Stable Carbon Fractionation In Size Segregated Aerosol Particles Produced By Controlled Biomass Burning

Science.gov (United States)

Masalaite, Agne; Garbaras, Andrius; Garbariene, Inga; Ceburnis, Darius; Martuzevicius, Dainius; Puida, Egidijus; Kvietkus, Kestutis; Remeikis, Vidmantas

2014-05-01

Biomass burning is the largest source of primary fine fraction carbonaceous particles and the second largest source of trace gases in the global atmosphere with a strong effect not only on the regional scale but also in areas distant from the source . Many studies have often assumed no significant carbon isotope fractionation occurring between black carbon and the original vegetation during combustion. However, other studies suggested that stable carbon isotope ratios of char or BC may not reliably reflect carbon isotopic signatures of the source vegetation. Overall, the apparently conflicting results throughout the literature regarding the observed fractionation suggest that combustion conditions may be responsible for the observed effects. The purpose of the present study was to gather more quantitative information on carbonaceous aerosols produced in controlled biomass burning, thereby having a potential impact on interpreting ambient atmospheric observations. Seven different biomass fuel types were burned under controlled conditions to determine the effect of the biomass type on the emitted particulate matter mass and stable carbon isotope composition of bulk and size segregated particles. Size segregated aerosol particles were collected using the total suspended particle (TSP) sampler and a micro-orifice uniform deposit impactor (MOUDI). The results demonstrated that particle emissions were dominated by the submicron particles in all biomass types. However, significant differences in emissions of submicron particles and their dominant sizes were found between different biomass fuels. The largest negative fractionation was obtained for the wood pellet fuel type while the largest positive isotopic fractionation was observed during the buckwheat shells combustion. The carbon isotope composition of MOUDI samples compared very well with isotope composition of TSP samples indicating consistency of the results. The measurements of the stable carbon isotope ratio in

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.

Linking remotely sensed aerosol types to their chemical composition

Science.gov (United States)

Dawson, K. W.; Kacenelenbogen, M. S.; Johnson, M. S.; Burton, S. P.; Hostetler, C. A.; Meskhidze, N.

2016-12-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% ± 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into `dark' and `light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

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

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

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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

Estimation of black carbon content for biomass burning aerosols from multi-channel Raman lidar data

Science.gov (United States)

Talianu, Camelia; Marmureanu, Luminita; Nicolae, Doina

2015-04-01

Biomass burning due to natural processes (forest fires) or anthropical activities (agriculture, thermal power stations, domestic heating) is an important source of aerosols with a high content of carbon components (black carbon and organic carbon). Multi-channel Raman lidars provide information on the spectral dependence of the backscatter and extinction coefficients, embedding information on the black carbon content. Aerosols with a high content of black carbon have large extinction coefficients and small backscatter coefficients (strong absorption), while aerosols with high content of organic carbon have large backscatter coefficients (weak absorption). This paper presents a method based on radiative calculations to estimate the black carbon content of biomass burning aerosols from 3b+2a+1d lidar signals. Data is collected at Magurele, Romania, at the cross-road of air masses coming from Ukraine, Russia and Greece, where burning events are frequent during both cold and hot seasons. Aerosols are transported in the free troposphere, generally in the 2-4 km altitude range, and reaches the lidar location after 2-3 days. Optical data are collected between 2011-2012 by a multi-channel Raman lidar and follows the quality assurance program of EARLINET. Radiative calculations are made with libRadTran, an open source radiative model developed by ESA. Validation of the retrievals is made by comparison to a co-located C-ToF Aerosol Mass Spectrometer. Keywords: Lidar, aerosols, biomass burning, radiative model, black carbon Acknowledgment: This work has been supported by grants of the Romanian National Authority for Scientific Research, Programme for Research- Space Technology and Advanced Research - STAR, project no. 39/2012 - SIAFIM, and by Romanian Partnerships in priority areas PNII implemented with MEN-UEFISCDI support, project no. 309/2014 - MOBBE

Study of total column atmospheric aerosol optical depth, ozone and ...

Indian Academy of Sciences (India)

Extensive observations of the columnar aerosol optical depth (AOD), total column ozone (TCO) and precipitable water content (PWC) have been carried out using the on-line, multi-band solar radiometers onboard ORV Sagar Kanya (Cruise#SK 147B) over Bay of Bengal during 11th-28th August 1999. Aerosol optical and ...

Comparison of methods for the quantification of the different carbon fractions in atmospheric aerosol samples

Science.gov (United States)

