 at 550 nm), with a relative error of 1%. With degree freedom for signal analysis and the sequential forward selection method, the common bands for different aerosol mixture types and surface types can be selected for aerosol retrieval. The first 20% of our selected bands accounts for more than 90% of information content for aerosols, and only 4 PCs are needed to reconstruct surface reflectance. However, the information content in these common bands from each TEMPO individual observation is insufficient for the simultaneous retrieval of surface's PC weight coefficients and multiple aerosol parameters (other than Vtotal). In contrast, with multiple observations for the same location from TEMPO in multiple consecutive days, 1-3 additional aerosol parameters could be retrieved. Consequently, a self-adjustable aerosol retrieval algorithm to account for surface types, AOD conditions, and multiple-consecutive observations is recommended to derive

  12. The composition and variability of atmospheric aerosol over Southeast Asia during 2008

    Directory of Open Access Journals (Sweden)

    W. Trivitayanurak

    2012-01-01

    the model has the least skill at reproducing the data, where the model has a negative bias of 76% and only captures 14% of the observed variability. This model performance reflects the small-scale island-marine environment and the mix of aerosol species, with the model showing more skill at reproducing observed AOD over larger continental regions such as China where AOD is dominated by one aerosol type. The model shows that AOD over Borneo is approximately evenly split between organic and sulphate aerosol with sea salt representing 10–20% during May–September; we find a similar breakdown over continental Southeast Asia but with less sea salt aerosol and more dust aerosol. In contrast, East China AOD is determined mainly by sulphate aerosol and a seasonal source of dust aerosol, as expected. Realistic sensitivity runs, designed to test our underlying assumptions about emissions and chemistry over Borneo, show that model AOD is most sensitive to isoprene emissions and organic gas-phase partitioning but all fail to improve significantly upon the control model calculation. This emphasises the multi-faceted dimension of the problem and the need for concurrent and coordinated development of BVOC emissions, and BVOC chemistry and organic aerosol formation mechanisms.

  13. The composition and variability of atmospheric aerosol over Southeast Asia during 2008

    Science.gov (United States)

    Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

    2012-01-01

    has the least skill at reproducing the data, where the model has a negative bias of 76% and only captures 14% of the observed variability. This model performance reflects the small-scale island-marine environment and the mix of aerosol species, with the model showing more skill at reproducing observed AOD over larger continental regions such as China where AOD is dominated by one aerosol type. The model shows that AOD over Borneo is approximately evenly split between organic and sulphate aerosol with sea salt representing 10-20% during May-September; we find a similar breakdown over continental Southeast Asia but with less sea salt aerosol and more dust aerosol. In contrast, East China AOD is determined mainly by sulphate aerosol and a seasonal source of dust aerosol, as expected. Realistic sensitivity runs, designed to test our underlying assumptions about emissions and chemistry over Borneo, show that model AOD is most sensitive to isoprene emissions and organic gas-phase partitioning but all fail to improve significantly upon the control model calculation. This emphasises the multi-faceted dimension of the problem and the need for concurrent and coordinated development of BVOC emissions, and BVOC chemistry and organic aerosol formation mechanisms.

  14. New aerosol particles formation in the Sao Paulo Metropolitan Area

    Science.gov (United States)

    Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

    2016-04-01

    The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

  15. Aerosol measurements over Southern Africa using LIDAR, satellite and sun-photometer

    CSIR Research Space (South Africa)

    Sivakumar, V

    2009-08-01

    Full Text Available .csir.co.za Dust Sea Salt Giant nuclei Natural Particles Chemical chemical condensables : SOA, H2SO4, HNO3 … nucleation condensation Aerosol Formation and processes Health Aerosols Solar Radiation Clouds Slide 3 © CSIR 2008 www....csir.co.za Emissions from Industries, vechicle and urban Volatile Components SO2, NOx, NH3, VOC Transformation Humidity and deposition of particules Primary Aerosols, BC, OC, Marine Salts, Natural resources 0 - 16 k m U p t o 50 k m 26 – 29...

  16. Factors Affecting Aerosol Radiative Forcing from Both Production-based and Consumption-based View

    Science.gov (United States)

    Wang, J.; Lin, J.; Ni, R.

    2017-12-01

    Aerosol radiative forcing (RF) is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. This problem becomes more complicated when taking into account the role of international trade, which means reallocated aerosol RF due to separation of regions producing goods and emissions and regions consuming those goods. Here we analyze major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA) and black carbon (BC), extending the work of Lin et al. (2016, Nature Geoscience). We contrast five factors determining production-based (RFp, due to a region's production of goods) and consumption-based (RFc, due to a region's consumption) forcing by 11 major regions, including population size, per capita output, emission intensity (emission per output), chemical efficiency (mass per unit emission) and radiative efficiency (RF per unit mass). Comparing across the 11 regions, East Asia produces the strongest RFp and RFc of SIOA and BC and the second largest RFp and RFc of POA primarily due to its high emission intensity. Although Middle East and North Africa has low emissions, its RFp is strengthened by its largest chemical efficiency for POA and BC and second largest chemical efficiency for SIOA. However, RFp of South-East Asia and Pacific is greatly weakened by its lowest chemical efficiency. Economic trade means that net importers (Western Europe, North America and Pacific OECD) have higher RFc than RFp by 50-100%. And such forcing difference is mainly due to the high emission intensity of the exporters supplying these regions. For North America, SIOA's RFc is 50% stronger than RFp, for that emission intensity of SIOA is 5.2 times in East Asia and 2.5 times in Latin America and Caribbean compared with that in North America, and the chemical efficiency in the top four exporters are

  17. Atmospheric aerosols in Rome, Italy: sources, dynamics and spatial variations during two seasons

    Directory of Open Access Journals (Sweden)

    C. Struckmeier

    2016-12-01

    Full Text Available Investigations on atmospheric aerosols and their sources were carried out in October/November 2013 and May/June 2014 consecutively in a suburban area of Rome (Tor Vergata and in central Rome (near St Peter's Basilica. During both years a Saharan dust advection event temporarily increased PM10 concentrations at ground level by about 12–17 µg m−3. Generally, in October/November the ambient aerosol was more strongly influenced by primary emissions, whereas higher relative contributions of secondary particles (sulfate, aged organic aerosol were found in May/June. Absolute concentrations of anthropogenic emission tracers (e.g. NOx, CO2, particulate polycyclic aromatic hydrocarbons, traffic-related organic aerosol were generally higher at the urban location. Positive matrix factorization was applied to the PM1 organic aerosol (OA fraction of aerosol mass spectrometer (HR-ToF-AMS data to identify different sources of primary OA (POA: traffic, cooking, biomass burning and (local cigarette smoking. While biomass burning OA was only found at the suburban site, where it accounted for the major fraction of POA (18–24 % of total OA, traffic and cooking were more dominant sources at the urban site. A particle type associated with cigarette smoke emissions, which is associated with a potential characteristic marker peak (m∕z 84, C5H10N+, a nicotine fragment in the mass spectrum, was only found in central Rome, where it was emitted in close vicinity to the measurement location. Regarding secondary OA, in October/November, only a very aged, regionally advected oxygenated OA was found, which contributed 42–53 % to the total OA. In May/June total oxygenated OA accounted for 56–76 % of the OA. Here a fraction (18–26 % of total OA of a fresher, less oxygenated OA of more local origin was also observed. New particle formation events were identified from measured particle number concentrations and size distributions in May/June 2014 at

  18. NOAA's National Air Quality Prediction and Development of Aerosol and Atmospheric Composition Prediction Components for NGGPS

    Science.gov (United States)

    Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.

    2017-12-01

    NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.

  19. Aerosol sources and their contribution to the chemical composition of aerosols in the Eastern Mediterranean Sea during summertime

    Directory of Open Access Journals (Sweden)

    J. Sciare

    2003-01-01

    Full Text Available A detailed study on the temporal variability of compounds important in controlling aerosol chemical composition was performed during a one-month experiment conducted during summer 2000 at a background site on Crete, in the Eastern Mediterranean Sea. Contribution of different aerosol sources in the Eastern Mediterranean Basin could be investigated at this location since the site is influenced by a wide range of air masses originating mainly in Europe and Africa. Chemical apportionment was performed for various air mass origins and showed a strong impact of anthropogenic emissions in the Turkey and Central Europe sectors, with black carbon (BC and non-sea-salt sulfate (nss-SO4 concentrations higher than observed in the Eastern and Western Europe sectors. High levels of non-sea-salt calcium (nss-Ca were associated with air masses from Africa but also from Central Turkey. Evidence was found that BC calculation based on light absorbance during dust events was biased. This quality-controlled high temporal resolution dataset allowed to investigate in detail the source-receptor relationships responsible for the levels of BC, nss-SO4 and sulfur dioxide (SO2, observed in Crete. Among the results obtained from this model, the major contribution of Turkey and Central Europe was confirmed in terms of anthropogenic emissions. Comparisons with remote optical properties obtained from Satellite observations (SEAWIFS north of Crete indicates that our ground based aerosol characterization was suitable for describing aerosol properties in the atmospheric column for most of the time during the campaign.

  20. Aerosol emissions from forest and grassland burnings in the southern amazon basin and central Brazil

    Science.gov (United States)

    Leslie, Alistair C. D.

    1981-03-01

    Forest and grassland clearing by means of prescribed fires in tropical areas of the world may be responsible for large inputs of fine particulates to the global atmosphere besides being a major source of trace gases. The major continents on which extensive biomass burning takes place are Africa and South America. Such agricultural practices of burning have been employed throughout man's existence, but the importance and significance of such burning relative to anthropogenic industrial emissions to the atmosphere has not until extremely recently been seriously studied. In August-September 1979 project "Brushfire 1979" took place based in Brasília, Brazil. The Air Quality Division of the National Center for Atmospheric Research made ground level and aircraft measurements of trace gases (e.g. CO 2, CO, CH 4, N 2O, H 2, CH 3Cl, COS, NO, NO 2, O 3) and Florida State University sampled ground level aerosol emissions from grass and forest burnings. Aerosols were sampled using plastic 7-stage single orifice cascade impactors and FSU type linear and circular "streakers". Long term sampling was made of regional background for total particulates (8 μmad). Short term sampling within grass or forest fires was made using impactors incorporated into portable kits containing 4 miniature 12-18 V dc Brailsford pumps and a disposable dry cell power pack. Sampling times of 5-15 min were found optimal under these conditions. Grass fires were sampled in the savannah area northeast of Brasília and forest fires in the state of Mato Grosso on the southern edge of the dryland forest of the Amazon basin. Residual ash samples were collected. All of the samples were analyzed at Florida State University using PIXE for 15-20 elements including Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Pb and Sr. Computer reduction of the X-ray spectra was made using the "HEXB" program. One of the prominent features found was the large flux of small particles (<2.0 μm) from both fire

  1. Influence of aerosol particles, clouds, and condensation trails on the climate in Bavaria

    International Nuclear Information System (INIS)

    Wiegner, M.

    1994-01-01

    Human interventions in the climate system occur mainly through the emission of trace gases and aerosol particles. Emissions of aerosol particles can also change the properties of clouds. Climate model calculations have shown that an increase in trace gas concentrations causes the lower atmosphere to warm. According to numerical studies performed during the past few years, anthropogenic aerosol sources can have a cooling effect which is of the same order as the warming caused by greenhouse gases. However, due to their differing time constants and spatial characteristics the two effects are unlikely to neutralise each other over extended regions for any length of time. The currently available models with their very coarse spatial resolution are not suitable for making climatological predictions for Bavaria on the basis of cloud or aerosol properties. What can be done at present is to formulate warnings and propose measures for reducing environmental hazards and conserving our natural surroundings as far as possible. (orig.) [de

  2. Regional emission metrics for short-lived climate forcers from multiple models

    Directory of Open Access Journals (Sweden)

    B. Aamaas

    2016-06-01

    Full Text Available For short-lived climate forcers (SLCFs, the impact of emissions depends on where and when the emissions take place. Comprehensive new calculations of various emission metrics for SLCFs are presented based on radiative forcing (RF values calculated in four different (chemical-transport or coupled chemistry–climate models. We distinguish between emissions during summer (May–October and winter (November–April for emissions in Europe and East Asia, as well as from the global shipping sector and global emissions. The species included in this study are aerosols and aerosol precursors (BC, OC, SO2, NH3, as well as ozone precursors (NOx, CO, VOCs, which also influence aerosols to a lesser degree. Emission metrics for global climate responses of these emissions, as well as for CH4, have been calculated using global warming potential (GWP and global temperature change potential (GTP, based on dedicated RF simulations by four global models. The emission metrics include indirect cloud effects of aerosols and the semi-direct forcing for BC. In addition to the standard emission metrics for pulse and sustained emissions, we have also calculated a new emission metric designed for an emission profile consisting of a ramping period of 15 years followed by sustained emissions, which is more appropriate for a gradual implementation of mitigation policies.For the aerosols, the emission metric values are larger in magnitude for emissions in Europe than East Asia and for summer than winter. A variation is also observed for the ozone precursors, with largest values for emissions in East Asia and winter for CO and in Europe and summer for VOCs. In general, the variations between the emission metrics derived from different models are larger than the variations between regions and seasons, but the regional and seasonal variations for the best estimate also hold for most of the models individually. Further, the estimated climate impact of an illustrative mitigation

  3. A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

    Science.gov (United States)

    Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

    2017-08-01

    To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions

  4. Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

    Science.gov (United States)

    Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

    2018-03-01

    Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

  5. Characteristics of particulate matter emissions from toy cars with electric motors.

    Science.gov (United States)

    Wang, Xiaofei; Williams, Brent J; Biswas, Pratim

    2015-04-01

    Aerosol emissions from toy cars with electric motors were characterized. Particle emission rates from the toy cars, as high as 7.47×10(7) particles/s, were measured. This emission rate is lower than other indoor sources such as smoking and cooking. The particles emitted from toy cars are generated from spark discharges inside the electric motors that power the toy cars. Size distribution measurements indicated that most particles were below 100 nm in diameter. Copper was the dominant inorganic species in these particles. By deploying aerosol mass spectrometers, high concentrations of particulate organic matter were also detected and characterized in detail. Several organic compounds were identified using a thermal desorption aerosol gas chromatography. The mass size distribution of particulate organic matter was bimodal. The formation mechanism of particulate organic matter from toy cars was elucidated. A possible new source of indoor air pollution, particles from electric motors in toy cars, was identified. This study characterized aerosol emissions from toy cars in detail. Most of these particles have a diameter less than 100 nm. Copper and some organics are the major components of these particles. Conditions that minimize these emissions were determined.

  6. An investigation of the sub-grid variability of trace gases and aerosols for global climate modeling

    Directory of Open Access Journals (Sweden)

    Y. Qian

    2010-07-01

    Full Text Available One fundamental property and limitation of grid based models is their inability to identify spatial details smaller than the grid cell size. While decades of work have gone into developing sub-grid treatments for clouds and land surface processes in climate models, the quantitative understanding of sub-grid processes and variability for aerosols and their precursors is much poorer. In this study, WRF-Chem is used to simulate the trace gases and aerosols over central Mexico during the 2006 MILAGRO field campaign, with multiple spatial resolutions and emission/terrain scenarios. Our analysis focuses on quantifying the sub-grid variability (SGV of trace gases and aerosols within a typical global climate model grid cell, i.e. 75×75 km2.

    Our results suggest that a simulation with 3-km horizontal grid spacing adequately reproduces the overall transport and mixing of trace gases and aerosols downwind of Mexico City, while 75-km horizontal grid spacing is insufficient to represent local emission and terrain-induced flows along the mountain ridge, subsequently affecting the transport and mixing of plumes from nearby sources. Therefore, the coarse model grid cell average may not correctly represent aerosol properties measured over polluted areas. Probability density functions (PDFs for trace gases and aerosols show that secondary trace gases and aerosols, such as O3, sulfate, ammonium, and nitrate, are more likely to have a relatively uniform probability distribution (i.e. smaller SGV over a narrow range of concentration values. Mostly inert and long-lived trace gases and aerosols, such as CO and BC, are more likely to have broad and skewed distributions (i.e. larger SGV over polluted regions. Over remote areas, all trace gases and aerosols are more uniformly distributed compared to polluted areas. Both CO and O3 SGV vertical profiles are nearly constant within the PBL during daytime, indicating that trace gases

  7. Submicron aerosol distributions and CCN activity measured in and around the Korean Peninsula during KORUS-AQ

    Science.gov (United States)

    Park, M.; Kim, N.; Yum, S. S.; Thornhill, K. L., II; Anderson, B. E.; Kim, D. S.; Kim, H. J.; Jeon, H. E.; Park, Y. S.; Lee, S. B.

    2017-12-01

    KORUS-AQ is a field campaign aimed at investigating formation of ozone and aerosol and interactions between chemistry, transport and various sources in the Korean Peninsula which is the region affected both by long-range transport and local emission. Aerosol number concentration and size distribution, and CCN number concentration were measured on board the NASA DC-8 research aircraft and at a ground site at Olympic Park in Seoul, capital city of Korea during the KORUS-AQ campaign (May 2nd to June 10th, 2017). There were 20 flights during the KORUS-AQ campaign and total flight time was about 150 hours. CCN counter (CCNC) on the airborne platform was operated at the fixed internal supersaturation of 0.6% and CCNC at the ground site was operated at five different supersaturations (0.2%, 0.4%, 0.6%, 0.8%, and 1.0%). Aerosol hygroscopic parameter κ was also estimated from CCN number concentration and aerosol size distribution. Airborne measurements showed a large spatio-temporal variation of aerosol number concentration and CCN activity in and around the Korean peninsula, and the ground measurements also showed a large temporal variation. The campaign period can be classified into long-range transport dominant cases, local emission dominant cases due to stagnant air mass, and others. Aerosol number concentration in the Korean Peninsula measured in stagnant air mass period was higher than those in long-range transport period, but CCN number concentration showed an opposite tendency. Both aerosol and CCN number concentrations over the Yellow Sea in local emission period were slightly higher than those in long-range transport period. Since CCN activity is different depending on time and space, our focus is on understanding how CCN activity and aerosol hygroscopicity vary with the source of aerosol. Comprehensive analysis results will be shown at the conference.

  8. Modeling of pollution aerosols in Ile-de-France

    International Nuclear Information System (INIS)

    Hodzic, A.