Nunes, Teresa; Mirante, Fátima; Almeida, Elza; Pio, Casimiro

2010-05-01

Atmospheric carbon consists of: organic carbon (OC, including various organic compounds), elemental carbon (EC, or black carbon [BC]/soot, a non-volatile/light-absorbing carbon), and a small quantity of carbonate carbon. Thermal/optical methods (TOM) have been widely used for quantifying total carbon (TC), OC, and EC in ambient and source particulate samples. Unfortunately, the different thermal evolution protocols in use can result in a wide elemental carbon-to-total carbon variation. Temperature evolution in thermal carbon analysis is critical to the allocation of carbon fractions. Another critical point in OC and EC quantification by TOM is the interference of carbonate carbon (CC) that could be present in the particulate samples, mainly in the coarse fraction of atmospheric aerosol. One of the methods used to minimize this interference consists on the use of a sample pre-treatment with acid to eliminate CC prior to thermal analysis (Chow et al., 2001; Pio et al., 1994). In Europe, there is currently no standard procedure for determining the carbonaceous aerosol fraction, which implies that data from different laboratories at various sites are of unknown accuracy and cannot be considered comparable. In the framework of the EU-project EUSAAR, a comprehensive study has been carried out to identify the causes of differences in the EC measured using different thermal evolution protocols. From this study an optimised protocol, the EUSAAR-2 protocol, was defined (Cavali et al., 2009). During the last two decades thousands of aerosol samples have been taken over quartz filters at urban, industrial, rural and background sites, and also from plume forest fires and biomass burning in a domestic closed stove. These samples were analysed for OC and EC, by a TOM, similar to that in use in the IMPROVE network (Pio et al., 2007). More recently we reduced the number of steps in thermal evolution protocols, without significant repercussions in the OC/EC quantifications. In order

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-.

Contribution of Black Carbon Aerosol to Drying of the Mediterranean

Science.gov (United States)

Tang, T.; Shindell, D. T.; Samset, B. H.; Boucher, O.; Forster, P.; Hodnebrog, Ø.; Myhre, G.; Sillmann, J.; Voulgarakis, A.; Andrews, T.; Faluvegi, G.; Fläschner, D.; Iverson, T.; Kasoar, M.; Kharin, V. V.; Kirkevag, A.; Lamarque, J. F.; Olivié, D.; Richardson, T.; Stjern, C.; Takemura, T.; Zwiers, F. W.

2017-12-01

Atmospheric aerosols affect cloud properties, radiative balance and thus, the hydrological cycle. Many studies have reported that precipitation has decreased in the Mediterranean since the mid-20th century, and investigated possible mechanisms. So far, however, the effects of aerosol forcing on Mediterranean precipitation remain largely unknown. Here we compare observed Mediterranean precipitation trends during 1951-2010 with responses to individual forcing in a set of state-of-the-art global climate models. Our analyses suggest that nearly one-third (30%) of the observed precipitation decrease may be attributable to black carbon forcing. The remainder is most strongly linked to forcing of well-mixed greenhouse gases (WMGHGs), with scattering sulfate aerosols having negligible impacts. Black carbon caused an enhanced positive North Atlantic Oscillation (NAO)/Arctic Oscillation (AO)-like sea level pressure (SLP) pattern, characterized by higher SLP at mid-latitudes and lower SLP at high-latitudes. This SLP change diverted the jet stream and storm tracks further northward, reducing precipitation in the Mediterranean while increasing precipitation in Northern Europe. The results from this study suggest that future black carbon emissions may significantly affect regional water resources, agricultural practices, ecosystems, and economy in the Mediterranean region.

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

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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.

The role of iron and black carbon in aerosol light absorption

Directory of Open Access Journals (Sweden)

Y. Derimian

2008-07-01

Full Text Available Iron is a major component of atmospheric aerosols, influencing the light absorption ability of mineral dust, and an important micronutrient that affects oceanic biogeochemistry. The regional distribution of the iron concentration in dust is important for climate studies; however, this is difficult to obtain since it requires in-situ aerosol sampling or simulation of complex natural processes. Simultaneous studies of aerosol chemical composition and radiometric measurements of aerosol optical properties, which were performed in the Negev desert of Israel continuously for about eight years, suggest a potential for deriving a relationship between chemical composition and light absorption properties, in particular the spectral single-scattering albedo.

The two main data sets of the present study were obtained by a sun/sky radiometer and a stacked filter unit sampler that collects particles in coarse and fine size fractions. Analysis of chemical and optical data showed the presence of mixed dust and pollution aerosol in the study area, although their sources appear to be different. Spectral SSA showed an evident response to increased concentrations of iron, black carbon equivalent matter, and their mixing state. A relationship that relates the spectral SSA, the percentage of iron in total particulate mass, and the pollution components was derived. Results calculated, using this relationship, were compared with measurements from dust episodes in several locations around the globe. The comparison showed reasonable agreement between the calculated and the observed iron concentrations, and supported the validity of the suggested approach for the estimation of iron concentrations in mineral dust.

Stable carbon and nitrogen isotopic compositions of ambient aerosols collected from Okinawa Island in the western North Pacific Rim, an outflow region of Asian dusts and pollutants

Science.gov (United States)

Kunwar, Bhagawati; Kawamura, Kimitaka; Zhu, Chunmao

2016-04-01

Stable carbon (δ13C) and nitrogen (δ15N) isotope ratios were measured for total carbon (TC) and nitrogen (TN), respectively, in aerosol (TSP) samples collected at Cape Hedo, Okinawa, an outflow region of Asian pollutants, during 2009-2010. The averaged δ13C and δ15N ratios are -22.2‰ and +12.5‰, respectively. The δ13C values are similar in both spring (-22.5‰) and winter (-22.5‰), suggesting the similar sources and/or source regions. We found that δ13C from Okinawa aerosols are ca. 2‰ higher than those reported from Chinese megacities probably due to photochemical aging of organic aerosols. A strong correlation (r = 0.81) was found between nss-Ca and TSP, suggesting that springtime aerosols are influenced from Asian dusts. However, carbonates in the Asian dusts were titrated with acidic species such as sulfuric acid and oxalic acid during atmospheric transport although two samples suggested the presence of remaining carbonate. No correlations were found between δ13C and tracer compounds (levoglucosan, elemental carbon, oxalic acid, and Na+). During winter and spring, coal burning is significant source in China. Based on isotopic mass balance, contribution of coal burning origin particles to total aerosol carbon was estimated as ca. 97% in winter, which is probably associated with the high emissions in China. Contribution of NO3- to TN was on average 45% whereas that of NH4+ was 18%. These results suggest that vehicular exhaust is an important source of TN in Okinawa aerosols. Concentration of water-soluble organic nitrogen (WSON) is higher in summer, suggesting that WSON is more emitted from the ocean in warmer season whereas inorganic nitrogen is more emitted in winter and spring from pollution sources in the Asian continent.

Microparticles and human health: particulate materials, trace metals elements and black carbon in aerosols collected at Andravoahangy-Antananarivo, Madagascar

International Nuclear Information System (INIS)

Rasoazanany, E. O.; Andriamahenina, N. N.; Harinoely, M.; Ravoson, H. N.; Randriamanivo, L. V.; Raoelina Andriambololona; Ramaherison, H.

2013-01-01

The present work is to determine the concentrations of microparticles having diameter inferior to 10 μm (PM 10 ), the metal trace elements and the black carbon in the aerosols sampled in Andravoahangy-Antananarivo, Madagascar in 2008. The air sampler GENT is used to collect aerosol samples. The total reflection X-ray fluorescence spectrometer is used for qualitative and quantitative analysis of simultaneous way all metallic trace elements contained in the aerosols. The M43D reflectometer permits to measure the reflectances in order to determine the black carbon concentrations. The results show that the average concentrations of the particulate matters PM 2,5-10 are higher than those of PM 2,5 . The average concentrations of PM 10 in the aerosols are exceeding the World Health Organisation (WHO) and European Union guidelines, set at 50 μg.m -3 and those of PM 2,5 are higher than the 2005 WHO (25 μg.m-3) and the United States Environment Protection Agency (35 μg.m -3 ) guidelines. Consequently, air quality in Andravoahangy does not respect these daily guidelines. The identified metallic trace elements in the aerosols are Ti, Cr, Mn, Fe, Ni, Cu, Zn and Pb. The average concentrations of these elements are also higher in the coarse particles than in the fine particles. The concentrations of black carbon are higher in the fine particles. The maximum value is 9.12 μg.m -3 . [fr

Diurnal variations of organic molecular tracers and stable carbon isotopic compositions in atmospheric aerosols over Mt. Tai in North China Plain: an influence of biomass burning

Science.gov (United States)

Fu, P. Q.; Kawamura, K.; Chen, J.; Li, J.; Sun, Y. L.; Liu, Y.; Tachibana, E.; Aggarwal, S. G.; Okuzawa, K.; Tanimoto, H.; Kanaya, Y.; Wang, Z. F.

2012-04-01

Organic tracer compounds of tropospheric aerosols, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated for aerosol samples collected during early and late periods of Mount Tai eXperiment 2006 (MTX2006) field campaign in North China Plain. Total solvent extracts were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in North China Plain were very active, the total identified organics (2090 ± 1170 ng m-3) were double those in late June (926 ± 574 ng m-3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88-1210 ng m-3, 403 ng m-3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude and then transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai

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.

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

Climate and health effects of atmospheric aerosols are determined by their properties such as their chemical composition. Aerosol chemical composition can be studied indirectly by measuring volatility of aerosol particles. The volatility of submicron aerosol particles (20-500 nm) was studied in a boreal forest site at SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations II) station (Vesala et al., 1998) in Hyytiälä, Finland, during 01/2008-05/2010. The instrument used for the measurements was VDMPS (Volatility Differential Mobility Particle Sizer), which consists of two separate instruments: DMPS (Differential Mobility Particle Sizer, Aalto et al., 2001) and TD (Thermodenuder, Wehner et al., 2002). Aerosol evaporation was examined by heating the aerosol and comparing the total aerosol mass before and after heating. In the VDMPS system ambient aerosol sample was heated up to temperatures ranging from 80 °C to 280 °C. The higher the heating temperature was the more aerosol material was evaporated. There was a non-volatile residual present in aerosol particles when heated up to 280 °C. This residual explained (20±8)% of the total aerosol mass. Aerosol non-volatile mass fraction was highest during winter and smallest during summer months. The role of black carbon in the observed non-volatile residual was determined. Black carbon explained 40 to 90% of the non-volatile mass. Especially during colder seasons noticeable amount of non-volatile material, something else than black carbon, was observed. According to Kalberer et al. (2004) some atmospheric organic species can form polymers that have high evaporation temperatures. Also low-volatile organic salts may contribute to the non-volatile aerosol (Smith et al., 2010). Aerosol mass composition measured directly with AMS (Aerosol Mass Spectrometer, Jayne et al., 2000) was analyzed in order to examine the properties of the non-volatile material (other than black carbon). The AMS measurements were performed

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

Science.gov (United States)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

Absorbing Aerosols: Field and Laboratory Studies of Black Carbon and Dust

Science.gov (United States)

Aiken, A. C.; Flowers, B. A.; Dubey, M. K.