    2005-10-01

    The modeling of aerosols is a major stake in the understanding of the emission processes and evolution of particulates in the atmosphere. However, the parameterizations used in today's aerosol models still comprise many uncertainties. This work has been motivated by the need of better identifying the weaknesses of aerosols modeling tools and by the necessity of having new validation methods for a 3D evaluation of models. The studies have been carried out using the CHIMERE chemistry-transport model, which allows to simulate the concentrations and physico-chemical characteristics of pollution aerosols at the European scale and in Ile-de-France region. The validation approach used is based on the complementarity of the measurements performed on the ground by monitoring networks with those acquired during the ESQUIF campaign (study and simulation of air quality in Ile-de-France), with lidar and photometric measurements and with satellite observations. The comparison between the observations and the simulations has permitted to identify and reduce the modeling errors, and to characterize the aerosol properties in the vicinity of an urban area. (J.S.)

  9. Vapour pressure of ammonium chloride aerosol: Effect of temperature and humidity

    Science.gov (United States)

    Pio, Casimiro A.; Harrison, Roy M.

    The effect of relative humidity (RH) on the constant for dissociation of ammonium chloride into gaseous HCl and NH 3 has been estimated for different temperatures, using thermodynamic data. At RH over 75-85% the ammonium chloride aerosol exists in the liquid phase, with the dissociation constant two orders of magnitude lower at 98% RH than for solid aerosol at the same temperature. It is predicted that ammonium chloride aqueous aerosol forms predominantly in fogwater and cloud droplets, and in regions where local emissions of NH 3 are important.

  10. PIXE investigation of aerosol composition over the Zambian Copperbelt

    Science.gov (United States)

    Meter, S. L.; Formenti, P.; Piketh, S. J.; Annegarn, H. J.; Kneen, M. A.

    1999-04-01

    Atmospheric sulphate aerosol concentrations are of interest in climate change studies because of their negative climate forcing potential. Quantification of their forcing strength requires the compilation of global sulphur emission inventories to determine the magnitude of regional sources. We report on measurements of the ambient aerosol concentrations in proximity to a copper refinery in the central African Copperbelt, along the border of Zambia and the Democratic Republic of the Congo. This region is historically regarded as one of the largest African sources of sulphate aerosols. Sulphate is produced by oxidation in the atmosphere of SO 2 emitted during the pyrometallurgical processing of Cu-Co sulphide ores. Since the last quantification of sulphur emissions (late 1960s), there has been large-scale reduction in copper production and more frequent use of the leaching technique with negligible sulphur emissions. Samples were collected over four weeks, November-December 1996, at Kitwe, Zambia. A low volume two-stage time-resolving aerosol sampler (streaker) was used. Coarse and fine mode aerosols were separated at >2.5 and >10 μmad. Hourly elemental concentrations were determined by 3.2 MeV PIXE, and routinely yielded Si, S, K, Ca, Ti, Mn, Fe, Cu and Zn, above detection limits. Si, K, Ca and Fe (major crustal components) dominated the coarse elemental mass. In the fine stage, S and Si accounted for up to 80% of the measured mass, and S alone up to 60%. Time series analysis allowed the division of sulphur and crustal elements (Si, K, Ca, Fe) between (i) background concentrations representative of synoptic scale air masses; and (ii) contributions from local sources, i.e., copper smelter and re-suspended soil dust. Short duration episodes of S concentrations, up to 26 μg/m 3, were found simultaneously with enhanced Cu, Fe and Zn. Contributions from individual pyrometallurgic processes and the cobalt slag dump could be distinguished from the elemental signatures

  11. PIXE investigation of aerosol composition over the Zambian Copperbelt

    International Nuclear Information System (INIS)

    Meter, S.L.; Formenti, P.; Piketh, S.J.; Annegarn, H.J.; Kneen, M.A.

    1999-01-01

    Atmospheric sulphate aerosol concentrations are of interest in climate change studies because of their negative climate forcing potential. Quantification of their forcing strength requires the compilation of global sulphur emission inventories to determine the magnitude of regional sources. We report on measurements of the ambient aerosol concentrations in proximity to a copper refinery in the central African Copperbelt, along the border of Zambia and the Democratic Republic of the Congo. This region is historically regarded as one of the largest African sources of sulphate aerosols. Sulphate is produced by oxidation in the atmosphere of SO 2 emitted during the pyrometallurgical processing of Cu-Co sulphide ores. Since the last quantification of sulphur emissions (late 1960s), there has been large-scale reduction in copper production and more frequent use of the leaching technique with negligible sulphur emissions. Samples were collected over four weeks, November-December 1996, at Kitwe, Zambia. A low volume two-stage time-resolving aerosol sampler (streaker) was used. Coarse and fine mode aerosols were separated at >2.5 and >10 μmad. Hourly elemental concentrations were determined by 3.2 MeV PIXE, and routinely yielded Si, S, K, Ca, Ti, Mn, Fe, Cu and Zn, above detection limits. Si, K, Ca and Fe (major crustal components) dominated the coarse elemental mass. In the fine stage, S and Si accounted for up to 80% of the measured mass, and S alone up to 60%. Time series analysis allowed the division of sulphur and crustal elements (Si, K, Ca, Fe) between (i) background concentrations representative of synoptic scale air masses; and (ii) contributions from local sources, i.e., copper smelter and re-suspended soil dust. Short duration episodes of S concentrations, up to 26 μg/m 3 , were found simultaneously with enhanced Cu, Fe and Zn. Contributions from individual pyrometallurgic processes and the cobalt slag dump could be distinguished from the elemental signatures

  12. Organic aerosols and inorganic species from post-harvest agricultural-waste burning emissions over northern India: impact on mass absorption efficiency of elemental carbon.

    Science.gov (United States)

    Rajput, Prashant; Sarin, M M; Sharma, Deepti; Singh, Darshan

    2014-01-01

    Atmospheric PM2.5 (particulate matter with aerodynamic diameter of ≤ 2.5 μm), collected from a source region [Patiala: 30.2 °N; 76.3 °E; 250 m above mean sea level] of emissions from post-harvest agricultural-waste (paddy-residue) burning in the Indo-Gangetic Plain (IGP), North India, has been studied for its chemical composition and impact on regional atmospheric radiative forcing. On average, organic aerosol mass accounts for 63% of PM2.5, whereas the contribution of elemental carbon (EC) is ∼3.5%. Sulphate, nitrate and ammonium contribute up to ∼85% of the total water-soluble inorganic species (WSIS), which constitutes ∼23% of PM2.5. The potassium-to-organic carbon ratio from paddy-residue burning emissions (KBB(+)/OC: 0.05 ± 0.01) is quite similar to that reported from Amazonian and Savanna forest-fires; whereas non-sea-salt-sulphate-to-OC ratio (nss-SO4(2-)/OC: 0.21) and nss-SO4(2-)/EC ratio of 2.6 are significantly higher (by factor of 5 to 8). The mass absorption efficiency of EC (3.8 ± 1.3 m(2) g(-1)) shows significant decrease with a parallel increase in the concentrations of organic aerosols and scattering species (sulphate and nitrate). A cross plot of OC/EC and nss-SO4(2-)/EC ratios show distinct differences for post-harvest burning emissions from paddy-residue as compared to those from fossil-fuel combustion sources in south-east Asia.

  13. Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

    Energy Technology Data Exchange (ETDEWEB)

    Petäjä, T

    2013-12-01

    Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

  14. Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

    Science.gov (United States)

    Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

    2017-12-01

    The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

  15. Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

    Directory of Open Access Journals (Sweden)

    F. Freutel

    2013-01-01

    Full Text Available During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively. For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be

  16. Characterization of urban aerosol sources in Debrecen, Hungary

    International Nuclear Information System (INIS)

    Kertesz, Zs.; Szoboszlai, T.; Angyal, A.; Dobos, E.; Borbely-Kiss, I.

    2009-01-01

    Complete text of publication follows. Aerosol pollution represents significant health hazard in urban environments. Despite the fact that Debrecen has not a much stressed environment the city is highly exposed to aerosol pollution. In order to evaluate the impact of aerosol particles on health, the knowledge of the particle size distribution, chemical composition, sources, and their change in time and space is needed. This work presents a source apportionment study of fine (particles with aerodynamic diameter less than 2.5 μm) and coarse (particles with aerodynamic diameter between 2.5 and 10 μm) particulate matter in Debrecen by following the evolution of the elemental components with hourly time resolution. The variation of the elemental concentrations, their periodicity, correlation with other elements and meteorological parameters were studied on samples collected in different seasons. Aerosol sources were determined using the positive matrix factorization (PMF) method. Aerosol samples were collected in the garden of the ATOMKI with a 2-stage sequential streaker sampler manufactured by PIXE International, which collected the fine and coarse fraction separately with few hours' time resolution. Between October 2007 and January 2009 five 10-days long sampling campaigns were carried out. The elemental composition was determined by Particle Induced X-ray emission (PIXE) for Z ≥ 13, and the elemental carbon (BC) content was estimated with a smoke stain reflectometer. Source apportionment was carried out with the PMF receptor model developed for aerosol source characterization, provided by US EPA. Mass of species apportioned to factor, percentage of species apportioned to factors and average factor contributions of the campaigns, of working days and weekends and within the days were calculated. The PMF analysis resulted seven factors in the fine and seven factors in the coarse mode. The main sources of atmospheric aerosol in the city of Debrecen were traffic

  17. Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

    Science.gov (United States)

    Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

    2010-03-01

    This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

  18. Biomass burning contributions to urban aerosols in a coastal Mediterranean city.

    Science.gov (United States)

    Reche, C; Viana, M; Amato, F; Alastuey, A; Moreno, T; Hillamo, R; Teinilä, K; Saarnio, K; Seco, R; Peñuelas, J; Mohr, C; Prévôt, A S H; Querol, X

    2012-06-15

    Mean annual biomass burning contributions to the bulk particulate matter (PM(X)) load were quantified in a southern-European urban environment (Barcelona, Spain) with special attention to typical Mediterranean winter and summer conditions. In spite of the complexity of the local air pollution cocktail and the expected low contribution of biomass burning emissions to PM levels in Southern Europe, the impact of these emissions was detected at an urban background site by means of tracers such as levoglucosan, K(+) and organic carbon (OC). The significant correlation between levoglucosan and OC (r(2)=0.77) and K(+) (r(2)=0.65), as well as a marked day/night variability of the levoglucosan levels and levoglucosan/OC ratios was indicative of the contribution from regional scale biomass burning emissions during night-time transported by land breezes. In addition, on specific days (21-22 March), the contribution from long-range transported biomass burning aerosols was detected. Quantification of the contribution of biomass burning aerosols to PM levels on an annual basis was possible by means of the Multilinear Engine (ME). Biomass burning emissions accounted for 3% of PM(10) and PM(2.5) (annual mean), while this percentage increased up to 5% of PM(1). During the winter period, regional-scale biomass burning emissions (agricultural waste burning) were estimated to contribute with 7±4% of PM(2.5) aerosols during night-time (period when emissions were clearly detected). Long-range transported biomass burning aerosols (possibly from forest fires and/or agricultural waste burning) accounted for 5±2% of PM(2.5) during specific episodes. Annually, biomass burning emissions accounted for 19%-21% of OC levels in PM(10), PM(2.5) and PM(1). The contribution of this source to K(+) ranged between 48% for PM(10) and 97% for PM(1) (annual mean). Results for K(+) from biomass burning evidenced that this tracer is mostly emitted in the fine fraction, and thus coarse K(+) could not be

  19. Biomass burning emissions in north Australia during the early dry season: an overview of the 2014 SAFIRED campaign

    Directory of Open Access Journals (Sweden)

    M. D. Mallet

    2017-11-01

    Full Text Available The SAFIRED (Savannah Fires in the Early Dry Season campaign took place from 29 May until 30 June 2014 at the Australian Tropical Atmospheric Research Station (ATARS in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS.Biomass burning emissions dominated the gas and aerosol concentrations in this region. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north-west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. Here we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign.

  20. Biomass burning emissions in north Australia during the early dry season: an overview of the 2014 SAFIRED campaign

    Science.gov (United States)

    Mallet, Marc D.; Desservettaz, Maximilien J.; Miljevic, Branka; Milic, Andelija; Ristovski, Zoran D.; Alroe, Joel; Cravigan, Luke T.; Rohan Jayaratne, E.; Paton-Walsh, Clare; Griffith, David W. T.; Wilson, Stephen R.; Kettlewell, Graham; van der Schoot, Marcel V.; Selleck, Paul; Reisen, Fabienne; Lawson, Sarah J.; Ward, Jason; Harnwell, James; Cheng, Min; Gillett, Rob W.; Molloy, Suzie B.; Howard, Dean; Nelson, Peter F.; Morrison, Anthony L.; Edwards, Grant C.; Williams, Alastair G.; Chambers, Scott D.; Werczynski, Sylvester; Williams, Leah R.; Winton, V. Holly L.; Atkinson, Brad; Wang, Xianyu; Keywood, Melita D.

    2017-11-01

    The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29 May until 30 June 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS.Biomass burning emissions dominated the gas and aerosol concentrations in this region. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north-west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. Here we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign.

  1. Substantial secondary organic aerosol formation in a coniferous forest: observations of both day- and nighttime chemistry

    OpenAIRE

    A. K. Y. Lee; J. P. D. Abbatt; W. R. Leaitch; S.-M. Li; S. J. Sjostedt; S. J. Sjostedt; J. J. B. Wentzell; J. Liggio; A. M. Macdonald

    2016-01-01

    Substantial biogenic secondary organic aerosol (BSOA) formation was investigated in a coniferous forest mountain region at Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment with limited influence from anthropogenic emissions. Positive matrix factorization of aerosol mass spectrometry (AMS) measurement identifie...

  2. Quantitative characterization of urban sources of organic aerosol by high-resolution gas chromatography

    International Nuclear Information System (INIS)

    Hildemann, L.M.; Mazurek, M.A.; Cass, G.R.; Simoneit, B.R.T.

    1991-01-01

    Fine aerosol emissions have been collected from a variety of urban combustion sources, including an industrial boiler, a fireplace, automobiles, diesel trucks, gas-fired home appliances, and meat cooking operations, by use of a dilution sampling system. Other sampling techniques have been utilized to collect fine aerosol samples of paved road dust, brake wear, tire wear, cigarette smoke, tar pot emissions, and vegetative detritus. The organic matter contained in each of these samples has been analyzed via high-resolution gas chromatography. By use of a simple computational approach, a quantitative, 50-parameter characterization of the elutable fine organic aerosol emitted from each source type has been determined. The organic mass distribution fingerprints obtained by this approach are shown to differ significantly from each other for most of the source types tested, using hierarchical cluster analysis

  3. Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

    Energy Technology Data Exchange (ETDEWEB)

    Ching, Ping Pui; Riemer, Nicole; West, Matthew

    2016-05-27

    Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcel cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.

  4. Ambient Aerosols in the Southern Hemisphere on Ascension Island during the LASIC Campaign: Biomass Burning Season versus Near Pristine Background Conditions

    Science.gov (United States)

    Aiken, A. C.; Springston, S. R.; Watson, T. B.; Sedlacek, A. J., III; Zuidema, P.; Adebiyi, A. A.; Uin, J.; Kuang, C.; Flynn, C. J.

    2017-12-01

    Ascension Island is located 8 degrees South of the Equator and 15 degrees West Longitude in the middle of the South Atlantic Ocean, at least 1000 miles from any major shoreline and closest to the continent of Africa. While low Southern Hemisphere background aerosol and trace gas measurements are observed most of the year, that picture changes during the South African Biomass Burning (BB) season. BB emissions are a large source of carbon to the atmosphere via particles and gas phase species and with a potential rise in drought and extreme events in the future, these numbers are expected to increase. From approximately June-October every year, the plume of South African BB emissions, the largest BB source in the world, are advected West and are known to impact both the boundary layer and free troposphere at Ascension Island (Zuidema et al., 2016). During the U.S. DOE ARM field campaign, Layered Atlantic Smoke Interactions with Clouds (LASIC), aerosol and trace gas measurements were collected continuously from June 2016 through October 2017 over a 1.5 year period. Two BB seasons are contrasted with the near pristine background conditions during the campaign from the ARM Aerosol Mobile Facility 1 (AMF1) and Mobile Aerosol Observing System (MAOS). Numerous direct in situ aerosol and trace gas measurements are presented, e.g. black carbon (BC), carbon monoxide (CO), PM1 and PM10 aerosol absorption and scattering, submicron non-refractory chemical composition (Organics, Sulfate, Nitrate, Ammonium, Chloride), etc. Aerosol and trace gas signatures are investigated along with backtrajectories to identify sources. Carbonaceous aerosols emitted with gas-phase CO are used to determine particulate emission ratios along with intrinsic and extrinsic aerosol properties. BC mass concentrations reach 1 µg m-3 during multiday plumes and exceed 25% of the total aerosol submicron mass concentration. Organic Aerosol (OA) to BC Ratios of 2.4 in the plume are much higher than previously

  5. Distribution of sulfur aerosol precursors in the SPCZ released by continuous volcanic degassing at Ambrym, Vanuatu

    Science.gov (United States)

    Lefèvre, Jérôme; Menkes, Christophe; Bani, Philipson; Marchesiello, Patrick; Curci, Gabriele; Grell, Georg A.; Frouin, Robert

    2016-08-01

    The Melanesian Volcanic Arc (MVA) emits about 12 kT d- 1 of sulfur dioxide (SO2) to the atmosphere from continuous passive (non-explosive) volcanic degassing, which contributes 20% of the global SO2 emission from volcanoes. Here we assess, from up-to-date and long-term observations, the SO2 emission of the Ambrym volcano, one of the dominant volcanoes in the MVA, and we investigate its role as sulfate precursor on the regional distribution of aerosols, using both satellite observations and model results at 1° × 1° spatial resolution from WRF-Chem/GOCART. Without considering aerosol forcing on clouds, our model parameterizations for convection, vertical mixing and cloud properties provide a reliable chemical weather representation, making possible a cross-examination of model solution and observations. This preliminary work enables the identification of biases and limitations affecting both the model (missing sources) and satellite sensors and algorithms (for aerosol detection and classification) and leads to the implementation of improved transport and aerosol processes in the modeling system. On the one hand, the model confirms a 50% underestimation of SO2 emissions due to satellite swath sampling of the Ozone Monitoring Instrument (OMI), consistent with field studies. The OMI irregular sampling also produces a level of noise that impairs its monitoring capacity during short-term volcanic events. On the other hand, the model reveals a large sensitivity on aerosol composition and Aerosol Optical Depth (AOD) due to choices of both the source function in WRF-Chem and size parameters for sea-salt in FlexAOD, the post-processor used to compute offline the simulated AOD. We then proceed to diagnosing the role of SO2 volcanic emission in the regional aerosol composition. The model shows that both dynamics and cloud properties associated with the South Pacific Convergence Zone (SPCZ) have a large influence on the oxidation of SO2 and on the transport pathways of

  6. Aerosols from fires: an examination of the effects on ozone photochemistry in the Western United States.

    Science.gov (United States)

    Jiang, Xiaoyan; Wiedinmyer, Christine; Carlton, Annmarie G

    2012-11-06

    This study presents a first attempt to investigate the roles of fire aerosols in ozone (O(3)) photochemistry using an online coupled meteorology-chemistry model, the Weather Research and Foresting model with Chemistry (WRF-Chem). Four 1-month WRF-Chem simulations for August 2007, with and without fire emissions, were carried out to assess the sensitivity of O(3) predictions to the emissions and subsequent radiative feedbacks associated with large-scale fires in the Western United States (U.S.). Results show that decreases in planetary boundary layer height (PBLH) resulting from the radiative effects of fire aerosols and increases in emissions of nitrogen oxides (NO(x)) and volatile organic compounds (VOCs) from the fires tend to increase modeled O(3) concentrations near the source. Reductions in downward shortwave radiation reaching the surface and surface temperature due to fire aerosols cause decreases in biogenic isoprene emissions and J(NO(2)) photolysis rates, resulting in reductions in O(3) concentrations by as much as 15%. Thus, the results presented in this study imply that considering the radiative effects of fire aerosols may reduce O(3) overestimation by traditional photochemical models that do not consider fire-induced changes in meteorology; implementation of coupled meteorology-chemistry models are required to simulate the atmospheric chemistry impacted by large-scale fires.