2011-12-01

Currently, absorbing aerosols are thought to be the most uncertain factor in atmospheric climate models (~0.4-1.2 W/m2), and the 2nd most important factor after CO2 in global warming (1.6 W/m2; Ramanathan and Carmichael, Nature Geoscience, 2008; Myhre, Science, 2009). While most well-recognized atmospheric aerosols, e.g., sulfate from power-plants, have a cooling effect on the atmosphere by scattering solar radiation, black carbon (BC or soot) absorbs sunlight strongly which results in a warming of the atmosphere. Dust particles are also present globally and can absorb radiation, contributing to a warmer and drier atmosphere. Direct on-line measurements of BC and hematite, an absorbing dust aerosol, can be made with the Single Particle Soot Photometer (SP2), which measures the mass of the particles by incandescence on an individual particle basis. Measurements from the SP2 are combined with absorption measurements from the three-wavelength photoacoustic soot spectrometer (PASS-3) at 405, 532, and 781 nm and the ultraviolet photoacoustic soot spectrometer (PASS-UV) at 375 nm to determine wavelength-dependent mass absorption coefficients (MACs). Laboratory aerosol samples include flame-generated soot, fullerene soot, Aquadag, hematite, and hematite-containing dusts. Measured BC MAC's compare well with published values, and hematite MAC's are an order of magnitude less than BC. Absorbing aerosols measured in the laboratory are compared with those from ambient aerosols measured during the Las Conchas fire and BEACHON-RoMBAS. The Las Conchas fire was a wildfire in the Jemez Mountains of New Mexico that burned over 100,000 acres during the Summer of 2011, and BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study) is a field campaign focusing on biogenic aerosols at the Manitou Forest Observatory near Colorado Springs, CO in Summer 2011. Optical properties and size

Total observed organic carbon (TOOC in the atmosphere: a synthesis of North American observations

Directory of Open Access Journals (Sweden)

C. L. Heald

2008-04-01

Full Text Available Measurements of organic carbon compounds in both the gas and particle phases made upwind, over and downwind of North America are synthesized to examine the total observed organic carbon (TOOC in the atmosphere over this region. These include measurements made aboard the NOAA WP-3 and BAe-146 aircraft, the NOAA research vessel Ronald H. Brown, and at the Thompson Farm and Chebogue Point surface sites during the summer 2004 ICARTT campaign. Both winter and summer 2002 measurements during the Pittsburgh Air Quality Study are also included. Lastly, the spring 2002 observations at Trinidad Head, CA, surface measurements made in March 2006 in Mexico City and coincidentally aboard the C-130 aircraft during the MILAGRO campaign and later during the IMPEX campaign off the northwestern United States are incorporated. Concentrations of TOOC in these datasets span more than two orders of magnitude. The daytime mean TOOC ranges from 4.0 to 456 μgC m⁻³ from the cleanest site (Trinidad Head to the most polluted (Mexico City. Organic aerosol makes up 3–17% of this mean TOOC, with highest fractions reported over the northeastern United States, where organic aerosol can comprise up to 50% of TOOC. Carbon monoxide concentrations explain 46 to 86% of the variability in TOOC, with highest TOOC/CO slopes in regions with fresh anthropogenic influence, where we also expect the highest degree of mass closure for TOOC. Correlation with isoprene, formaldehyde, methyl vinyl ketone and methacrolein also indicates that biogenic activity contributes substantially to the variability of TOOC, yet these tracers of biogenic oxidation sources do not explain the variability in organic aerosol observed over North America. We highlight the critical need to develop measurement techniques to routinely detect total gas phase VOCs, and to deploy comprehensive suites of TOOC instruments in diverse environments to quantify the ambient evolution of organic carbon from source

Source apportionment of carbonaceous aerosol in southern Sweden

Directory of Open Access Journals (Sweden)

J. Genberg

2011-11-01

Full Text Available A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM₁₀ were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (¹⁴C and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM₁₀ fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80%, which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32% and fossil fuel combustion (28% were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.

Desert dust and anthropogenic aerosol interactions in the Community Climate System Model coupled-carbon-climate model

Directory of Open Access Journals (Sweden)

N. Mahowald

2011-02-01

Full Text Available Coupled-carbon-climate simulations are an essential tool for predicting the impact of human activity onto the climate and biogeochemistry. Here we incorporate prognostic desert dust and anthropogenic aerosols into the CCSM3.1 coupled carbon-climate model and explore the resulting interactions with climate and biogeochemical dynamics through a series of transient anthropogenic simulations (20th and 21st centuries and sensitivity studies. The inclusion of prognostic aerosols into this model has a small net global cooling effect on climate but does not significantly impact the globally averaged carbon cycle; we argue that this is likely to be because the CCSM3.1 model has a small climate feedback onto the carbon cycle. We propose a mechanism for including desert dust and anthropogenic aerosols into a simple carbon-climate feedback analysis to explain the results of our and previous studies. Inclusion of aerosols has statistically significant impacts on regional climate and biogeochemistry, in particular through the effects on the ocean nitrogen cycle and primary productivity of altered iron inputs from desert dust deposition.

Atmospheric aerosol brown carbon in the high Himalayas

Science.gov (United States)

Kirillova, Elena; Decesari, Stefano; Marinoni, Angela; Bonasoni, Paolo; Vuillermoz, Elisa; Facchini, M. Cristina; Fuzzi, Sandro

2016-04-01

Anthropogenic light-absorbing atmospheric aerosol can reach very high concentrations in the planetary boundary layer in South-East Asia ("brown clouds"), affecting atmospheric transparency and generating spatial gradients of temperature over land with a possible impact on atmospheric dynamics and monsoon circulation. Besides black carbon (BC), an important light-absorbing component of anthropogenic aerosols is the organic carbon component known as 'brown carbon' (BrC). In this research, we provided first measurements of atmospheric aerosol BrC in the high Himalayas during different seasons. Aerosol sampling was conducted at the GAW-WMO Global station "Nepal Climate Observatory-Pyramid" (NCO-P) located in the high Khumbu valley at 5079 m a.s.l. in the foothills of Mt. Everest. PM10 aerosol samples were collected from July 2013 to November 2014. The sampling strategy was set up in order to discriminate the daytime valley breeze bringing polluted air masses up to the observatory and free tropospheric air during nighttime. Water-soluble BrC (WS-BrC) and methanol-soluble BrC (MeS-BrC) were extracted and analyzed using a UV/VIS spectrophotometer equipped with a 50 cm liquid waveguide capillary cell. In the polluted air masses, the highest levels of the BrC light absorption coefficient at 365 nm (babs365) were observed during the pre-monsoon season (1.83±1.46 Mm-1 for WS-BrC and 2.86±2.49 Mm-1 for MeS-BrC) and the lowest during the monsoon season (0.21±0.22 Mm-1 for WS-BrC and 0.32±0.29 Mm-1 for MeS-BrC). The pre-monsoon season is the most frequently influenced by a strong atmospheric brown cloud (ABC) transport to NCO-P due to increased convection and mixing layer height over South Asia combined with the highest up-valley wind speed and the increase of the emissions from open fires due to the agricultural practice along the Himalayas foothills and the Indo-Gangetic Plain. In contrast, the monsoon season is characterized by a weakened valley wind regime and an

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

International Nuclear Information System (INIS)

Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

1991-01-01

Smoke aerosol and background aerosol particles were collected from the controlled burning of boreal forest where vegetation species and relative mass distributions are known. Chemical mass balances were constructed for the total mass of carbonaceous aerosol particles emitted during the prescribed burn. In addition, a carbonaceous species inventory was developed for aerosol particles presnt under background, smoldering, and full-fire conditions; the production of organic carbon and elemental carbon particles is noted for these two fire regimes. Distributions of the solvent-soluble organic components of the sampled aerosols were generated to identify molecular properties that can be traced to unburned and pyrolyzed materials present in the boreal forest fuels

Probabilistic estimates of 1.5-degree carbon budgets based on uncertainty in transient climate response and aerosol forcing

Science.gov (United States)

Partanen, A. I.; Mengis, N.; Jalbert, J.; Matthews, D.

2017-12-01

Nations agreed to limit the increase in global mean surface temperature relative to the preindustrial era below 2 degrees Celsius and pursue efforts to a more ambitious goal of 1.5 degrees Celsius. To achieve these goals, it is necessary to assess the amount of cumulative carbon emissions compatible with these temperature targets, i.e. so called carbon budgets. In this work, we use the intermediate complexity University of Victoria Earth System Climate Model (UVic ESCM) to assess how uncertainty in aerosol forcing and transient climate response transfers to uncertainty in future carbon budgets for burning fossil fuels. We create a perturbed parameter ensemble of model simulations by scaling aerosol forcing and transient climate response, and assess the likelihood of each simulation by comparing the simulated historical cumulative carbon emissions, CO2 concentration and radiative balance to observations. By weighting the results of each simulation with the likelihood of the simulation, the preliminary results give a carbon budget of 48 Pg C to reach 1.5 degree Celsius temperature increase. The small weighted mean is due to large fraction of simulations with strong aerosol forcing and transient climate response giving negative carbon budgets for this time period. The probability of the carbon budget being over 100 Pg C was 38% and 23% for over 200 Pg carbon budget. The carbon budgets after temperature stabilization at 1.5 degrees are even smaller with a weighted mean of -100 Pg C until the year 2200. The main reason for the negative carbon budgets after temperature stabilization is an assumed strong decrease in aerosol forcing in the 21st century. Conversely, simulations with weak aerosol forcing and transient climate response give positive carbon budgets. Our results highlight both the importance of reducing uncertainty in aerosol forcing and transient climate response, and of taking the non-CO2 forcers into account when estimating carbon budgets.

Do Regional Aerosols Contribute to the Riverine Export of Dissolved Black Carbon?

Science.gov (United States)

Jones, M. W.; Quine, T. A.; de Rezende, C. E.; Dittmar, T.; Johnson, B.; Manecki, M.; Marques, J. S. J.; de Aragão, L. E. O. C.