  7. Review of recent research on the climatic effect of aerosols

    International Nuclear Information System (INIS)

    Charlock, T.P.; Kondratyev, K.; Prokofyev, M.

    1993-01-01

    A review of relatively recent research on the climatic effects of aerosols is presented. Most of the inferences of the climatic effects of aerosols have been obtained through assuming a certain aerosol model in conjunction with a particular climate model. The following radiative effects of aerosols are identified: The planetary albedo is generally increased due to the backscatter of solar radiation by aerosols, with the exception of aerosols situated above a highly reflecting surface. Solar radiation absorption by some aerosols can offset the cooling due to aerosol backscatter. Although aerosol effects dominate for short-wave radiation, absorption and emission of terrestrial radiation by aerosols produces a warming effect. Various climate models are used to assess the impact of aerosols on climate. A two-stream approximation to the radiation transfer equation is adequate for optically thin layers where single scattering is applicable. Improved models to include aerosol terrestrial radiation effects, important feedback mechanisms, and the prediction of globally and seasonally averaged surface and atmospheric temperatures are provided by the so-called radiative-convective models (RCM's). The basic structure of the RCM's, which is regarded as adequate for many aerosol climate applications, is described. The general circulation model (GCM) is also described briefly. A full-scale GCM incorporating realistic aerosol inputs is yet to be formulated to include regional variability of the aerosol. Moreover, detailed computer modeling associated with GCM climate models can often confuse the basic physics. Because volcanic aerosols injected into the stratosphere have long residence times, they provide a good case study of the climate response to a change in the atmospheric aerosol. The chapter gives a critique of modeling work done to establish climatic effects of stratospheric aerosols

  8. Impacts of Anthropogenic Aerosols on Regional Climate: Extreme Events, Stagnation, and the United States Warming Hole

    Science.gov (United States)

    Mascioli, Nora R.

    Extreme temperatures, heat waves, heavy rainfall events, drought, and extreme air pollution events have adverse effects on human health, infrastructure, agriculture and economies. The frequency, magnitude and duration of these events are expected to change in the future in response to increasing greenhouse gases and decreasing aerosols, but future climate projections are uncertain. A significant portion of this uncertainty arises from uncertainty in the effects of aerosol forcing: to what extent were the effects from greenhouse gases masked by aerosol forcing over the historical observational period, and how much will decreases in aerosol forcing influence regional and global climate over the remainder of the 21st century? The observed frequency and intensity of extreme heat and precipitation events have increased in the U.S. over the latter half of the 20th century. Using aerosol only (AER) and greenhouse gas only (GHG) simulations from 1860 to 2005 in the GFDL CM3 chemistry-climate model, I parse apart the competing influences of aerosols and greenhouse gases on these extreme events. I find that small changes in extremes in the "all forcing" simulations reflect cancellations between the effects of increasing anthropogenic aerosols and greenhouse gases. In AER, extreme high temperatures and the number of days with temperatures above the 90th percentile decline over most of the U.S., while in GHG high temperature extremes increase over most of the U.S. The spatial response patterns in AER and GHG are significantly anti-correlated, suggesting a preferred regional mode of response that is largely independent of the type of forcing. Extreme precipitation over the eastern U.S. decreases in AER, particularly in winter, and increases over the eastern and central U.S. in GHG, particularly in spring. Over the 21 st century under the RCP8.5 emissions scenario, the patterns of extreme temperature and precipitation change associated with greenhouse gas forcing dominate. The

  9. Impacts of land use and land cover changes on biogenic emissions of volatile organic compounds in China from the late 1980s to the mid-2000s: implications for tropospheric ozone and secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    Yu Fu

    2014-11-01

    Full Text Available Based on the MEGAN (Model of Emissions of Gases and Aerosols from Nature module embedded within the global chemical transport model (GEOS-Chem, we estimate the changes in emissions of biogenic volatile organic compounds (BVOCs and their impacts on surface-layer O3 and secondary organic aerosols (SOA in China between the late 1980s and the mid-2000s by using the land cover dataset derived from remote sensing images and land use survey. The land cover change in China from the late 1980s to the mid-2000s can be characterised by an expansion of urban areas (the total urban area in the mid-2000s was four times that in the late 1980s and a reduction in total vegetation coverage by 4%. Regionally, the fractions of land covered by forests exhibited increases in southeastern and northeastern China by 10–30 and 5–15%, respectively, those covered by cropland decreased in most regions except that the farming–pastoral zone in northern China increased by 5–20%, and the factions of grassland in northern China showed a large reduction of 5–30%. With changes in both land cover and meteorological fields, annual BVOC emission in China is estimated to increase by 11.4% in the mid-2000s relative to the late 1980s. With anthropogenic emissions of O3 precursors, aerosol precursors and aerosols fixed at year 2005 levels, the changes in land cover and meteorological parameters from the late 1980s to the mid-2000s are simulated to change the seasonal mean surface-layer O3 concentrations by −4 to +6 ppbv (−10 to +20% and to change the seasonal mean surface-layer SOA concentrations by −0.4 to +0.6 µg m−3 (−20 to +30% over China. We find that the decadal changes in meteorological parameters had larger collective effects on BVOC emissions and surface-layer concentrations of O3 and SOA than those in land cover and land use alone. We also perform a sensitivity simulation to compare the impacts of changes in anthropogenic emissions on concentrations of O3

  10. Identification of secondary aerosol precursors emitted by an aircraft turbofan

    Directory of Open Access Journals (Sweden)

    D. Kılıç

    2018-05-01

    Full Text Available Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS for nonrefractory particulate matter (NR-PM1 were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5–7 %, more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

  11. Observed aerosol suppression of cloud ice in low-level Arctic mixed-phase clouds

    OpenAIRE

    Norgren, Matthew S.; Boer, Gijs; Shupe, Matthew D.

    2018-01-01

    The interactions that occur between aerosols and a mixed-phase cloud system, and the subsequent alteration of the microphysical state of such clouds, is a problem that has yet to be well constrained. Advancing our understanding of aerosol-ice processes is necessary to determine the impact of natural and anthropogenic emissions on Earth’s climate and to improve our capability to predict future climate states. This paper deals specifically with how aerosols influence ice mass production in low-...

  12. Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

    Science.gov (United States)

    Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

    2017-02-01

    Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

  13. Assessment of state-of-the-art dust emission scheme in GEOS

    Science.gov (United States)

    Darmenov, A.; Liu, X.; Prigent, C.

    2017-12-01

    The GEOS modeling system has been extended with state-of-the-art parameterization of dust emissions based on the vertical flux formulation described in Kok et al., 2014. The new dust scheme was coupled with the GOCART and MAM aerosol models. In the present study we compared dust emissions, aerosol optical depth (AOD) and radiative fluxes from GEOS experiments with the standard and new dust emissions. AOD from the model experiments were also compared with AERONET and satellite based AOD product. Based on this comparative analysis we concluded that the new parameterization improved the GEOS capability to model dust aerosols originating from African sources, however it led to overestimation of dust emissions from Asian and Middle-Eastern sources. Further regional tuning of key parameters controlling the threshold friction velocity may be required in order to attain more definitive and uniform improvement in the dust modeling skill with the newly implemented dust emissions scheme.

  14. New trajectory-driven aerosol and chemical process model Chemical and Aerosol Lagrangian Model (CALM

    Directory of Open Access Journals (Sweden)

    P. Tunved

    2010-11-01

    Full Text Available A new Chemical and Aerosol Lagrangian Model (CALM has been developed and tested. The model incorporates all central aerosol dynamical processes, from nucleation, condensation, coagulation and deposition to cloud formation and in-cloud processing. The model is tested and evaluated against observations performed at the SMEAR II station located at Hyytiälä (61° 51' N, 24° 17' E over a time period of two years, 2000–2001. The model shows good agreement with measurements throughout most of the year, but fails in reproducing the aerosol properties during the winter season, resulting in poor agreement between model and measurements especially during December–January. Nevertheless, through the rest of the year both trends and magnitude of modal concentrations show good agreement with observation, as do the monthly average size distribution properties. The model is also shown to capture individual nucleation events to a certain degree. This indicates that nucleation largely is controlled by the availability of nucleating material (as prescribed by the [H2SO4], availability of condensing material (in this model 15% of primary reactions of monoterpenes (MT are assumed to produce low volatile species and the properties of the size distribution (more specifically, the condensation sink. This is further demonstrated by the fact that the model captures the annual trend in nuclei mode concentration. The model is also used, alongside sensitivity tests, to examine which processes dominate the aerosol size distribution physical properties. It is shown, in agreement with previous studies, that nucleation governs the number concentration during transport from clean areas. It is also shown that primary number emissions almost exclusively govern the CN concentration when air from Central Europe is advected north over Scandinavia. We also show that biogenic emissions have a large influence on the amount of potential CCN observed

  15. Volatile chemical products emerging as largest petrochemical source of urban organic emissions

    Science.gov (United States)

    McDonald, Brian C.; de Gouw, Joost A.; Gilman, Jessica B.; Jathar, Shantanu H.; Akherati, Ali; Cappa, Christopher D.; Jimenez, Jose L.; Lee-Taylor, Julia; Hayes, Patrick L.; McKeen, Stuart A.; Cui, Yu Yan; Kim, Si-Wan; Gentner, Drew R.; Isaacman-VanWertz, Gabriel; Goldstein, Allen H.; Harley, Robert A.; Frost, Gregory J.; Roberts, James M.; Ryerson, Thomas B.; Trainer, Michael

    2018-02-01

    A gap in emission inventories of urban volatile organic compound (VOC) sources, which contribute to regional ozone and aerosol burdens, has increased as transportation emissions in the United States and Europe have declined rapidly. A detailed mass balance demonstrates that the use of volatile chemical products (VCPs)—including pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products—now constitutes half of fossil fuel VOC emissions in industrialized cities. The high fraction of VCP emissions is consistent with observed urban outdoor and indoor air measurements. We show that human exposure to carbonaceous aerosols of fossil origin is transitioning away from transportation-related sources and toward VCPs. Existing U.S. regulations on VCPs emphasize mitigating ozone and air toxics, but they currently exempt many chemicals that lead to secondary organic aerosols.

  16. Characterization of biogenic secondary organic aerosols using statistical methods; Charakterisierung Biogener Sekundaerer Organischer Aerosole mit Statistischen Methoden

    Energy Technology Data Exchange (ETDEWEB)

    Spindler, Christian

    2010-07-01

    Atmospheric aerosols have important influence on the radiation balance of the Earth, on visibility and human health. Secondary organic aerosol is formed from gas-to-particle conversion of oxidized volatile organic compounds. A dominant fraction of the gases originates from plant emissions, making biogenic secondary organic aerosol (BSOA) an especially important constituent of the atmosphere. Knowing the chemical composition of BSOA particles is crucial for a thorough understanding of aerosol processes in the environment. In this work, the chemical composition of BSOA particles was measured with aerosol mass spectrometry and analyzed with statistical methods. The experimental part of the work comprises process studies of the formation and aging of biogenic aerosols in simulation chambers. Using a plant chamber, real tree emissions were used to produce particles in a way close to conditions in forest environments. In the outdoor chamber SAPHIR, OH-radicals were produced from the photooxidation of ozone under illumination with natural sunlight. Here, BSOA was produced from defined mixtures of mono- and sesquiterpenes that represent boreal forest emissions. A third kind of experiments was performed in the indoor chamber AIDA. Here, particles were produced from ozonolysis of single monoterpenes and aged by condensing OH-oxidation products. Two aerosol mass spectrometers (AMS) were used to measure the chemical composition of the particles. One of the instruments is equipped with a quadrupole mass spectrometer providing unit mass resolution. The second instrument contains a time-of-flight mass spectrometer and provides mass resolution sufficient to distinguish different fragments with the same nominal mass. Aerosol mass spectra obtained with these instruments are strongly fragmented due to electron impact ionization of the evaporated molecules. In addition, typical BSOA mass spectra are very similar to each other. In order to get a more detailed knowledge about the mass

  17. Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

    Science.gov (United States)

    Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

    2017-06-01

    A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

  18. Time Dependence of Aerosol Light Scattering Downwind of Forest Fires

    Science.gov (United States)

    Kleinman, L. I.; Sedlacek, A. J., III; Wang, J.; Lewis, E. R.; Springston, S. R.; Chand, D.; Shilling, J.; Arnott, W. P.; Freedman, A.; Onasch, T. B.; Fortner, E.; Zhang, Q.; Yokelson, R. J.; Adachi, K.; Buseck, P. R.

    2017-12-01

    In the first phase of BBOP (Biomass Burn Observation Project), a Department of Energy (DOE) sponsored study, wildland fires in the Pacific Northwest were sampled from the G-1 aircraft via sequences of transects that encountered emission whose age (time since emission) ranged from approximately 15 minutes to four hours. Comparisons between transects allowed us to determine the near-field time evolution of trace gases, aerosol particles, and optical properties. The fractional increase in aerosol concentration with plume age was typically less than a third of the fractional increase in light scattering. In some fires the increase in light scattering exceeded a factor of two. Two possible causes for the discrepancy between scattering and aerosol mass are i) the downwind formation of refractory tar balls that are not detected by the AMS and therefore contribute to scattering but not to aerosol mass and ii) changes to the aerosol size distribution. Both possibilities are considered. Our information on tar balls comes from an analysis of TEM grids. A direct determination of size changes is complicated by extremely high aerosol number concentrations that caused coincidence problems for the PCASP and UHSAS probes. We instead construct a set of plausible log normal size distributions and for each member of the set do Mie calculations to determine mass scattering efficiency (MSE), angstrom exponents, and backscatter ratios. Best fit size distributions are selected by comparison with observed data derived from multi-wavelength scattering measurements, an extrapolated FIMS size distribution, and mass measurements from an SP-AMS. MSE at 550 nm varies from a typical near source value of 2-3 to about 4 in aged air.

  19. Geochemistry of regional background aerosols in the Western Mediterranean

    Science.gov (United States)

    Pey, J.; Pérez, N.; Castillo, S.; Viana, M.; Moreno, T.; Pandolfi, M.; López-Sebastián, J. M.; Alastuey, A.; Querol, X.

    2009-11-01

    The chemical composition of regional background aerosols, and the time variability and sources in the Western Mediterranean are interpreted in this study. To this end 2002-2007 PM speciation data from an European Supersite for Atmospheric Aerosol Research (Montseny, MSY, located 40 km NNE of Barcelona in NE Spain) were evaluated, with these data being considered representative of regional background aerosols in the Western Mediterranean Basin. The mean PM 10, PM 2.5 and PM 1 levels at MSY during 2002-2007 were 16, 14 and 11 µg/m 3, respectively. After compiling data on regional background PM speciation from Europe to compare our data, it is evidenced that the Western Mediterranean aerosol is characterised by higher concentrations of crustal material but lower levels of OM + EC and ammonium nitrate than at central European sites. Relatively high PM 2.5 concentrations due to the transport of anthropogenic aerosols (mostly carbonaceous and sulphate) from populated coastal areas were recorded, especially during winter anticyclonic episodes and summer midday PM highs (the latter associated with the transport of the breeze and the expansion of the mixing layer). Source apportionment analyses indicated that the major contributors to PM 2.5 and PM 10 were secondary sulphate, secondary nitrate and crustal material, whereas the higher load of the anthropogenic component in PM 2.5 reflects the influence of regional (traffic and industrial) emissions. Levels of mineral, sulphate, sea spray and carbonaceous aerosols were higher in summer, whereas nitrate levels and Cl/Na were higher in winter. A considerably high OC/EC ratio (14 in summer, 10 in winter) was detected, which could be due to a combination of high biogenic emissions of secondary organic aerosol, SOA precursors, ozone levels and insolation, and intensive recirculation of aged air masses. Compared with more locally derived crustal geological dusts, African dust intrusions introduce relatively quartz-poor but clay

  20. Determination of Monthly Aerosol Types in Manila Observatory and Notre Dame of Marbel University from Aerosol Robotic Network (AERONET) measurements.

    Science.gov (United States)

    Ong, H. J. J.; Lagrosas, N.; Uy, S. N.; Gacal, G. F. B.; Dorado, S.; Tobias, V., Jr.; Holben, B. N.

    2016-12-01

    This study aims to identify aerosol types in Manila Observatory (MO) and Notre Dame of Marbel University (NDMU) using Aerosol Robotic Network (AERONET) Level 2.0 inversion data and five dimensional specified clustering and Mahalanobis classification. The parameters used are the 440-870 nm extinction Angström exponent (EAE), 440 nm single scattering albedo (SSA), 440-870 nm absorption Angström exponent (AAE), 440 nm real and imaginary refractive indices. Specified clustering makes use of AERONET data from 7 sites to define 7 aerosol classes: mineral dust (MD), polluted dust (PD), urban industrial (UI), urban industrial developing (UID), biomass burning white smoke (BBW), biomass burning dark smoke (BBD), and marine aerosols. This is similar to the classes used by Russell et al, 2014. A data point is classified into a class based on the closest 5-dimensional Mahalanobis distance (Russell et al, 2014 & Hamill et al, 2016). This method is applied to all 173 MO data points from January 2009 to June 2015 and to all 24 NDMU data points from December 2009 to July 2015 to look at monthly and seasonal variations of aerosol types. The MO and NDMU aerosols are predominantly PD ( 77%) and PD & UID ( 75%) respectively (Figs.1a-b); PD is predominant in the months of February to May in MO and February to March in NDMU. PD results from less strict emission and environmental regulations (Catrall 2005). Average SSA values in MO is comparable to the mean SSA for PD ( 0.89). This can be attributed to presence of high absorbing aerosol types, e.g., carbon which is a product of transportation emissions. The second most dominant aerosol type in MO is UID ( 15%), in NDMU it is BBW ( 25%). In Manila, the high sources of PD and UID (fine particles) is generally from vehicular combustion (Oanh, et al 2006). The detection of BBW in MO from April to May can be attributed to the fires which are common in these dry months. In NDMU, BBW source is from biomass burning (smoldering). In this

  1. Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign

    Energy Technology Data Exchange (ETDEWEB)

    Gyawali, Madhu; Arnott, W.; Zaveri, Rahul; Song, Chen; Flowers, Bradley; Dubey, Manvendra; Setyan, Ari; Zhang, Qi; China, Swarup; Mazzoleni, Claudio; Gorkowski, Kyle; Subramanian, R.; Moosmüller, Hans

    2017-11-01

    We present the evolution of multispectral optical properties as urban aerosols aged and interacted with biogenic emissions resulting in stronger short wavelength absorption and formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made during June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths ranging from 355 to 870 nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From the 22nd to the 28th of June, secondary organic aerosol mass increased significantly at both sites due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared to the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. These results suggest formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.

  2. Lidar Investigation of Aerosol Pollution Distribution near a Coal Power Plant

    Science.gov (United States)

    Mitsev, TS.; Kolarov, G.

    1992-01-01

    Using aerosol lidars with high spatial and temporal resolution with the possibility of real-time data interpretation can solve a large number of ecological problems related to the aerosol-field distribution and variation and the structure of convective flows. Significantly less expensive specialized lidars are used in studying anthropogenic aerosols in the planetary boundary layer. Here, we present results of lidar measurements of the mass-concentration field around a coal-fired power plant with intensive local aerosol sources. We studied the pollution evolution as a function of the emission dynamics and the presence of retaining layers. The technique used incorporates complex analysis of three types of lidar mapping: horizontal map of the aerosol field, vertical cross-section map, and a series of profiles along a selected path. The lidar-sounding cycle was performed for the time of atmosphere's quasi-stationarity.

  3. Lidar investigation of aerosol pollution distribution near a coal power plant

    International Nuclear Information System (INIS)

    Mitsev, T.S.; Kolarov, G.

    1992-01-01

    Using aerosol lidars with high spatial and temporal resolution with the possibility of real-time data interpretation can solve a large number of ecological problems related to the aerosol-field distribution and variation and the structure of convective flows. Significantly less expensive specialized lidars are used in studying anthropogenic aerosols in the planetary boundary layer. Here, results are presented of lidar measurements of the mass-concentration field around a coal-fired power plant with intensive local aerosol sources. The authors studied the pollution evolution as a function of the emission dynamics and the presence of retaining layers. The technique used incorporates complex analysis of three types of lidar mapping: horizontal map of the aerosol field, vertical cross-section map, and a series of profiles along a selected path. The lidar-sounding cycle was performed for the time of atmosphere's quasi-stationarity

  4. The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

    Directory of Open Access Journals (Sweden)

    K. M. Sakamoto

    2016-06-01

    Full Text Available Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width

  5. The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

    Science.gov (United States)

    Sakamoto, Kimiko M.; Laing, James R.; Stevens, Robin G.; Jaffe, Daniel A.; Pierce, Jeffrey R.

    2016-06-01

    Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The

  6. Experimental Characterization of Radiation Forcing due to Atmospheric Aerosols

    Science.gov (United States)

    Sreenivas, K. R.; Singh, D. K.; Ponnulakshmi, V. K.; Subramanian, G.

    2011-11-01

    Micro-meteorological processes in the nocturnal atmospheric boundary layer (NBL) including the formation of radiation-fog and the development of inversion layers are controlled by heat transfer and the vertical temperature distribution close to the ground. In a recent study, it has been shown that the temperature profile close to the ground in stably-stratified, NBL is controlled by the radiative forcing due to suspended aerosols. Estimating aerosol forcing is also important in geo-engineering applications to evaluate the use of aerosols to mitigate greenhouse effects. Modeling capability in the above scenarios is limited by our knowledge of this forcing. Here, the design of an experimental setup is presented which can be used for evaluating the IR-radiation forcing on aerosols under either Rayleigh-Benard condition or under conditions corresponding to the NBL. We present results indicating the effect of surface emissivities of the top and bottom boundaries and the aerosol concentration on the temperature profiles. In order to understand the observed enhancement of the convection-threshold, we have determined the conduction-radiation time constant of an aerosol laden air layer. Our results help to explain observed temperature profiles in the NBL, the apparent stability of such profiles and indicate the need to account for the effect of aerosols in climatic/weather models.

  7. Interpreting aerosol lifetimes using the GEOS-Chem model and constraints from radionuclide measurements

    Energy Technology Data Exchange (ETDEWEB)

    Croft, B. [Dalhousie Univ., Halifax (Canada). Dept. of Physics and Atmospheric Science; Pierce, J.R. [Dalhousie Univ., Halifax (Canada). Dept. of Physics and Atmospheric Science; Colorado State Univ., Fort Collins, CO (United States); Martin, R.V. [Dalhousie Univ., Halifax (Canada). Dept. of Physics and Atmospheric Science; Harvard-Smithsonian Center for Astrophysics, Cambridge, MA (United States)

    2014-07-01

    Aerosol removal processes control global aerosol abundance, but the rate of that removal remains uncertain. A recent study of aerosol-bound radionuclide measurements after the Fukushima Daiichi nuclear power plant accident documents {sup 137}Cs removal (e-folding) times of 10.0-13.9 days, suggesting that mean aerosol lifetimes in the range of 3-7 days in global models might be too short by a factor of two. In this study, we attribute this discrepancy to differences between the e-folding and mean aerosol lifetimes. We implement a simulation of {sup 137}Cs and {sup 133}Xe into the GEOS-Chem chemical transport model and examine the removal rates for the Fukushima case. We find a general consistency between modelled and measured e-folding times. The simulated {sup 137}Cs global burden e-folding time is about 14 days. However, the simulated mean lifetime of aerosol-bound {sup 137}Cs over a 6-month post-accident period is only 1.8 days. We find that the mean lifetime depends strongly on the removal rates in the first few days after emissions, before the aerosols leave the boundary layer and are transported to altitudes and latitudes where lifetimes with respect to wet removal are longer by a few orders of magnitude. We present sensitivity simulations that demonstrate the influence of differences in altitude and location of the radionuclides on the mean lifetime. Global mean lifetimes are shown to strongly depend on the altitude of injection. The global mean {sup 137}Cs lifetime is more than one order of magnitude greater for the injection at 7 km than into the boundary layer above the Fukushima site. Instantaneous removal rates are slower during the first few days after the emissions for a free tropospheric versus boundary layer injection and this strongly controls the mean lifetimes. Global mean aerosol lifetimes for the GEOS-Chem model are 3-6 days, which is longer than that for the {sup 137}Cs injected at the Fukushima site (likely due to precipitation shortly after

  8. Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

    2010-03-15

    Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

  9. Coupling aerosol-cloud-radiative processes in the WRF-Chem model: Investigating the radiative impact of elevated point sources

    Directory of Open Access Journals (Sweden)

    E. G. Chapman

    2009-02-01

    Full Text Available The local and regional influence of elevated point sources on summertime aerosol forcing and cloud-aerosol interactions in northeastern North America was investigated using the WRF-Chem community model. The direct effects of aerosols on incoming solar radiation were simulated using existing modules to relate aerosol sizes and chemical composition to aerosol optical properties. Indirect effects were simulated by adding a prognostic treatment of cloud droplet number and adding modules that activate aerosol particles to form cloud droplets, simulate aqueous-phase chemistry, and tie a two-moment treatment of cloud water (cloud water mass and cloud droplet number to precipitation and an existing radiation scheme. Fully interactive feedbacks thus were created within the modified model, with aerosols affecting cloud droplet number and cloud radiative properties, and clouds altering aerosol size and composition via aqueous processes, wet scavenging, and gas-phase-related photolytic processes. Comparisons of a baseline simulation with observations show that the model captured the general temporal cycle of aerosol optical depths (AODs and produced clouds of comparable thickness to observations at approximately the proper times and places. The model overpredicted SO2 mixing ratios and PM2.5 mass, but reproduced the range of observed SO2 to sulfate aerosol ratios, suggesting that atmospheric oxidation processes leading to aerosol sulfate formation are captured in the model. The baseline simulation was compared to a sensitivity simulation in which all emissions at model levels above the surface layer were set to zero, thus removing stack emissions. Instantaneous, site-specific differences for aerosol and cloud related properties between the two simulations could be quite large, as removing above-surface emission sources influenced when and where clouds formed within the modeling domain. When summed spatially over the finest

  10. Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

    Directory of Open Access Journals (Sweden)

    R. A. de Villiers

    2010-06-01

    Full Text Available Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm including volume depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions. Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient 532 nm,volume depolarization and color ratio between 1064 and 532 nm in aerosol layers along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Optical depth of the aerosol layers are always rather small (<4% while transported over the Arctic and ratio of the total attenuated backscatter (i.e. including molecular contribution provide more stable result than conventional aerosol backscatter ratio. Above Asia, CALIPSO data indicate more depolarization (up to 15% and largest color ratio (>0.5 for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust, while low depolarization together with smaller and quasi constant color ratio (≈0.3 are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarization ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European

  11. Characterization of regional atmospheric aerosols over Hungary by PIXE elemental analysis

    International Nuclear Information System (INIS)

    Koltay, E.; Szabo, G.; Borbely Kiss, I.; Somorjai, E.; Kiss, A.Z.

    1994-01-01

    Studying the characteristic features of atmospheric aerosols emitted by natural and anthropogenic sources is of basic importance for a detailed understanding of the physics and chemistry of the atmosphere. Environmental pollution by atmospheric aerosols and their impact can be tested in the same way, too. The separation of natural and anthropogenic components of the aerosol can be done through enrichment factors and size distribution curves deduced from analytical information. The Particle Induced X-ray Emission (PIXE) technique has been applied in aerosol studies by the authors. Results obtained on atmospheric aerosols collected over Hungary and presented in terms of concentrations, enrichment factors, regional signatures, deposition velocities, transport properties and apportionment of sources illustrate the scope and proportions of the potential contribution of PIXE to the methodology of atmospheric aerosol studies. Continued activity planned in the framework of the present CRP may widen the scope of the investigations mainly in the field of size-fractioned sampling and - possibly - in the direction of individual characterization of aerosol particles. (author). 14 refs

  12. New approaches to quantifying aerosol influence on the cloud radiative effect.

    Science.gov (United States)

    Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S; Carslaw, Kenneth S; Schmidt, K Sebastian

    2016-05-24

    The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

  13. Continental anthropogenic primary particle number emissions

    Science.gov (United States)

    Paasonen, Pauli; Kupiainen, Kaarle; Klimont, Zbigniew; Visschedijk, Antoon; Denier van der Gon, Hugo A. C.; Amann, Markus

    2016-06-01

    Atmospheric aerosol particle number concentrations impact our climate and health in ways different from those of aerosol mass concentrations. However, the global, current and future anthropogenic particle number emissions and their size distributions are so far poorly known. In this article, we present the implementation of particle number emission factors and the related size distributions in the GAINS (Greenhouse Gas-Air Pollution Interactions and Synergies) model. This implementation allows for global estimates of particle number emissions under different future scenarios, consistent with emissions of other pollutants and greenhouse gases. In addition to determining the general particulate number emissions, we also describe a method to estimate the number size distributions of the emitted black carbon particles. The first results show that the sources dominating the particle number emissions are different to those dominating the mass emissions. The major global number source is road traffic, followed by residential combustion of biofuels and coal (especially in China, India and Africa), coke production (Russia and China), and industrial combustion and processes. The size distributions of emitted particles differ across the world, depending on the main sources: in regions dominated by traffic and industry, the number size distribution of emissions peaks in diameters range from 20 to 50 nm, whereas in regions with intensive biofuel combustion and/or agricultural waste burning, the emissions of particles with diameters around 100 nm are dominant. In the baseline (current legislation) scenario, the particle number emissions in Europe, Northern and Southern Americas, Australia, and China decrease until 2030, whereas especially for India, a strong increase is estimated. The results of this study provide input for modelling of the future changes in aerosol-cloud interactions as well as particle number related adverse health effects, e.g. in response to tightening

  14. Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

    Directory of Open Access Journals (Sweden)

    X. Zhang

    2018-04-01

    Full Text Available An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l. in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1 and obtain the dynamic processes (emissions, transport, and chemical evolution of biomass burning (BB, frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ PM1 mass concentration was 4.44 (±4.54 µg m−3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA was the dominant PM1 species (accounting for 54.3 % of total PM1 on average followed by black carbon (BC (25.0 %, sulfate (9.3 %, ammonium (5.8 %, nitrate (5.1 %, and chloride (0.4 %. The average size distributions of PM1 species all peaked at an overlapping accumulation mode (∼ 500 nm, suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %, a nitrogen-containing OA (NOA, 13.9 % and a more-oxidized oxygenated OA (MO-OOA, 42.4 %. Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

  15. Field and Laboratory Studies of Atmospheric Organic Aerosol

    Science.gov (United States)

    Coggon, Matthew Mitchell

    This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed

  16. ISS Ambient Air Quality: Updated Inventory of Known Aerosol Sources

    Science.gov (United States)

    Meyer, Marit

    2014-01-01

    Spacecraft cabin air quality is of fundamental importance to crew health, with concerns encompassing both gaseous contaminants and particulate matter. Little opportunity exists for direct measurement of aerosol concentrations on the International Space Station (ISS), however, an aerosol source model was developed for the purpose of filtration and ventilation systems design. This model has successfully been applied, however, since the initial effort, an increase in the number of crewmembers from 3 to 6 and new processes on board the ISS necessitate an updated aerosol inventory to accurately reflect the current ambient aerosol conditions. Results from recent analyses of dust samples from ISS, combined with a literature review provide new predicted aerosol emission rates in terms of size-segregated mass and number concentration. Some new aerosol sources have been considered and added to the existing array of materials. The goal of this work is to provide updated filtration model inputs which can verify that the current ISS filtration system is adequate and filter lifetime targets are met. This inventory of aerosol sources is applicable to other spacecraft, and becomes more important as NASA considers future long term exploration missions, which will preclude the opportunity for resupply of filtration products.

  17. Agricultural Fires in the Southeastern U.S. During SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol

    Science.gov (United States)

    Liu, X.; Zhang, Y.; Huey, L. G.; Yokelson, R. J.; Wang, Y.; Jimenez, J. L.; Campuzano-Jost, P.; Beyersdorf, A. J.; Blake, D. R.; Choi, Y.; hide

    2016-01-01

    Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for 1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with (Delta)O3/(Delta)CO, (Delta)PAN/(Delta)NOy, and (Delta)nitrate/(Delta)NOy reaching approx. 0.1, approx. 0.3, and approx.0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of approx. 2) to be equivalent to approx. 2% SO2 from coal combustion and approx. 1% NOx and approx. 9% CO from mobile sources.

  18. Secondary aerosols from power plant effluents: delivery and in vivo detection systems

    International Nuclear Information System (INIS)

    Parks, N.J.; Raabe, O.G.; Bradley, E.; Raub, J.

    1976-01-01

    An experimental system is described for the generation of radiolabeled monodisperse aerosols, which are physico-chemically analogous to aerosols produced as secondary products of gaseous fossil fuel power plant emissions of SO 2 and NO 2 . The experimental system for inhalation exposure of non-human primates to these particles and the in vivo determination of systemic distribution and target organs is discussed

  19. Impact of increasing ship emissions on air quality and deposition over Europe by 2030

    Energy Technology Data Exchange (ETDEWEB)

    Collins, Bill; Sanderson, Michael G.; Johnson, Colin E. [Met Office Hadley Centre for Climate Change, Exeter (United Kingdom)

    2009-07-01

    A global chemistry-transport model has been used to study the effect of shipping emissions on air quality and ecosystems over Europe, through changes in surface ozone and surface sulphate aerosols, and changes in the deposition of sulphur and oxidised nitrogen. Scenarios are chosen to determine the impact of current (2000) shipping emissions, and the combined impact of changes in land-based and shipping emissions by 2030. The effects of shipping on ozone are small, compared to land-based emissions changes, and can be both positive and negative. Due to the non-linear nature of ozone chemistry, the effects of shipping depend on the magnitude of the emission change, and on the choice of scenario for the land-based emissions. The effects on sulphate aerosol levels and deposition fluxes of sulphate aerosols and oxidised nitrogen species are larger, and are comparable to expected changes in land-based emissions. This is particularly true for SO{sub 2} emissions from shipping. SO{sub 2} has a sufficiently short lifetime that most of the impacts are felt within the European region, although much of that is over the sea. The increase in sulphate aerosols and sulphur deposition due to the SO{sub 2} from shipping will offset 75 % of the benefits in air quality that would be expect from land-based emission controls under the SRES A2 scenario. (orig.)

  20. Carbonaceous aerosol particles from common vegetation in the Grand Canyon

    International Nuclear Information System (INIS)

    Hallock, K.A.; Mazurek, M.A.; Cass, G.R.

    1992-05-01

    The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon

  1. Black Carbon and Sulfate Aerosols in the Arctic: Long-term Trends, Radiative Impacts, and Source Attributions

    Science.gov (United States)

    Wang, H.; Zhang, R.; Yang, Y.; Smith, S.; Rasch, P. J.