2017-11-01

The fate of black carbon (BC), a stable form of thermally altered organic carbon produced during biomass and fuel combustion, remains an area of uncertainty in the global carbon cycle. The transfer of photosynthetically derived BC into extremely long-term oceanic storage is of particular significance and rivers are the key linkage between terrestrial sources and oceanic stores. Significant fluvial fluxes of dissolved BC to oceans result from the slow release of BC from degrading charcoal stocks; however, these fluvial fluxes may also include undetermined contributions of aerosol BC, produced by biomass and fossil fuel combustion, which are deposited in river catchments following atmospheric transport. By investigation of the Paraíba do Sul River catchment in Southeast Brazil we show that aerosol deposits can be substantial contributors to fluvial fluxes of BC. We derived spatial distributions of BC stocks within the catchment associated with soil charcoal and with aerosol from both open biomass burning and fuel combustion. We then modeled the fluvial concentrations of dissolved BC (DBC) in scenarios with varying rates of export from each stock. We analyzed the ability of each scenario to reproduce the variability in DBC concentrations measured in four data sets of river water samples collected between 2010 and 2014 and found that the best performing scenarios included a 5-18% (135-486 Mg DBC year-1) aerosol contribution. Our results suggest that aerosol deposits of BC in river catchments have a shorter residence time in catchments than charcoal BC and, therefore, contribute disproportionately (with respect to stock magnitude) toward fluvial fluxes of BC.

Mechanical desorption of immobilized proteins using carbon dioxide aerosols for reusable biosensors

International Nuclear Information System (INIS)

Singh, Renu; Hong, Seongkyeol; Jang, Jaesung

2015-01-01

Highlights: • Immobilized proteins were removed using carbon dioxide aerosols. • We observed high removal efficiencies due to the aerosol treatment. • We confirmed the removal with FTIR and X-ray photoelectron spectroscopy. • This CO 2 aerosol treatment did not undermine re-functionalization. • This technique is a fast and damage-free method to reuse a sensor surface. - Abstract: Reusability of a biosensor has recently received considerable attention, and it is closely related with the effective desorption of probe molecules. We present a novel mechanical desorption technique to reuse biosensors by using periodic jets of carbon dioxide (CO 2 ) aerosols (a mixture of solid and gaseous CO 2 ), and demonstrate its feasibility by removing physically adsorbed and covalently bonded fluorescent proteins i.e., Escherichia coli fluorescein isothiocyanate antibody and bovine serum albumin (E. coli FITC–Ab and FITC–BSA) from silicon chips. The proteins on the chip surfaces were measured by fluorescent images before and after applying the aerosols. The removal efficiency of the aerosol treatment was measured for various concentrations (1–20 μg mL −1 ) of E. coli FITC–Ab and FITC–BSA with two different removal cycles (5 and 11 cycles; each cycle: 8 s). We observed high removal efficiencies (>93.5% for physically adsorbed Ab and >84.6% for covalently bonded Ab) at 11 cycle aerosol treatment. This CO 2 aerosol treatment did not undermine re-functionalization, which was confirmed by the fluorescent images of FITC–Abs for fresh and reused chips. Desorption of the immobilized layers was validated by Fourier transform infrared and X-ray photoelectron spectroscopic analyses. We also conducted an experiment on the regeneration of E. coli sensing chips using this aerosol treatment, and the chips were re-used 5 times successfully. This mechanical desorption technique is a highly effective and novel strategy for reusable biosensors

Diurnal variations of organic molecular tracers and stable carbon isotopic composition in atmospheric aerosols over Mt. Tai in the North China Plain: an influence of biomass burning

Science.gov (United States)

Fu, P. Q.; Kawamura, K.; Chen, J.; Li, J.; Sun, Y. L.; Liu, Y.; Tachibana, E.; Aggarwal, S. G.; Okuzawa, K.; Tanimoto, H.; Kanaya, Y.; Wang, Z. F.

2012-09-01

Organic tracer compounds, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated in aerosol samples collected during early and late periods of the Mount Tai eXperiment 2006 (MTX2006) field campaign in the North China Plain. Total solvent-extractable fractions were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in the North China Plain were very active, the total identified organics (2090 ± 1170 ng m-3) were double those in late June (926 ± 574 ng m-3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88-1210 ng m-3, mean 403 ng m-3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude, which could be further transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the

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.

Aerosol Absorption by Black Carbon and Dust: Implications of Climate Change and Air Quality in Asia

Science.gov (United States)

Chin, Mian

2010-01-01

Atmospheric aerosol distributions from 2000 to 2007 are simulated with the global model GOCART to attribute light absorption by aerosol to its composition and sources. We show the seasonal and interannual variations of absorbing aerosols in the atmosphere over Asia, mainly black carbon and dust. and their linkage to the changes of anthropogenic and dust emissions in the region. We compare our results with observations from satellite and ground-based networks, and estimate the importance of black carbon and dust on regional climate forcing and air quality.