    2017-12-01

    The Arctic has warmed dramatically in recent decades. As one of the important short-lived climate forcers, aerosols affect the Arctic radiative budget directly by interfering radiation and indirectly by modifying clouds. Light-absorbing particles (e.g., black carbon) in snow/ice can reduce the surface albedo. The direct radiative impact of aerosols on the Arctic climate can be either warming or cooling, depending on their composition and location, which can further alter the poleward heat transport. Anthropogenic emissions, especially, BC and SO2, have changed drastically in low/mid-latitude source regions in the past few decades. Arctic surface observations at some locations show that BC and sulfate aerosols had a decreasing trend in the recent decades. In order to understand the impact of long-term emission changes on aerosols and their radiative effects, we use the Community Earth System Model (CESM) equipped with an explicit BC and sulfur source-tagging technique to quantify the source-receptor relationships and decadal trends of Arctic sulfate and BC and to identify variations in their atmospheric transport pathways from lower latitudes. The simulation was conducted for 36 years (1979-2014) with prescribed sea surface temperatures and sea ice concentrations. To minimize potential biases in modeled large-scale circulations, wind fields in the simulation are nudged toward an atmospheric reanalysis dataset, while atmospheric constituents including water vapor, clouds, and aerosols are allowed to evolve according to the model physics. Both anthropogenic and open fire emissions came from the newly released CMIP6 datasets, which show strong regional trends in BC and SO2 emissions during the simulation time period. Results show that emissions from East Asia and South Asia together have the largest contributions to Arctic sulfate and BC concentrations in the upper troposphere, which have an increasing trend. The strong decrease in emissions from Europe, Russia and

  2. The effect of regional changes in anthropogenic aerosols on rainfall of the East Asian Summer Monsoon

    Directory of Open Access Journals (Sweden)

    L. Guo

    2013-02-01

    Full Text Available The response of East Asian Summer Monsoon (EASM precipitation to long term changes in regional anthropogenic aerosols (sulphate and black carbon is explored in an atmospheric general circulation model, the atmospheric component of the UK High-Resolution Global Environment Model v1.2 (HiGAM. Separately, sulphur dioxide (SO2 and black carbon (BC emissions in 1950 and 2000 over East Asia are used to drive model simulations, while emissions are kept constant at year 2000 level outside this region. The response of the EASM is examined by comparing simulations driven by aerosol emissions representative of 1950 and 2000. The aerosol radiative effects are also determined using an off-line radiative transfer model. During June, July and August, the EASM was not significantly changed as either SO2 or BC emissions increased from 1950 to 2000 levels. However, in September, precipitation is significantly decreased by 26.4% for sulphate aerosol and 14.6% for black carbon when emissions are at the 2000 level. Over 80% of the decrease is attributed to changes in convective precipitation. The cooler land surface temperature over China in September (0.8 °C for sulphate and 0.5 °C for black carbon due to increased aerosols reduces the surface thermal contrast that supports the EASM circulation. However, mechanisms causing the surface temperature decrease in September are different between sulphate and BC experiments. In the sulphate experiment, the sulphate direct and the 1st indirect radiative effects contribute to the surface cooling. In the BC experiment, the BC direct effect is the main driver of the surface cooling, however, a decrease in low cloud cover due to the increased heating by BC absorption partially counteracts the direct effect. This results in a weaker land surface temperature response to BC changes than to sulphate changes. The resulting precipitation response is also weaker, and the responses of the monsoon circulation

  3. Real-Time Observations of Secondary Aerosol Formation and Aging from Different Emission Sources and Environments

    Science.gov (United States)

    Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Rappenglueck, B.; Bon, D.; Graus, M.; Warneke, C.; Gilman, J.; Kuster, W.; De Gouw, J. A.; Jimenez, J. L.

    2013-12-01

    To investigate atmospheric processing of direct urban and wildfire emissions, we deployed a photochemical flow reactor (Potential Aerosol Mass, PAM) with submicron aerosol size and chemical composition measurements during FLAME-3, a biomass-burning study at USDA Fire Sciences Laboratory in Missoula, MT, and CalNex, a field study investigating the nexus of air quality and climate change at a receptor site in the LA-Basin at Pasadena, CA. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent aging of ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min in both field studies. Results show the value of this approach as a tool for in-situ evaluation of changes in OA concentration and composition due to photochemical processing. In FLAME-3, the average OA enhancement factor was 1.42 × 0.36 of the initial POA. Reactive VOCs, such as toluene, monoterpenes, and acetaldehyde, decreased with increased OHexp; however, formic acid, acetone, and some unidentified OVOCs increased after significant exposure. Net SOA formation in the photochemical reactor increased with OHexp, typically peaking around 3 days of equivalent atmospheric photochemical age (OHexp ~3.9e11 molecules cm-3 s), then leveling off at higher exposures. Unlike other studies, no decrease in OA is observed at high exposure, likely due to lower max OHexp in this study due to very high OH reactivity. The amount of additional OA mass added from aging is positively correlated with initial POA concentration, but not with the total VOC concentration or the concentration of known SOA precursors. The mass of SOA formed often exceeded the mass of the known VOC precursors, indicating the likely importance of primary semivolatile/intermediate volatility species, and possibly of unidentified VOCs as SOA precursors in biomass burning smoke. Results from CalNex show enhancement of OA and inorganic aerosol from gas-phase precursors

  4. Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

    Directory of Open Access Journals (Sweden)

    Y. Wang

    2013-03-01

    Full Text Available We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3 from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC and Sichuan Basin (SCB, while nitrate and sulfate contribute equally over North China (NC. Based on emission reduction targets in the 12th (2011–2015 Five-Year Plan (FYP, China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

  5. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    Science.gov (United States)

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-06

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  6. Nuclear microprobe analysis and source apportionment of individual atmospheric aerosol particles

    International Nuclear Information System (INIS)

    Artaxo, P.; Rabello, M.L.C.; Watt, F.; Grime, G.; Swietlicki, E.

    1993-01-01

    In atmospheric aerosol reserach, one key issue is to determine the sources of the airborne particles. Bulk PIXE analysis coupled with receptor modeling provides a useful, but limited view of the aerosol sources influencing one particular site or sample. The scanning nuclear microprobe (SNM) technique is a microanalytical technique that gives unique information on individual aerosol particles. In the SNM analyses a 1.0 μm size 2.4 MeV proton beam from the Oxford SNM was used. The trace elements with Z>11 were measured by the particle induced X-ray emission (PIXE) method with detection limits in the 1-10 ppm range. Carbon, nitrogen and oxygen are measured simultaneously using Rutherford backscattering spectrometry (RBS). Atmospheric aerosol particles were collected at the Brazilian Antarctic Station and at biomass burning sites in the Amazon basin tropical rain forest in Brazil. In the Antarctic samples, the sea-salt aerosol particles were clearly predominating, with NaCl and CaSO 4 as major compounds with several trace elements as Al, Si, P, K, Mn, Fe, Ni, Cu, Zn, Br, Sr, and Pb. Factor analysis of the elemental data showed the presence of four components: 1) Soil dust particles; 2) NaCl particles; 3) CaSO 4 with Sr; and 4) Br and Mg. Strontium, observed at 20-100 ppm levels, was always present in the CaSO 4 particles. The hierarchical cluster procedure gave results similar to the ones obtained through factor analysis. For the tropical rain forest biomass burning aerosol emissions, biogenic particles with a high organic content dominate the particle population, while K, P, Ca, Mg, Zn, and Si are the dominant elements. Zinc at 10-200 ppm is present in biogenic particles rich in P and K. The quantitative aspects and excellent detection limits make SNM analysis of individual aerosol particles a very powerful analytical tool. (orig.)

  7. Sources and composition of urban aerosol particles

    Science.gov (United States)

    Vogt, M.; Johansson, C.; Mårtensson, M.; Struthers, H.; Ahlm, L.; Nilsson, D.

    2011-09-01

    From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp) from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass removed at 0.6 μm Dp. Further heating to 300 °C caused very little additional losses road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles <0.6 μm Dp to be 2.4±1.4 mg veh-1 km-1 based on either CO2 fluxes or traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and reveal that for non-volatile particulate matter in the 0.25 to 0.6 μm Dp range, the EFHDV is approximately twice as high as the EFLDV, the difference not being statistically significant.

  8. Potential influence of inter-continental transport of sulfate aerosols on air quality

    International Nuclear Information System (INIS)

    Liu Junfeng; Mauzerall, Denise L

    2007-01-01

    In this study, we compare the potential influence of inter-continental transport of sulfate aerosols on the air quality of (different) continental regions. We use a global chemical transport model, Model of Ozone and Related Tracers, version 2 (MOZART-2), to quantify the source-receptor relationships of inter-continental transport of sulfate aerosols among ten regions in 2000. In order to compare the importance of foreign with domestic emissions and to estimate the effect of future changes in emissions on human exposure, we define an 'influence potential' (IP). The IP quantifies the human exposure that occurs in a receptor region as a result of a unit of SO 2 emissions from a source region. We find that due to the non-linear nature of sulfate production, regions with low SO 2 emissions usually have large domestic IP, and vice versa. An exception is East Asia (EA), which has both high SO 2 emissions and relatively large domestic IP, mostly caused by the spatial coincidence of emissions and population. We find that inter-continental IPs are usually less than domestic IPs by 1-3 orders of magnitude. SO 2 emissions from the Middle East (ME) and Europe (EU) have the largest potential to influence populations in surrounding regions. By comparing the IP ratios (IPR) between foreign and domestic SO 2 emissions, we find that the IPR values range from 0.000 01 to 0.16 and change with season. Therefore, if reducing human exposure to sulfate aerosols is the objective, all regions should first focus on reducing domestic SO 2 emissions. In addition, we find that relatively high IPR values exist among the EU, ME, the former Soviet Union (FSU) and African (AF) regions. Therefore, on the basis of the IP and IPR values, we conclude that a regional agreement among EA countries, and an inter-regional agreement among EU, ME, FSU and (north) AF regions to control sulfur emissions could benefit public health in these regions

  9. Response of northern hemisphere environmental and atmospheric conditions to climate changes using Greenland aerosol records from the Eemian to the Holocene

    Science.gov (United States)

    Fischer, H.

    2017-12-01

    The Northern Hemisphere experienced dramatic climate changes over the last glacial cycle, including vast ice sheet expansion and frequent abrupt climate events. Moreover, high northern latitudes during the last interglacial (Eemian) were warmer than today and may provide guidance for future climate change scenarios. However, little evidence exists regarding the environmental alterations connected to these climate changes. Using aerosol concentration records in decadal resolution from the North Greenland Eemian Ice Drilling (NEEM) over the last 128,000 years we extract quantitative information on environmental changes, including the first comparison of northern hemisphere environmental conditions between the warmer than present Eemian and the early Holocene. Separating source changes from transport effects, we find that changes in the ice concentration greatly overestimate the changes in atmospheric concentrations in the aerosol source region, the latter mirroring changes in aerosol emissions. Glacial times were characterized by a strong reduction in terrestrial biogenic emissions (only 10-20% of the early Holocene value) reflecting the net loss of vegetated area in mid to high latitudes, while rapid climate changes during the glacial had essentially no effect on terrestrial biogenic aerosol emissions. An increase in terrestrial dust emissions of approximately a factor of eight during peak glacial and cold stadial intervals indicates higher aridity and dust storm activity in Asian deserts. Glacial sea salt aerosol emissions increased only moderately (by approximately 50%), likely due to sea ice expansion, while marked stadial/interstadial variations in sea salt concentrations in the ice reflect mainly changes in wet deposition en route. Eemian ice contains lower aerosol concentrations than ice from the early Holocene, due to shortened atmospheric residence time during the warmer Eemian, suggesting that generally 2°C warmer climate in high northern latitudes did not

  10. Comparisons of Airborne HSRL and Modeled Aerosol Profiles

    Science.gov (United States)

    Ferrare, R. A.; Burton, S. P.; Hostetler, C. A.; Hair, J. W.; Ismail, S.; Rogers, R. R.; Notari, A.; Berkoff, T.; Butler, C. F.; Collins, J. E., Jr.; Fenn, M. A.; Scarino, A. J.; Clayton, M.; Mueller, D.; Chemyakin, E.; Fast, J. D.; Berg, L. K.; Randles, C. A.; Colarco, P. R.; daSilva, A.

    2014-12-01

    Aerosol profiles derived from a regional and a global model are compared with aerosol profiles acquired by NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidars (HSRLs) during recent field missions. We compare simulated aerosol profiles obtained from the WRF-Chem regional model with those measured by the airborne HSRL-2 instrument over the Atlantic Ocean east of Cape Cod in July 2012 during the Department of Energy Two-Column Aerosol Project (TCAP). While deployed on the LaRC King Air during TCAP, HSRL-2 acquired profiles of aerosol extinction at 355 and 532 nm, as well as aerosol backscatter and depolarization at 355, 532, and 1064 nm. Additional HSRL-2 data products include profiles of aerosol type, mixed layer depth, and aerosol microphysical parameters (e.g. effective radius, concentration). The HSRL-2 and WRF-Chem aerosol profiles are compared along the aircraft flight tracks. HSRL-2 profiles acquired during the NASA Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission over Houston during September 2013 are compared with the NASA Goddard Earth Observing System global model, version 5 (GEOS-5) profiles. In addition to comparing backscatter and extinction profiles, the fraction of aerosol extinction and optical thickness from various aerosol species from GEOS-5 are compared with aerosol extinction and optical thickness contributed by aerosol types derived from HSRL-2 data. We also compare aerosol profiles modeled by GEOS-5 with those measured by the airborne LaRC DIAL/HSRL instrument during August and September 2013 when it was deployed on the NASA DC-8 for the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) mission. DIAL/HSRL measured extinction (532 nm), backscatter (532 and 1064 nm), and depolarization profiles (532 and 1064 nm) in both nadir and zenith directions during long transects over the

  11. AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

    Science.gov (United States)

    Provencal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

    2017-01-01

    NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

  12. Model studies of the effect of aerosol wastewater emissions on terrestrial mollusks Achatina fulica

    Directory of Open Access Journals (Sweden)

    Kamardin Nikolaj Nikolaevich

    2016-12-01

    Full Text Available The laboratory experiments were carried on using the juvenile mollusk Achatina fulica as a bioindicator of soil contamination and air pollution. It is shown that when experimental animals breathed and had dermal contact with the aerosols prepared from the wastewater and those prepared from two solutions of Ni in distilled water at two concentrations they weighed significantly less than controls . According to the results of AAS, heavy metals (HM, in particular Cd, Cu, Ni of sewage accumulated in the digestive gland of the shell. In model experiments mollusks were contained in the chamber periodically (2 hours of input and 2 hours of pause filled with aerosol containing Ni at concentrations of 30 and 50 mg / dm3 nickel for two weeks It resulted in accumulation of Ni in the digestive gland of mollusks with concentrations 6 to 10 times exceeding controls, respectively. At that the experimental animals gained weight reliably slower than the controls contained in aquatic aerosol without Ni. The subsequent one week exposure of shells in aerosol, prepared from the distilled water without Ni reduced the concentration of nickel in the tissue of the digestive gland. Thus, bioavailability of HM and nickel solutions prepared from untreated wastewaters in breathing aerosol and possibly by skin contact was demonstrated. The toxicant delivery seems to occur apart from food intake.

  13. Organic aerosol formation in citronella candle plumes.

    Science.gov (United States)

    Bothe, Melanie; Donahue, Neil McPherson

    2010-09-01

    Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In repeated experiments, we observed rapid and substantial SOA formation after ozone addition; this process must therefore be considered when assessing the risks and benefits of using citronella candle to repel insects.

  14. C1-C2 alkyl aminiums in urban aerosols: Insights from ambient and fuel combustion emission measurements in the Yangtze River Delta region of China

    International Nuclear Information System (INIS)

    Shen, Wenchao; Ren, Lili; Zhao, Yi; Zhou, Luyu; Dai, Liang; Ge, Xinlei; Kong, Shaofei; Yan, Qin; Xu, Honghui; Jiang, Yujun; He, Jun; Chen, Mindong; Yu, Huan

    2017-01-01

    We measured low molar-mass alkyl aminiums (methylaminium, dimethylaminium, ethylaminium and diethylaminium) in urban aerosols in the Yangtze River Delta region of eastern China in August 2014 and from November 2015 to May 2016. After examining artifact formation on sample filters, methylaminium, dimethylaminium and ethylaminium concentrations were quantified. The three C1-C2 aminiums exhibited a unimodal size distribution that maximized between 0.56 and 1.0 μm. Their concentrations in PM 2.5 were 5.7 ± 3.2 ng m −3 , 7.9 ± 5.4 ng m −3 and 20.3 ± 16.6 ng m −3 , respectively, with higher concentrations during the daytime and in warm seasons. On new particle growth days, amine uptake to particles larger than 56 nm was barely enhanced. The molar ratios of individual aminium/NH 4 + in PM 2.5 were on the order of 10 −4 and 10 −3 . Aminiums were thus far less to out-compete ammonium (NH 4 + ) in neutralizing acidic species in particle sizes down to 56 nm. Abundant nitrate (NO 3 − /SO 4 2− molar ratio = ∼3) and its correlation to methylaminium and ethylaminium implied that nitrate might be more important aminium salt than sulfate in urban aerosols of this area. Direct measurement of particle-phase amine emission from coal and biomass burning showed that coal burning is an important atmospheric amine source, considering coal burning is top-ranked particulate matter source in China. - Highlights: • Aminium concentration showed seasonal and diurnal variations in urban aerosols of our area. • Nitrate was more important aminium salt than sulfate in urban aerosols of our area. • Particle-phase amine emission from coal burning is an important atmospheric amine source. • Amine uptake to particles larger than 56 nm was barely enhanced on new particle growth events. • Aminiums cannot out-compete ammonium in neutralizing acidic species in urban aerosols with particle sizes down to 56 nm. - Aminiums cannot out-compete ammonium in

  15. An Investigation of Aerosol Scattering and Absorption Properties in Wuhan, Central China

    Directory of Open Access Journals (Sweden)

    Wei Gong

    2015-04-01

    Full Text Available Aerosol scattering and absorption properties were continuously measured and analyzed at the urban Laboratory for Information Engineering in Surveying, Mapping and Remote Sensing (LIESMARS site in Wuhan, central China, from 1 December 2009 to 31 March 2014. The mean aerosol scattering coefficient , absorption coefficient , and single scattering albedo (SSA were 377.54 Mm−1, 119.06 Mm−1, and 0.73, respectively. Both  and  showed obvious annual variability with large values in winter and small values in summer, principally caused by the annual characteristics of meteorological conditions, especially planetary boundary layer height (PBLH and local emissions. The SSA showed a slight annual variation. High values of SSA were related to formation of secondary aerosols in winter hazes and aerosol hygroscopic growth in humid summer. The large SSA in June can be attributed to the biomass combustion in Hubei and surrounding provinces. Both  and  showed double peak phenomena in diurnal variation resulting from the shallow stable PBLH at night and automobile exhaust emission during morning rush hours. The SSA also exhibited a double peak phenomenon related to the proportional variation of black carbon (BC and light scattering particulates in the day and night. The long-term exploration on quantified aerosol optical properties can help offer scientific basis of introducing timely environmental policies for local government.