Mechanical desorption of immobilized proteins using carbon dioxide aerosols for reusable biosensors

Energy Technology Data Exchange (ETDEWEB)

Singh, Renu; Hong, Seongkyeol [School of Mechanical and Nuclear Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798 (Korea, Republic of); Jang, Jaesung, E-mail: jjang@unist.ac.kr [School of Mechanical and Nuclear Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798 (Korea, Republic of); Department of Biomedical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798 (Korea, Republic of); School of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798 (Korea, Republic of)

2015-01-01

Highlights: • Immobilized proteins were removed using carbon dioxide aerosols. • We observed high removal efficiencies due to the aerosol treatment. • We confirmed the removal with FTIR and X-ray photoelectron spectroscopy. • This CO{sub 2} aerosol treatment did not undermine re-functionalization. • This technique is a fast and damage-free method to reuse a sensor surface. - Abstract: Reusability of a biosensor has recently received considerable attention, and it is closely related with the effective desorption of probe molecules. We present a novel mechanical desorption technique to reuse biosensors by using periodic jets of carbon dioxide (CO{sub 2}) aerosols (a mixture of solid and gaseous CO{sub 2}), and demonstrate its feasibility by removing physically adsorbed and covalently bonded fluorescent proteins i.e., Escherichia coli fluorescein isothiocyanate antibody and bovine serum albumin (E. coli FITC–Ab and FITC–BSA) from silicon chips. The proteins on the chip surfaces were measured by fluorescent images before and after applying the aerosols. The removal efficiency of the aerosol treatment was measured for various concentrations (1–20 μg mL{sup −1}) of E. coli FITC–Ab and FITC–BSA with two different removal cycles (5 and 11 cycles; each cycle: 8 s). We observed high removal efficiencies (>93.5% for physically adsorbed Ab and >84.6% for covalently bonded Ab) at 11 cycle aerosol treatment. This CO{sub 2} aerosol treatment did not undermine re-functionalization, which was confirmed by the fluorescent images of FITC–Abs for fresh and reused chips. Desorption of the immobilized layers was validated by Fourier transform infrared and X-ray photoelectron spectroscopic analyses. We also conducted an experiment on the regeneration of E. coli sensing chips using this aerosol treatment, and the chips were re-used 5 times successfully. This mechanical desorption technique is a highly effective and novel strategy for reusable biosensors.

Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

Energy Technology Data Exchange (ETDEWEB)

Massachusetts Institute of Technology; Kroll, Jesse H.; Donahue, Neil M.; Jimenez, Jose L.; Kessler, Sean H.; Canagaratna, Manjula R.; Wilson, Kevin R.; Altieri, Katye E.; Mazzoleni, Lynn R.; Wozniak, Andrew S.; Bluhm, Hendrik; Mysak, Erin R.; Smith, Jared D.; Kolb, Charles E.; Worsnop, Douglas R.

2010-11-05

A detailed understanding of the sources, transformations, and fates of organic species in the environment is crucial because of the central roles that organics play in human health, biogeochemical cycles, and Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state (OSC), a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of OSC , using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number (nC).

Characterization of urban aerosol in Cork city (Ireland) using aerosol mass spectrometry

Science.gov (United States)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Kourtchev, I.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2013-05-01

Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC), sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS) and was also found to comprise organic aerosol as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA) comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA) comprised 18%, "biomass burning" organic aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA) comprised 21%, and finally a species type characterized by primary {m/z} peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA), but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively).

Characterization of urban aerosol in Cork city (Ireland using aerosol mass spectrometry

Directory of Open Access Journals (Sweden)

M. Dall'Osto

2013-05-01

Full Text Available Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC, sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS and was also found to comprise organic aerosol as the most abundant species (62%, followed by nitrate (15%, sulphate (9% and ammonium (9%, and chloride (5%. Positive matrix factorization (PMF was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA comprised 18%, "biomass burning" organic aerosol (BBOA comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA comprised 21%, and finally a species type characterized by primary extit{m/z}~peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA, but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively.

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.

Diurnal variations of organic molecular tracers and stable carbon isotopic composition in atmospheric aerosols over Mt. Tai in the North China Plain: an influence of biomass burning

Directory of Open Access Journals (Sweden)

P. Q. Fu

2012-09-01

Full Text Available Organic tracer compounds, as well as organic carbon (OC, elemental carbon (EC, water-soluble organic carbon (WSOC, and stable carbon isotope ratios (δ¹³C of total carbon (TC have been investigated in aerosol samples collected during early and late periods of the Mount Tai eXperiment 2006 (MTX2006 field campaign in the North China Plain. Total solvent-extractable fractions were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs. In early June when the field burning activities of wheat straws in the North China Plain were very active, the total identified organics (2090 ± 1170 ng m⁻³ were double those in late June (926 ± 574 ng m⁻³. All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m⁻³, mean 403 ng m⁻³ was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude, which could be further transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary

Total Volcanic Stratospheric Aerosol Optical Depths and Implications for Global Climate Change

Science.gov (United States)

Ridley, D. A.; Solomon, S.; Barnes, J. E.; Burlakov, V. D.; Deshler, T.; Dolgii, S. I.; Herber, A. B.; Nagai, T.; Neely, R. R., III; Nevzorov, A. V.;

Monitoring of organic and elemental carbon (OC/EC) in the atmospheric aerosol

Energy Technology Data Exchange (ETDEWEB)

Hannemann, A.; Fuchs, J.; Jaeschke, W.; Weingartner, E.; Baltensperger, U.

2003-03-01

A new instrument for the measurement of ambient carbonaceous aerosol concentrations is described, which enables discrimination between organic and elemental carbon on a semi-continuous basis. (author)

Effect of variable power levels on the yield of total aerosol mass and formation of aldehydes in e-cigarette aerosols.