  16. Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

    Science.gov (United States)

    Zhang, Yan-Lin; El-Haddad, Imad; Huang, Ru-Jin; Ho, Kin-Fai; Cao, Jun-Ji; Han, Yongming; Zotter, Peter; Bozzetti, Carlo; Daellenbach, Kaspar R.; Slowik, Jay G.; Salazar, Gary; Prévôt, André S. H.; Szidat, Sönke

    2018-03-01

    Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32-47 % of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 %) and Xi'an (26 ± 9 %). The most important primary sources were biomass burning emissions, contributing 17-26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban and background regions in Asia, Europe and the USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 %) to WSOC aerosols in the Northern Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the eastern Asian pollution outflow, especially during winter, due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

  17. Biomass burning aerosol transport and vertical distribution over the South African-Atlantic region: Aerosol Transport Over SE Atlantic

    Energy Technology Data Exchange (ETDEWEB)

    Das, Sampa [Department of Earth, Atmospheric and Planetary Sciences, Purdue University, West Lafayette Indiana USA; Harshvardhan, H. [Department of Earth, Atmospheric and Planetary Sciences, Purdue University, West Lafayette Indiana USA; Bian, Huisheng [Joint Center for Earth Systems Technology, UMBC, Baltimore Maryland USA; NASA Goddard Space Flight Center, Greenbelt Maryland USA; Chin, Mian [NASA Goddard Space Flight Center, Greenbelt Maryland USA; Curci, Gabriele [Department of Physical and Chemical Sciences, University of L' Aquila, L' Aquila Italy; Center of Excellence in Telesensing of Environment and Model Prediction of Severe events, University of L' Aquila, L' Aquila Italy; Protonotariou, Anna P. [Department of Physics, University of Athens, Athens Greece; Mielonen, Tero [Finnish Meteorological Institute, Kuopio Finland; Zhang, Kai [Pacific Northwest National Laboratory, Richland Washington USA; Wang, Hailong [Pacific Northwest National Laboratory, Richland Washington USA; Liu, Xiaohong [Department of Atmospheric Science, University of Wyoming, Laramie Wyoming USA

    2017-06-21

    Aerosols from wild-land fires could significantly perturb the global radiation balance and induce the climate change. In this study, the Community Atmospheric Model version 5 (CAM5) with prescribed daily fire aerosol emissions is used to investigate the spatial and seasonal characteristics of radiative forcings of wildfire aerosols including black carbon (BC) and particulate organic matter (POM). The global annual mean direct radiative forcing (DRF) of all fire aerosols is 0.15 W m-2, mainly due to the absorption of fire BC (0.25 W m-2), while fire POM induces a weak negative forcing (-0.05 W m-2). Strong positive DRF is found in the Arctic and in the oceanic regions west of South Africa and South America as a result of amplified absorption of fire BC above low-level clouds, in general agreement with satellite observations. The global annual mean cloud radiative forcing due to all fire aerosols is -0.70 W m-2, resulting mainly from the fire POM indirect forcing (-0.59 W m-2). The large cloud liquid water path over land areas of the Arctic favors the strong fire aerosol indirect forcing (up to -15 W m-2) during the Arctic summer. Significant surface cooling, precipitation reduction and low-level cloud amount increase are also found in the Arctic summer as a result of the fire aerosol indirect effect. The global annual mean surface albedo forcing over land areas (0.03 W m-2) is mainly due to the fire BC-on-snow forcing (0.02 W m-2) with the maximum albedo forcing occurring in spring (0.12 W m-2) when snow starts to melt.

  18. Aerosol indirect effect on tropospheric ozone via lightning

    Science.gov (United States)

    Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

    2012-12-01

    Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications

  19. Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget

    Directory of Open Access Journals (Sweden)

    A. Lauer

    2007-10-01

    Full Text Available International shipping contributes significantly to the fuel consumption of all transport related activities. Specific emissions of pollutants such as sulfur dioxide (SO2 per kg of fuel emitted are higher than for road transport or aviation. Besides gaseous pollutants, ships also emit various types of particulate matter. The aerosol impacts the Earth's radiation budget directly by scattering and absorbing the solar and thermal radiation and indirectly by changing cloud properties. Here we use ECHAM5/MESSy1-MADE, a global climate model with detailed aerosol and cloud microphysics to study the climate impacts of international shipping. The simulations show that emissions from ships significantly increase the cloud droplet number concentration of low marine water clouds by up to 5% to 30% depending on the ship emission inventory and the geographic region. Whereas the cloud liquid water content remains nearly unchanged in these simulations, effective radii of cloud droplets decrease, leading to cloud optical thickness increase of up to 5–10%. The sensitivity of the results is estimated by using three different emission inventories for present-day conditions. The sensitivity analysis reveals that shipping contributes to 2.3% to 3.6% of the total sulfate burden and 0.4% to 1.4% to the total black carbon burden in the year 2000 on the global mean. In addition to changes in aerosol chemical composition, shipping increases the aerosol number concentration, e.g. up to 25% in the size range of the accumulation mode (typically >0.1 μm over the Atlantic. The total aerosol optical thickness over the Indian Ocean, the Gulf of Mexico and the Northeastern Pacific increases by up to 8–10% depending on the emission inventory. Changes in aerosol optical thickness caused by shipping induced modification of aerosol particle number concentration and chemical composition lead to a change in the shortwave radiation budget at the top of the

  20. Investigating the Linear Dependence of Direct and Indirect Radiative Forcing on Emission of Carbonaceous Aerosols in a Global Climate Model

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Yanju [Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana IL USA; Wang, Hailong [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Singh, Balwinder [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Ma, Po-Lun [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Rasch, Philip J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Bond, Tami C. [Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana IL USA

    2018-02-02

    The linearity of dependence of aerosol direct and indirect radiative forcing (DRF and IRF) on emissions is essential to answer the policy-relevant question on how the change in forcing would result from a change in emission. In this study, the forcing-to-emission relationship is investigated for black carbon (BC) and primary organic carbon (OC) emitted from North America and Asia. Direct and indirect radiative forcing of BC and OC are simulated with the Community Atmosphere Model (CAM5.1). Two diagnostics are introduced to aid in policy-relevant discussion: emission-normalized forcing (ENF) and linearity (R). DRF is linearly related to emission for both BC and OC from the two regions and emission-normalized DRF is similar, within 15%. IRF is linear to emissions for weaker sources and regions far from source (North American BC and OC), while for large emission sources and near source regions (Asian OC) the response of forcing to emission is sub-linear. In North America emission-normalized IRF (ENIRF) is 2-4 times higher than that in Asia. The difference among regions and species is primarily caused by failure of accumulation mode particles to become CCN, and then to activate into CDNC. Optimal aggregation area (30ºx 30º) has been used to communicate the regional variation of forcing-to-emission relationship. For IRF, only 15-40% of the Earth’s surface is significantly affected by the two emission regions, but the forcing in these regions comprises most of the global impact. Linearity of IRF occurs in about two-thirds of the significant regions except for Asian OC. ENF is an effective tool to estimate forcing changes due to reduction of surface emissions, as long as there is sufficient attention to the causes of nonlinearity in the simulations used to derive ENIRF (emission into polluted regions and emission elevation). The differences in ENIRF have important implications for policy decisions. Lower ENIRF in more polluted region like Asia means that reductions of

  1. Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

    Science.gov (United States)

    Dreyfus, Matthew A.

    Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

  2. Present and potential future contributions of sulfate, black and organic carbon aerosols from China to global air quality, premature mortality and radiative forcing

    Science.gov (United States)

    Saikawa, Eri; Naik, Vaishali; Horowitz, Larry W.; Liu, Junfeng; Mauzerall, Denise L.

    Aerosols are harmful to human health and have both direct and indirect effects on climate. China is a major contributor to global emissions of sulfur dioxide (SO 2), a sulfate (SO 42-) precursor, organic carbon (OC), and black carbon (BC) aerosols. Although increasingly examined, the effect of present and potential future levels of these emissions on global premature mortality and climate change has not been well quantified. Through both direct radiative effects and indirect effects on clouds, SO 42- and OC exert negative radiative forcing (cooling) while BC exerts positive forcing (warming). We analyze the effect of China's emissions of SO 2, SO 42-, OC and BC in 2000 and for three emission scenarios in 2030 on global surface aerosol concentrations, premature mortality, and radiative forcing (RF). Using global models of chemical transport (MOZART-2) and radiative transfer (GFDL RTM), and combining simulation results with gridded population data, mortality rates, and concentration-response relationships from the epidemiological literature, we estimate the contribution of Chinese aerosols to global annual premature mortality and to RF in 2000 and 2030. In 2000, we estimate these aerosols cause approximately 470 000 premature deaths in China and an additional 30 000 deaths globally. In 2030, aggressive emission controls lead to a 50% reduction in premature deaths from the 2000 level to 240 000 in China and 10 000 elsewhere, while under a high emissions scenario premature deaths increase 50% from the 2000 level to 720 000 in China and to 40 000 elsewhere. Because the negative RF from SO 42- and OC is larger than the positive forcing from BC, Chinese aerosols lead to global net direct RF of -74 mW m -2 in 2000 and between -15 and -97 mW m -2 in 2030 depending on the emissions scenario. Our analysis indicates that increased effort to reduce greenhouse gases is essential to address climate change as China's anticipated reduction of aerosols will result in the

  3. Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: impact of anthropogenic sources.

    Science.gov (United States)

    Ram, Kirpa; Sarin, M M

    2015-01-15

    In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20-70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO4(2-), and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale. Copyright © 2014 Elsevier Ltd. All rights reserved.

  4. The Influence of Air-Sea Fluxes on Atmospheric Aerosols During the Summer Monsoon Over the Tropical Indian Ocean

    Science.gov (United States)

    Zavarsky, Alex; Booge, Dennis; Fiehn, Alina; Krüger, Kirstin; Atlas, Elliot; Marandino, Christa

    2018-01-01

    During the summer monsoon, the western tropical Indian Ocean is predicted to be a hot spot for dimethylsulfide emissions, the major marine sulfur source to the atmosphere, and an important aerosol precursor. Other aerosol relevant fluxes, such as isoprene and sea spray, should also be enhanced, due to the steady strong winds during the monsoon. Marine air masses dominate the area during the summer monsoon, excluding the influence of continentally derived pollutants. During the SO234-2/235 cruise in the western tropical Indian Ocean from July to August 2014, directly measured eddy covariance DMS fluxes confirm that the area is a large source of sulfur to the atmosphere (cruise average 9.1 μmol m-2 d-1). The directly measured fluxes, as well as computed isoprene and sea spray fluxes, were combined with FLEXPART backward and forward trajectories to track the emissions in space and time. The fluxes show a significant positive correlation with aerosol data from the Terra and Suomi-NPP satellites, indicating a local influence of marine emissions on atmospheric aerosol numbers.

  5. GEM-AQ/EC, an on-line global multi-scale chemical weather modelling system: model development and evaluation of global aerosol climatology

    Directory of Open Access Journals (Sweden)

    S. L. Gong

    2012-09-01

    Full Text Available A global air quality modeling system GEM-AQ/EC was developed by implementing tropospheric chemistry and aerosol processes on-line into the Global Environmental Multiscale weather prediction model – GEM. Due to the multi-scale features of the GEM, the integrated model, GEM-AQ/EC, is able to investigate chemical weather at scales from global to urban domains. The current chemical mechanism is comprised of 50 gas-phase species, 116 chemical and 19 photolysis reactions, and is complemented by a sectional aerosol module CAM (The Canadian Aerosol Module with 5 aerosols types: sulphate, black carbon, organic carbon, sea-salt and soil dust. Monthly emission inventories of black carbon and organic carbon from boreal and temperate vegetation fires were assembled using the most reliable areas burned datasets by countries, from statistical databases and derived from remote sensing products of 1995–2004. The model was run for ten years from from 1995–2004 with re-analyzed meteorology on a global uniform 1° × 1° horizontal resolution domain and 28 hybrid levels extending up to 10 hPa. The simulating results were compared with various observations including surface network around the globe and satellite data. Regional features of global aerosols are reasonably captured including emission, surface concentrations and aerosol optical depth. For various types of aerosols, satisfactory correlations were achieved between modeled and observed with some degree of systematic bias possibly due to large uncertainties in the emissions used in this study. A global distribution of natural aerosol contributions to the total aerosols is obtained and compared with observations.

  6. Aerosol transport model evaluation of an extreme smoke episode in Southeast Asia

    Science.gov (United States)

    Hyer, Edward J.; Chew, Boon Ning

    2010-04-01

    Biomass burning is one of many sources of particulate pollution in Southeast Asia, but its irregular spatial and temporal patterns mean that large episodes can cause acute air quality problems in urban areas. Fires in Sumatra and Borneo during September and October 2006 contributed to 24-h mean PM 10 concentrations above 150 μg m -3 at multiple locations in Singapore and Malaysia over several days. We use the FLAMBE model of biomass burning emissions and the NAAPS model of aerosol transport and evolution to simulate these events, and compare our simulation results to 24-h average PM 10 measurements from 54 stations in Singapore and Malaysia. The model simulation, including the FLAMBE smoke source as well as dust, sulfate, and sea salt aerosol species, was able to explain 50% or more of the variance in 24-h PM 10 observations at 29 of 54 sites. Simulation results indicated that biomass burning smoke contributed to nearly all of the extreme PM 10 observations during September-November 2006, but the exact contribution of smoke was unclear because the model severely underestimated total smoke emissions. Using regression analysis at each site, the bias in the smoke aerosol flux was determined to be a factor of between 2.5 and 10, and an overall factor of 3.5 was estimated. After application of this factor, the simulated smoke aerosol concentration averaged 20% of observed PM 10, and 40% of PM 10 for days with 24-h average concentrations above 150 μg m -3. These results suggest that aerosol transport models can aid analysis of severe pollution events in Southeast Asia, but that improvements are needed in models of biomass burning smoke emissions.

  7. Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

    Science.gov (United States)

    Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

    2012-11-01

    Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish

  8. On the relationship between aerosol model uncertainty and radiative forcing uncertainty.

    Science.gov (United States)

    Lee, Lindsay A; Reddington, Carly L; Carslaw, Kenneth S

    2016-05-24

    The largest uncertainty in the historical radiative forcing of climate is caused by the interaction of aerosols with clouds. Historical forcing is not a directly measurable quantity, so reliable assessments depend on the development of global models of aerosols and clouds that are well constrained by observations. However, there has been no systematic assessment of how reduction in the uncertainty of global aerosol models will feed through to the uncertainty in the predicted forcing. We use a global model perturbed parameter ensemble to show that tight observational constraint of aerosol concentrations in the model has a relatively small effect on the aerosol-related uncertainty in the calculated forcing between preindustrial and present-day periods. One factor is the low sensitivity of present-day aerosol to natural emissions that determine the preindustrial aerosol state. However, the major cause of the weak constraint is that the full uncertainty space of the model generates a large number of model variants that are equally acceptable compared to present-day aerosol observations. The narrow range of aerosol concentrations in the observationally constrained model gives the impression of low aerosol model uncertainty. However, these multiple "equifinal" models predict a wide range of forcings. To make progress, we need to develop a much deeper understanding of model uncertainty and ways to use observations to constrain it. Equifinality in the aerosol model means that tuning of a small number of model processes to achieve model-observation agreement could give a misleading impression of model robustness.

  9. Improved attribution of climate forcing to emissions by pollutant and sector

    Science.gov (United States)

    Shindell, D. T.

    2009-12-01

    Evaluating multi-component climate change mitigation strategies requires knowledge of the diverse direct and indirect effects of emissions. Methane, ozone and aerosols are linked through atmospheric chemistry so that emissions of a single pollutant can affect several species. I will show new calculations of atmospheric composition changes, radiative forcing, and the global warming potential (GWP) for increased emissions of tropospheric ozone and aerosol precursors in a coupled composition-climate model. The results demonstrate that gas-aerosol interactions substantially alter the relative importance of the various emissions, suggesting revisions to the GWPs used in international carbon trading. Additionally, I will present results showing how the net climate impact of particular activities depends strongly upon non-CO2 forcing agents for some sectors. These results will be highlighted by discussing the interplay between air quality emissions controls and climate for the case of emissions from coal-fired power plants. The changing balance between CO2 and air quality pollutants from coal plants may have contributed to the 20th century spatial and temporal patterns of climate change, and is likely to continue to do so as more and more plants are constructed in Asia.

  10. Formation of the natural sulfate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kerminen, V M; Hillamo, R; Maekinen, M; Virkkula, A; Maekelae, T; Pakkanen, T [Helsinki Univ. (Finland). Dept. of Physics

    1997-12-31

    Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

  11. Formation of the natural sulfate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

    1996-12-31

    Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

  12. Development of the Multi-Angle Stratospheric Aerosol Radiometer (MASTAR) Instrument

    Science.gov (United States)

    DeLand, M. T.; Colarco, P. R.; Kowalewski, M. G.; Gorkavyi, N.; Ramos-Izquierdo, L.

    2017-12-01

    Aerosol particles in the stratosphere ( 15-25 km altitude), both produced naturally and perturbed by volcanic eruptions and anthropogenic emissions, continue to be a source of significant uncertainty in the Earth's energy budget. Stratospheric aerosols can offset some of the warming effects caused by greenhouse gases. These aerosols are currently monitored using measurements from the Ozone Mapping and Profiling Suite (OMPS) Limb Profiler (LP) instrument on the Suomi NPP satellite. In order to improve the sensitivity and spatial coverage of these aerosol data, we are developing an aerosol-focused compact version of the OMPS LP sensor called Multi-Angle Stratospheric Aerosol Radiometer (MASTAR) to fly on a 3U Cubesat satellite, using a NASA Instrument Incubator Program (IIP) grant. This instrument will make limb viewing measurements of the atmosphere in multiple directions simultaneously, and uses only a few selected wavelengths to reduce size and cost. An initial prototype version has been constructed using NASA GSFC internal funding and tested in the laboratory. Current design work is targeted towards a preliminary field test in Spring 2018. We will discuss the scientific benefits of MASTAR and the status of the project.

  13. Time resolved aerosol monitoring in the urban centre of Soweto

    Science.gov (United States)

    Formenti, P.; Annegarn, H. J.; Piketh, S. J.

    1998-03-01

    A programme of aerosol sampling was conducted from 1982 to 1984 in the urban area of Soweto, Johannesburg, South Africa. The particulate matter (aerodynamic diameter source apportionment of crustal elements between coal smoke and traffic induced road dust, based on chemical elemental measurements. A novel technique is demonstrated for processing PIXE-derived time sequence elemental concentration vectors. Slowly varying background components have been extracted from sulphur and crustal aerosol components, using alternatively two digital filters: a moving minimum, and a moving average. The residuals of the crustal elements, assigned to locally generated aerosol components, were modelled using surrogate tracers: sulphur as a surrogate for coal smoke; and Pb as a surrogate for traffic activity. Results from this source apportionment revealed coal emissions contributed between 40% and 50% of the aerosol mineral matter, while 18-22% originated from road dust. Background aerosol, characteristic of the regional winter aerosol burden over the South African Highveld, was between 12% and 21%. Minor contributors identified included a manganese smelter, located 30 km from the sampling site, and informal trash burning, as the source of intermittent heavy metals (Cu, Zn). Elemental source profiles derived for these various sources are presented.

  14. Primary gas- and particle-phase emissions and secondary organic aerosol production from gasoline and diesel off-road engines.

    Science.gov (United States)

    Gordon, Timothy D; Tkacik, Daniel S; Presto, Albert A; Zhang, Mang; Jathar, Shantanu H; Nguyen, Ngoc T; Massetti, John; Truong, Tin; Cicero-Fernandez, Pablo; Maddox, Christine; Rieger, Paul; Chattopadhyay, Sulekha; Maldonado, Hector; Maricq, M Matti; Robinson, Allen L

    2013-12-17

    Dilution and smog chamber experiments were performed to characterize the primary emissions and secondary organic aerosol (SOA) formation from gasoline and diesel small off-road engines (SOREs). These engines are high emitters of primary gas- and particle-phase pollutants relative to their fuel consumption. Two- and 4-stroke gasoline SOREs emit much more (up to 3 orders of magnitude more) nonmethane organic gases (NMOGs), primary PM and organic carbon than newer on-road gasoline vehicles (per kg of fuel burned). The primary emissions from a diesel transportation refrigeration unit were similar to those of older, uncontrolled diesel engines used in on-road vehicles (e.g., premodel year 2007 heavy-duty diesel trucks). Two-strokes emitted the largest fractional (and absolute) amount of SOA precursors compared to diesel and 4-stroke gasoline SOREs; however, 35-80% of the NMOG emissions from the engines could not be speciated using traditional gas chromatography or high-performance liquid chromatography. After 3 h of photo-oxidation in a smog chamber, dilute emissions from both 2- and 4-stroke gasoline SOREs produced large amounts of semivolatile SOA. The effective SOA yield (defined as the ratio of SOA mass to estimated mass of reacted precursors) was 2-4% for 2- and 4-stroke SOREs, which is comparable to yields from dilute exhaust from older passenger cars and unburned gasoline. This suggests that much of the SOA production was due to unburned fuel and/or lubrication oil. The total PM contribution of different mobile source categories to the ambient PM burden was calculated by combining primary emission, SOA production and fuel consumption data. Relative to their fuel consumption, SOREs are disproportionately high total PM sources; however, the vastly greater fuel consumption of on-road vehicles renders them (on-road vehicles) the dominant mobile source of ambient PM in the Los Angeles area.

  15. Study on substrate metabolism process of saline waste sludge and its biological hydrogen production potential.

    Science.gov (United States)

    Zhang, Zengshuai; Guo, Liang; Li, Qianqian; Zhao, Yangguo; Gao, Mengchun; She, Zonglian

    2017-07-01

    With the increasing of high saline waste sludge production, the treatment and utilization of saline waste sludge attracted more and more attention. In this study, the biological hydrogen production from saline waste sludge after heating pretreatment was studied. The substrate metabolism process at different salinity condition was analyzed by the changes of soluble chemical oxygen demand (SCOD), carbohydrate and protein in extracellular polymeric substances (EPS), and dissolved organic matters (DOM). The excitation-emission matrix (EEM) with fluorescence regional integration (FRI) was also used to investigate the effect of salinity on EPS and DOM composition during hydrogen fermentation. The highest hydrogen yield of 23.6 mL H 2 /g VSS and hydrogen content of 77.6% were obtained at 0.0% salinity condition. The salinity could influence the hydrogen production and substrate metabolism of waste sludge.

  16. An off-line two-dimensional analytical procedure for determination of polcyclic aromatic hydrocarbons in smoke aerosol

    NARCIS (Netherlands)

    Claessens, H.A.; Lammerts van Bueren, L.G.D.

    1987-01-01

    Smoke aerosol from stoves consists of a wide variety of chemical substances of which a number have toxic properties. To study the impact of aerosol emissions on health and environment reliable analytical procedures must be available for these samples. An off-line two-dimensional HPLC method is

  17. Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis

    Directory of Open Access Journals (Sweden)

    K. Tsigaridis

    2003-01-01

    Full Text Available A global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC, sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the

  18. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    Science.gov (United States)

    McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

    2011-08-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

  19. Assessment of source-receptor relationships of aerosols: An integrated forward and backward modeling approach

    Science.gov (United States)

    Kulkarni, Sarika

    This dissertation presents a scientific framework that facilitates enhanced understanding of aerosol source -- receptor (S/R) relationships and their impact on the local, regional and global air quality by employing a complementary suite of modeling methods. The receptor -- oriented Positive Matrix Factorization (PMF) technique is combined with Potential Source Contribution Function (PSCF), a trajectory ensemble model, to characterize sources influencing the aerosols measured at Gosan, Korea during spring 2001. It is found that the episodic dust events originating from desert regions in East Asia (EA) that mix with pollution along the transit path, have a significant and pervasive impact on the air quality of Gosan. The intercontinental and hemispheric transport of aerosols is analyzed by a series of emission perturbation simulations with the Sulfur Transport and dEposition Model (STEM), a regional scale Chemical Transport Model (CTM), evaluated with observations from the 2008 NASA ARCTAS field campaign. This modeling study shows that pollution transport from regions outside North America (NA) contributed ˜ 30 and 20% to NA sulfate and BC surface concentration. This study also identifies aerosols transported from Europe, NA and EA regions as significant contributors to springtime Arctic sulfate and BC. Trajectory ensemble models are combined with source region tagged tracer model output to identify the source regions and possible instances of quasi-lagrangian sampled air masses during the 2006 NASA INTEX-B field campaign. The impact of specific emission sectors from Asia during the INTEX-B period is studied with the STEM model, identifying residential sector as potential target for emission reduction to combat global warming. The output from the STEM model constrained with satellite derived aerosol optical depth and ground based measurements of single scattering albedo via an optimal interpolation assimilation scheme is combined with the PMF technique to

  20. Methane fluxes along a salinity gradient on a restored salt marsh, Harpswell, ME

    Science.gov (United States)

    Gunn, Cailene; Johnson, Beverly, ,, Dr.; Dostie, Phil; Bohlen, Curtis; Craig, Matthew

    2016-04-01

    This study functions as a pilot project to understand the relationship between salinity and methane emissions on a recently restored salt marsh in Casco Bay, Maine. Salt marshes are dynamic and highly productive ecosystems that provide a multitude of ecosystem services including nutrient filtration, storm-water buffering and carbon sequestration. These ecosystems are highly susceptible to anthropogenic alteration. The emplacement of causeways and narrow culverts, restricts tidal flow and leads to loss of healthy salinity gradients. Consequently, numerous salt marshes have experienced increases in freshwater vegetation growth as a result of coastal population expansion. Recent restoration efforts on Long Marsh, Harpswell, ME replaced a severely undersized culvert with a larger one in February, 2014. The salinity gradient has since been restored along much of the marsh, and freshwater vegetation that encroached on the marsh platform has died back. Vegetation and salinity are key indicators and drivers of CH4 emissions on salt marshes. Using static gas chambers, we quantified CH4 fluxes along two transects at five diverse sites ranging from healthy marsh (salinity of 27 to 31 psu) with Spartina vegetation, to regions invaded by Typha and other freshwater vegetation (salinity of 0 to 4 psu). Sampling was executed in the months of July, August and October. CH4 concentrations were determined using a gas chromatograph with a flame-ionization detector. Preliminary findings suggest reintroduction of healthy tidal flows into the marsh inhibits CH4 production, where the lowest fluxes with least variability were observed at the most saline sites with Spartina vegetation. The largest range of CH4 fluxes exhibited emissions from 0.75 μmol CH4/m2/hr to 518.4 μmol CH4/m2/hr at the Typha dominated sites from July to October. Fluxes at the saltwater and brackish regions were far less variable with ranges from 0.94 μmol CH4/m2/hr to 8.2 μmol CH4/m2/hr and 2.6 to 9.5 μmol CH4/m2

  1. AOD distributions and trends of major aerosol species over a selection of the world’s most populated cities based on the 1st Version of NASA’s MERRA Aerosol Reanalysis

    Science.gov (United States)

    Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

    2018-01-01

    NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003–2015) and over a selection of 200 of the world’s most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don’t tend

  2. Fire emission heights in the climate system – Part 2: Impact on transport, black carbon concentrations and radiation

    Directory of Open Access Journals (Sweden)

    A. Veira

    2015-07-01

    Full Text Available Wildfires represent a major source for aerosols impacting atmospheric radiation, atmospheric chemistry and cloud micro-physical properties. Previous case studies indicated that the height of the aerosol–radiation interaction may crucially affect atmospheric radiation, but the sensitivity to emission heights has been examined with only a few models and is still uncertain. In this study we use the general circulation model ECHAM6 extended by the aerosol module HAM2 to investigate the impact of wildfire emission heights on atmospheric long-range transport, black carbon (BC concentrations and atmospheric radiation. We simulate the wildfire aerosol release using either various versions of a semi-empirical plume height parametrization or prescribed standard emission heights in ECHAM6-HAM2. Extreme scenarios of near-surface or free-tropospheric-only injections provide lower and upper constraints on the emission height climate impact. We find relative changes in mean global atmospheric BC burden of up to 7.9±4.4 % caused by average changes in emission heights of 1.5–3.5 km. Regionally, changes in BC burden exceed 30–40 % in the major biomass burning regions. The model evaluation of aerosol optical thickness (AOT against Moderate Resolution Imaging Spectroradiometer (MODIS, AErosol RObotic NETwork (AERONET and Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP observations indicates that the implementation of a plume height parametrization slightly reduces the ECHAM6-HAM2 biases regionally, but on the global scale these improvements in model performance are small. For prescribed emission release at the surface, wildfire emissions entail a total sky top-of-atmosphere (TOA radiative forcing (RF of −0.16±0.06 W m−2. The application of a plume height parametrization which agrees reasonably well with observations introduces a slightly stronger negative TOA RF of −0.20±0.07 W m−2. The standard ECHAM6-HAM2 model in which 25 % of the

  3. On the representation of aerosol activation and its influence on model-derived estimates of the aerosol indirect effect

    Science.gov (United States)

    Rothenberg, Daniel; Avramov, Alexander; Wang, Chien

    2018-06-01

    Interactions between aerosol particles and clouds contribute a great deal of uncertainty to the scientific community's understanding of anthropogenic climate forcing. Aerosol particles serve as the nucleation sites for cloud droplets, establishing a direct linkage between anthropogenic particulate emissions and clouds in the climate system. To resolve this linkage, the community has developed parameterizations of aerosol activation which can be used in global climate models to interactively predict cloud droplet number concentrations (CDNCs). However, different activation schemes can exhibit different sensitivities to aerosol perturbations in different meteorological or pollution regimes. To assess the impact these different sensitivities have on climate forcing, we have coupled three different core activation schemes and variants with the CESM-MARC (two-Moment, Multi-Modal, Mixing-state-resolving Aerosol model for Research of Climate (MARC) coupled with the National Center for Atmospheric Research's (NCAR) Community Earth System Model (CESM; version 1.2)). Although the model produces a reasonable present-day CDNC climatology when compared with observations regardless of the scheme used, ΔCDNCs between the present and preindustrial era regionally increase by over 100 % in zonal mean when using the most sensitive parameterization. These differences in activation sensitivity may lead to a different evolution of the model meteorology, and ultimately to a spread of over 0.8 W m-2 in global average shortwave indirect effect (AIE) diagnosed from the model, a range which is as large as the inter-model spread from the AeroCom intercomparison. Model-derived AIE strongly scales with the simulated preindustrial CDNC burden, and those models with the greatest preindustrial CDNC tend to have the smallest AIE, regardless of their ΔCDNC. This suggests that present-day evaluations of aerosol-climate models may not provide useful constraints on the magnitude of the AIE, which

  4. Aerosol optical depth trend over the Middle East

    KAUST Repository

    Klingmüller, Klaus

    2016-04-22

    We use the combined Dark Target/Deep Blue aerosol optical depth (AOD) satellite product of the moderate-resolution imaging spectroradiometer (MODIS) collection 6 to study trends over the Middle East between 2000 and 2015. Our analysis corroborates a previously identified positive AOD trend over large parts of the Middle East during the period 2001 to 2012. We relate the annual AOD to precipitation, soil moisture and surface winds to identify regions where these attributes are directly related to the AOD over Saudi Arabia, Iraq and Iran. Regarding precipitation and soil moisture, a relatively small area in and surrounding Iraq turns out to be of prime importance for the AOD over these countries. Regarding surface wind speed, the African Red Sea coastal area is relevant for the Saudi Arabian AOD. Using multiple linear regression we show that AOD trends and interannual variability can be attributed to soil moisture, precipitation and surface winds, being the main factors controlling the dust cycle. Our results confirm the dust driven AOD trends and variability, supported by a decreasing MODIS-derived Ångström exponent and a decreasing AERONET-derived fine mode fraction that accompany the AOD increase over Saudi Arabia. The positive AOD trend relates to a negative soil moisture trend. As a lower soil moisture translates into enhanced dust emissions, it is not needed to assume growing anthropogenic aerosol and aerosol precursor emissions to explain the observations. Instead, our results suggest that increasing temperature and decreasing relative humidity in the last decade have promoted soil drying, leading to increased dust emissions and AOD; consequently an AOD increase is expected due to climate change.

  5. The contribution of ship emissions to air pollution in the North Sea regions

    Energy Technology Data Exchange (ETDEWEB)

    Matthias, Volker, E-mail: volker.matthias@gkss.d [GKSS Research Centre Geesthacht, Institute for Coastal Research, Max-Planck-Strasse 1, 21502 Geesthacht (Germany); Bewersdorff, Ines [GKSS Research Centre Geesthacht, Institute for Coastal Research, Max-Planck-Strasse 1, 21502 Geesthacht (Germany); Aulinger, Armin, E-mail: armin.aulinger@gkss.d [GKSS Research Centre Geesthacht, Institute for Coastal Research, Max-Planck-Strasse 1, 21502 Geesthacht (Germany); Quante, Markus, E-mail: markus.quante@gkss.d [GKSS Research Centre Geesthacht, Institute for Coastal Research, Max-Planck-Strasse 1, 21502 Geesthacht (Germany)

    2010-06-15

    As a consequence of the global distribution of manufacturing sites and the increasing international division of labour, ship traffic is steadily increasing and is becoming more and more important as an origin of air pollution. This study investigates the impact of ship emissions in coastal areas of the North Sea under conditions of the year 2000 by means of a regional chemistry transport model which runs on a sufficiently high resolution to study air pollution in coastal regions. It was found that northern Germany and Denmark in summer suffer from more than 50% higher sulphate, nitrate and ammonium aerosol concentrations due to contributions from ships. The implementation of a sulphur emission control area (SECA) in the North Sea, as it was implemented at the end of 2007, directly results in reduced sulphur dioxide and sulphate aerosol concentrations while nitrate aerosol concentrations are slightly increased. - Ship emissions lead to significantly enhanced air pollution by secondary inorganic aerosols in North Sea coastal areas.

  6. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    Directory of Open Access Journals (Sweden)

    M. F. Heringa

    2012-02-01

    Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

    The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

    Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions.

    The HR data of the four sources could be clustered and separated using

  7. Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

    Directory of Open Access Journals (Sweden)

    I. S. A. Isaksen

    2007-11-01

    Full Text Available The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA. Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics. A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr−1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA is the dominant OA component than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes

  8. Size distribution and concentrations of heavy metals in atmospheric aerosols originating from industrial emissions as predicted by the HYSPLIT model

    Science.gov (United States)

    Chen, Bing; Stein, Ariel F.; Maldonado, Pabla Guerrero; Sanchez de la Campa, Ana M.; Gonzalez-Castanedo, Yolanda; Castell, Nuria; de la Rosa, Jesus D.

    2013-06-01

    This study presents a description of the emission, transport, dispersion, and deposition of heavy metals contained in atmospheric aerosols emitted from a large industrial complex in southern Spain using the HYSPLIT model coupled with high- (MM5) and low-resolution (GDAS) meteorological simulations. The dispersion model was configured to simulate eight size fractions (17 μm) of metals based on direct measurements taken at the industrial emission stacks. Twelve stacks in four plants were studied and the stacks showed considerable differences for both emission fluxes and size ranges of metals. We model the dispersion of six major metals; Cr, Co, Ni, La, Zn, and Mo, which represent 77% of the total mass of the 43 measured elements. The prediction shows that the modeled industrial emissions produce an enrichment of heavy metals by a factor of 2-5 for local receptor sites when compared to urban and rural background areas in Spain. The HYSPLIT predictions based on the meteorological fields from MM5 show reasonable consistence with the temporal evolution of concentrations of Cr, Co, and Ni observed at three sites downwind of the industrial area. The magnitude of concentrations of metals at two receptors was underestimated for both MM5 (by a factor of 2-3) and GDAS (by a factor of 4-5) meteorological runs. The model prediction shows that heavy metal pollution from industrial emissions in this area is dominated by the ultra-fine (<0.66 μm) and fine (<2.5 μm) size fractions.

  9. Characterization of aerosol emitted by the combustion of nanocomposites

    Energy Technology Data Exchange (ETDEWEB)

    Motzkus, C; Chivas-Joly, C; Guillaume, E; Ducourtieux, S; Saragoza, L; Lesenechal, D; Mace, T, E-mail: charles.motzkus@lne.fr [LNE, 29 Avenue Roger Hennequin, 78197 Trappes Cedex (France)

    2011-07-06

    Day after day, new applications using nanoparticles appear in industry, increasing the probability to find these particles in the workplace as well as in ambient air. As epidemiological studies have shown an association between increased particulate air pollution and adverse health effects in susceptible members of the population, it is particularly important to characterize aerosols emitted by different sources of emission, during the combustion of composites charged with nanoparticles for example. The present study is led in the framework of the NANOFEU project, supported by the French Research Agency (ANR), in order to characterize the fire behaviour of polymers charged with suitable nanoparticles and make an alternative to retardant systems usually employed. To determine the impact of these composites on the emission of airborne particles produced during their combustions, an experimental setup has been developed to measure the mass distribution in the range of 30 nm - 10 {mu}m and the number concentration of submicrometric particles of the produced aerosol. A comparison is performed on the aerosol emitted during the combustion of several polymers alone (PMMA, PA-6), polymers containing nanofillers (silica, alumina, and carbon nanotubes) and polymers containing both nanofillers and a conventional flame retardant system (ammonium polyphosphate). The results on the morphology of particles were also investigated using AFM.

  10. Effects of increasing aerosol on regional climate change in China: Observation and modeling

    Science.gov (United States)

    Qian, Y.; Leung, L.; Ghan, S. J.

    2002-12-01

    We present regional simulations of climate, aerosol properties, and direct radiative forcing and climatic effects of aerosol and analyze the pollutant emissions and observed climatic data during the latter decades of last century in China. The regional model generally captures the spatial distributions and seasonal pattern of temperature and precipitation. Aerosol extinction coefficient and aerosol optical depth are generally well simulated in both magnitude and spatial distribution, which provides a reliable foundation for estimating the radiative forcing and climatic effects of aerosol. The radiative forcing of aerosol is in the range of -1 to -14 W m-2 in autumn and summer and -1 to -9 W m-2 in spring and winter, with substantial spatial variability at the sub-regional scale. A strong maximum in negative radiative forcing corresponding to the maximum optical depth is found over the Sichuan Basin, where emission as well as relative humidity are high, and stagnant atmospheric conditions inhibit pollutants dispersion. Negative radiative forcing of aerosol induces a surface cooling, which is stronger in the range of -0.6 to -1.2oC in autumn and winter than in spring (-0.3 to -0.6oC) and summer (0.0 to -0.9oC) over the Sichuan Basin and East China due to more significant effects of cloud and precipitation in the summer and spring. Aerosol-induced cooling is mainly contributed by cooling in the daytime temperature. The cooling reaches a maximum and is statistically significant in the Sichuan Basin. The effect of aerosol on precipitation is not evident in our simulations. The temporal and spatial patterns of temperature trends observed in the second half of the twentieth century, including the asymmetric daily maximum and minimum temperature trends, are at least qualitatively consistent with the simulated aerosol-induced cooling over the Sichuan Basin and East China. It supports the hypothesis that the observed temperature trends during the latter decades of the

  11. The Effect of Central American Smoke Aerosols on the Air Quality and Climate over the Southeastern United States: First Results from RAMS-AROMA

    Science.gov (United States)

    Wang, J.; Christopher, S. A.; Nair, U. S.; Reid, J.; Prins, E. M.; Szykman, J.

    2004-12-01

    Observation shows that smoke aerosols from biomass burning activities in Central America can be transported to the Southeastern United States (SEUS). In this study, the Regional Atmospheric Modeling System - Assimilation and Radiation Online Modeling of Aerosols (RAMS-AROMA) is used to investigate the effect of transported smoke aerosols on climate and air quality over the SEUS. AROMA is an aerosol transport model with capabilities of online integration of aerosol radiation effects and online assimilation of satellite-derived aerosol and emission products. It is assembled within the RAMS, so two-way interactions between aerosol fields and other meteorology fields are achieved simultaneously during each model time step. RAMS-AROMA is a unique tool that can be used to examine the aerosol radiative impacts on the surface energy budget and atmospheric heating rate and to investigate how atmospheric thermal and dynamical processes respond to such impacts and consequently affect the aerosol distribution (so called feedbacks). First results regarding air quality effects and radiative forcing of transported smoke aerosols will be presented from RAMS-AROMA based on assimilation of smoke emission products from the Fire Locating and Modeling of Burning Emissions (FLAMBE) project and aerosol optical thickness data derived from the MODIS instrument on the Terra and Aqua satellites. Comparisons with PM2.5 data collected from the EPA observation network and the aerosol optical thickness data from the DOE Atmosphere Radiation Measurements in the Southern Great Plains (ARM SGP) showed that RAMS-AROMA can predict the timing and spatial distribution of smoke events very well, with an accuracy useful for air quality forecasts. The smoke radiative effects on the surface temperature and atmospheric heating rate as well as their feedbacks will also be discussed.

  12. Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

    Science.gov (United States)

    Spracklen, D. V.; Carslaw, K. S.; Merikanto, J.; Mann, G. W.; Reddington, C. L.; Pickering, S.; Ogren, J. A.; Andrews, E.; Baltensperger, U.; Weingartner, E.; Boy, M.; Kulmala, M.; Laakso, L.; Lihavainen, H.; Kivekäs, N.; Komppula, M.; Mihalopoulos, N.; Kouvarakis, G.; Jennings, S. G.; O'Dowd, C.; Birmili, W.; Wiedensohler, A.; Weller, R.; Gras, J.; Laj, P.; Sellegri, K.; Bonn, B.; Krejci, R.; Laaksonen, A.; Hamed, A.; Minikin, A.; Harrison, R. M.; Talbot, R.; Sun, J.

    2010-05-01

    We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300-2000 cm-3 in the marine boundary layer and free troposphere (FT) and 1000-10 000 cm-3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2-10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=-88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=-25%). Simulated CN concentrations in the continental BL were also biased low (NMB=-74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation

  13. Recent intensification of winter haze in China linked to foreign emissions and meteorology.

    Science.gov (United States)

    Yang, Yang; Wang, Hailong; Smith, Steven J; Zhang, Rudong; Lou, Sijia; Qian, Yun; Ma, Po-Lun; Rasch, Philip J

    2018-02-01

    Wintertime aerosol pollution in the North China Plain has increased over the past several decades as anthropogenic emissions in China have increased, and has dramatically escalated since the beginning of the 21 st century, but the causes and their quantitative attributions remain unclear. Here we use an aerosol source tagging capability implemented in a global aerosol-climate model to assess long-term trends of PM 2.5 (particulate matter less than 2.5 μm in diameter) in the North China Plain. Our analysis suggests that the impact of China's increasing domestic emissions on PM 2.5 concentrations over the last two decades of 20 th century was partially offset (13%) by decreasing foreign emission over this period. As foreign emissions stabilized after 2000, their counteracting effect almost disappeared, uncovering the impact of China's increasing domestic emissions that had been partially offset in previous years by reductions in foreign emissions. A slowdown in the impact from foreign emission reductions together with weakening winds explain 25% of the increased PM 2.5 trend over 2000-2014 as compared to 1980-2000. Further reductions in foreign emissions are not expected to relieve China's pollution in the future. Reducing local emissions is the most certain way to improve future air quality in the North China Plain.

  14. Aerosol volatility in a boreal forest environment

    Science.gov (United States)

    Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

    2012-04-01

    during spring and autumn 2008. Results from the aerosol mass spectrometry indicate that the non-volatile residual consists of nitrate and organic compounds, especially during autumn. These compounds may be low-volatile organic nitrates or salts. During winter and spring the non-volatile core (black carbon removed) correlated markedly with carbon monoxide, which is a tracer of anthropogenic emissions. Due to this, the non-volatile residual may also contain other pollutants in addition to black carbon. Thus, it seems that the amount of different compounds in submicron aerosol particles varies with season and as a result the chemical composition of the non-volatile residual changes within a year. This work was supported by University of Helsinki three-year research grant No 490082 and Maj and Tor Nessling Foundation grant No 2010143. Aalto et al., (2001). Physical characterization of aerosol particles during nucleation events. Tellus B, 53, 344-358. Jayne, et al., (2000). Development of an aerosol mass spectrometer for size and composition analysis of submicron particles. Aerosol Sci. Technol., 33(1-2), 49-70. Kalberer et al., (2004). Identification of Polymers as Major Components of Atmospheric Organic Aerosols. Science, 303, 1659-1662. Smith et al., (2010). Observations of aminium salts in atmospheric nanoparticles and possible climatic implications. P. Natl. Acad. Sci., 107(15). Vesala et al., (1998). Long-term field measurements of atmosphere-surface interactions in boreal forest combining forest ecology, micrometeorology, aerosol physics and atmospheric chemistry. Trends Heat, Mass Mom. Trans., 4, 17-35. Wehner et al., (2002). Design and calibration of a thermodenuder with an improved heating unit to measure the size-dependent volatile fraction of aerosol particles. J. Aerosol Sci., 33, 1087-1093.

  15. Diagnosing causes of extreme aerosol optical depth events

    Science.gov (United States)

    Bernstein, D. N.; Sullivan, R.; Crippa, P.; Thota, A.; Pryor, S. C.

    2017-12-01

    Aerosol burdens and optical properties exhibit substantial spatiotemporal variability, and simulation of current and possible future aerosol burdens and characteristics exhibits relatively high uncertainty due to uncertainties in emission estimates and in chemical and physical processes associated with aerosol formation, dynamics and removal. We report research designed to improve understanding of the causes and characteristics of extreme aerosol optical depth (AOD) at the regional scale, and diagnose and attribute model skill in simulating these events. Extreme AOD events over the US Midwest are selected by identifying all dates on which AOD in a MERRA-2 reanalysis grid cell exceeds the local seasonally computed 90th percentile (p90) value during 2004-2016 and then finding the dates on which the highest number of grid cells exceed their local p90. MODIS AOD data are subsequently used to exclude events dominated by wildfires. MERRA-2 data are also analyzed within a synoptic classification to determine in what ways the extreme AOD events are atypical and to identify possible meteorological `finger-prints' that can be detected in regional climate model simulations of future climate states to project possible changes in the occurrence of extreme AOD. Then WRF-Chem v3.6 is applied at 12-km resolution and regridded to the MERRA-2 resolution over eastern North America to quantify model performance, and also evaluated using in situ measurements of columnar AOD (AERONET) and near-surface PM2.5 (US EPA). Finally the sensitivity to (i) spin-up time (including procedure used to spin-up the chemistry), (ii) modal versus sectional aerosol schemes, (iii) meteorological nudging, (iv) chemistry initial and boundary conditions, and (v) anthropogenic emissions is quantified. Despite recent declines in mean AOD, supraregional (> 1000 km) extreme AOD events continue to occur. During these events AOD exceeds 0.6 in many Midwestern grid cells for multiple consecutive days. In all

  16. The Influence of Anthropogenic Greenhouse Gases and Aerosols on the Surface Heat and Moisture Budgets.

    Science.gov (United States)

    Ramaswamy, V.; Freidenreich, S.; Ginoux, P. A.; Ming, Y.; Paynter, D.; Persad, G.; Schwarzkopf, M. D.

    2017-12-01

    Emissions of greenhouse gases and aerosols alter atmospheric composition and `force' major perturbations in the radiative fluxes at the top-of-the-atmosphere and surface. In this paper, we discuss the radiative changes caused by anthropogenic greenhouse gases and aerosols at the surface, and its importance in the context of effects on the global hydrologic cycle. An important characteristic of imbalances forced by radiative species is the tendency for responses to occur in the non-radiative components, in order for the surface energy and moisture budgets to re-establish equilibrium. Using the NOAA/ GFDL global climate models used in CMIP3 and CMIP5, and to be used in CMIP6, we investigate how the surface energy balance has evolved with time under the action of the emissions, and the manner of changes in the surface radiative, sensible and latent heat components. We diagnose the relative importance of the forcings on the global and continental scales, the differing mechanisms due to greenhouse gases and aerosols on surface heat and moisture budgets, and the relative roles of the atmospheric constituents on precipitation and evaporation. Scattering and absorbing properties of aerosols can have contrasting effects on precipitation, with the aerosol indirect effect presenting another complication owing to the uncertainty in its magnitude. We compare the modeled surface flux changes against observations made from multiple platforms over the 20th and the early period of the 21st centuries, and asses the models' strengths and weaknesses. We also explore the consequences for the surface balance and precipitation in the 21st century under various emission scenarios.

  17. Biogenic, anthropogenic and sea salt sulfate size-segregated aerosols in the Arctic summer

    Directory of Open Access Journals (Sweden)

    R. Ghahremaninezhad

    2016-04-01

    Full Text Available Size-segregated aerosol sulfate concentrations were measured on board the Canadian Coast Guard Ship (CCGS Amundsen in the Arctic during July 2014. The objective of this study was to utilize the isotopic composition of sulfate to address the contribution of anthropogenic and biogenic sources of aerosols to the growth of the different aerosol size fractions in the Arctic atmosphere. Non-sea-salt sulfate is divided into biogenic and anthropogenic sulfate using stable isotope apportionment techniques. A considerable amount of the average sulfate concentration in the fine aerosols with a diameter  <  0.49 µm was from biogenic sources (>  63 %, which is higher than in previous Arctic studies measuring above the ocean during fall (<  15 % (Rempillo et al., 2011 and total aerosol sulfate at higher latitudes at Alert in summer (>  30 % (Norman et al., 1999. The anthropogenic sulfate concentration was less than that of biogenic sulfate, with potential sources being long-range transport and, more locally, the Amundsen's emissions. Despite attempts to minimize the influence of ship stack emissions, evidence from larger-sized particles demonstrates a contribution from local pollution. A comparison of δ34S values for SO2 and fine aerosols was used to show that gas-to-particle conversion likely occurred during most sampling periods. δ34S values for SO2 and fine aerosols were similar, suggesting the same source for SO2 and aerosol sulfate, except for two samples with a relatively high anthropogenic fraction in particles  <  0.49 µm in diameter (15–17 and 17–19 July. The high biogenic fraction of sulfate fine aerosol and similar isotope ratio values of these particles and SO2 emphasize the role of marine organisms (e.g., phytoplankton, algae, bacteria in the formation of fine particles above the Arctic Ocean during the productive summer months.

  18. Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

    Science.gov (United States)

    Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

    2017-10-01

    The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

  19. Aerosol Properties under Air Quality Control Measures of APEC 2014 in Beijing

    Science.gov (United States)

    Chen, X.; Xu, H.; Lv, Y.; Xie, Y.; Li, K.; Li, Z.; Li, D.; Ma, Y.; Mei, X.

    2015-12-01

    Because the economic and society were developing fast in the middle of last century, Los Angeles and London both were polluted by photochemical smog, which massacred thousands of people. Now, many regions are often covered by heavy haze in those large developing countries, especially in China and India. The Asia-Pacific Economic Cooperation (APEC) was held in Beijing during 5-11 November 2014. Beijing, Hebei, Tianjin, Shandong, Shanxi, Inner Mongolia reduced air pollution emissions for the APEC 2014 meeting held in Beijing. Only in Hebei province, there were 1028 factories stopped or restricted and 881 construction sites stopped. Half of the cars were prohibited driving even in the Zibo city which is 400 km far from Beijing. For scientific aims, these control measures were indeed a huge and uncommon atmospheric experiment led by the government. During the experiment, what did the "APEC Blue" mean? We analyzed aerosol properties with the data of an AERONET site in Beijing which is located 500m far from the main reception hall of APEC 2014. The Cimel solar photometers can give a series parameters of aerosol and water vapor. In this paper, we used CE318 solar photometer which is the main instrument of NASA AERONET. The CE318 of RADI belongs to the Chinese SONET (Sun-sky radiometer Observation NETwork) too. We analyzed the total, coarse and fine Aerosol Optical Depth (AOD), Fine-Mode Fraction (FMF) and Ångström exponent, Size Distribution and Real Refractive Index. In conclusion, the aerosol properties were analysed with the measurements of a sun photometer. During the APEC 2014, AOD decreased obviously with a 0.27 mean value compared with the annual mean 0.7. Around Beijing, the southern is polluted emission area including the cross part of Shandong, Shanxi, Hebei, Henan four provinces, and the northern is clean for less fine mode particles emission in the large Inner Mongolia province. In fact, during the APEC 2014, the weather condition was not good for the

  20. Estimating Landscape Fire Particulate Matter (PM) Emissions over Southern Africa using MSG-SEVIRI Fire Radiative Power (FRP) and MODIS Aerosol Optical Thickness Observations

    Science.gov (United States)

    Mota, Bernardo; Wooster, Martin J.

    2016-04-01

    The approach to estimating landscape fire fuel consumption based on the remotely sensed fire radiative power (FRP) thermal energy release rate, as opposed to burned area, is now relatively widely used in studies of fire emissions, including operationally within the Copernicus Atmosphere Monitoring Service (CAMS). Nevertheless, there are still limitations to the approach, including uncertainties associated with using only the few daily overpasses typically provided by polar orbiting satellite systems, the conversion between FRP and smoke emissions, and the increased likelihood that the more frequent data from geostationary systems fails to detect the (probably highly numerous) smaller (i.e. low FRP) component of a regions fire regime. In this study, we address these limitations to directly estimate fire emissions of Particular Matter (PM; or smoke aerosols) by presenting an approach combining the "bottom-up" FRP observations available every 15 minutes across Africa from the Meteosat Spinning Enhanced Visible and Infrared Imager (SEVIRI) Fire Radiative Product (FRP) processed at the EUMETSAT LSA SAF, and the "top-down" aerosol optical thickness (AOT) measures of the fire plumes themselves as measured by the Moderate-resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Terra (MOD04_L2) and Aqua (MYD04_L2) satellites. We determine PM emission coefficients that relate directly to FRP measures by combining these two datasets, and the use of the almost continuous geostationary FRP observations allows us to do this without recourse to (uncertain) data on wind speed at the (unknown) height of the matching plume. We also develop compensation factors to address the detection limitations of small/low intensity (low FRP) fires, and remove the need to estimate fuel consumption by going directly from FRP to PM emissions. We derive the smoke PM emissions coefficients per land cover class by comparing the total fire radiative energy (FRE) released from individual fires