Science.gov (United States)

Gillman, I G; Kistler, K A; Stewart, E W; Paolantonio, A R

2016-03-01

The study objective was to determine the effect of variable power applied to the atomizer of refillable tank based e-cigarette (EC) devices. Five different devices were evaluated, each at four power levels. Aerosol yield results are reported for each set of 25 EC puffs, as mass/puff, and normalized for the power applied to the coil, in mass/watt. The range of aerosol produced on a per puff basis ranged from 1.5 to 28 mg, and, normalized for power applied to the coil, ranged from 0.27 to 1.1 mg/watt. Aerosol samples were also analyzed for the production of formaldehyde, acetaldehyde, and acrolein, as DNPH derivatives, at each power level. When reported on mass basis, three of the devices showed an increase in total aldehyde yield with increasing power applied to the coil, while two of the devices showed the opposite trend. The mass of formaldehyde, acetaldehyde, and acrolein produced per gram of total aerosol produced ranged from 0.01 to 7.3 mg/g, 0.006 to 5.8 mg/g, and acrolein from EC aerosols from specific devices, and were compared to estimated exposure from consumption of cigarettes, to occupational and workplace limits, and to previously reported results from other researchers. Copyright © 2015 The Authors. Published by Elsevier Inc. All rights reserved.

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

Black carbon's contribution to aerosol absorption optical depth over S. Korea

Science.gov (United States)

Lamb, K.; Perring, A. E.; Beyersdorf, A. J.; Anderson, B. E.; Segal-Rosenhaimer, M.; Redemann, J.; Holben, B. N.; Schwarz, J. P.

2017-12-01

Aerosol absorption optical depth (AAOD) monitored by ground-based sites (AERONET, SKYNET, etc.) is used to constrain climate radiative forcing from black carbon (BC) and other absorbing aerosols in global models, but few validation studies between in situ aerosol measurements and ground-based AAOD exist. AAOD is affected by aerosol size distributions, composition, mixing state, and morphology. Megacities provide appealing test cases for this type of study due to their association with very high concentrations of anthropogenic aerosols. During the KORUS-AQ campaign in S. Korea, which took place in late spring and early summer of 2016, in situ aircraft measurements over the Seoul Metropolitan Area and Taehwa Research Forest (downwind of Seoul) were repeated three times per flight over a 6 week period, providing significant temporal coverage of vertically resolved aerosol properties influenced by different meteorological conditions and sources. Measurements aboard the NASA DC-8 by the NOAA Humidified Dual Single Particle Soot Photometers (HD-SP2) quantified BC mass, size distributions, mixing state, and the hygroscopicity of BC containing aerosols. The in situ BC mass vertical profiles are combined with estimated absorption enhancement calculated from observed optical size and hygroscopicity using Mie theory, and then integrated over the depth of the profile to calculate BC's contribution to AAOD. Along with bulk aerosol size distributions and hygroscopicity, bulk absorbing aerosol optical properties, and on-board sky radiance measurements, these measurements are compared with ground-based AERONET site measurements of AAOD to evaluate closure between in situ vertical profiles of BC and AAOD measurements. This study will provide constraints on the relative importance of BC (including lensing and hygroscopicity effects) and non-BC components to AAOD over S. Korea.

Aerosol measurements from plasma torch cuts on stainless steel, carbon steel, and aluminum

International Nuclear Information System (INIS)

Novick, V.J.; Brodrick, C.J.; Crawford, S.; Nasiatka, J.; Pierucci, K.; Reyes, V.; Sambrook, J.; Wrobel, S.; Yeary, J.

1996-01-01

The main purpose of this project is to quantify aerosol particle size and generation rates produced by a plasma torch whencutting stainless steel, carbon steel and aluminum. the plasma torch is a common cutting tool used in the dismantling of nuclear facilities. Eventually, other cutting tools will be characterized and the information will be compiled in a user guide to aid in theplanning of both D ampersand D and other cutting operations. The data will be taken from controlled laboratory experiments on uncontaminated metals and field samples taken during D ampersand D operations at ANL nuclear facilities. The plasma torch data was collected from laboratory cutting tests conducted inside of a closed, filtered chamber. The particle size distributions were determined by isokinetically sampling the exhaust duct using a cascade impactor. Cuts on different thicknesses showed there was no observable dependence of the aerosol quantity produced as a function of material thickness for carbon steel. However, data for both stainless steel and aluminum revealed that the aerosol mass produced for these materials appear to have some dependance on thickness, with thinner materials producing tmore aerosols. The results of the laboratory cutting tests show that most measured particle size distributions are bimodal with one mode at about 0.2 μm and the other at about 10 μm. The average Mass Median Aerodynamic Diameters (MMAD's) for these tests are 0.36 ±0.08 μm for stainless steel, 0.48 ±0.17μm for aluminum and 0.52±0.12 μm for carbon steel

Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbon isotope analysis

Science.gov (United States)

Ceburnis, D.; Garbaras, A.; Szidat, S.; Rinaldi, M.; Fahrni, S.; Perron, N.; Wacker, L.; Leinert, S.; Remeikis, V.; Facchini, M. C.; Prevot, A. S. H.; Jennings, S. G.; O'Dowd, C. D.

2011-01-01

Dual carbon isotope analysis has been performed for the first time demonstrating a potential in organic matter apportionment between three principal sources: marine, terrestrial (non-fossil) and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides a conclusive evidence of a dominant biogenic organic fraction to organic aerosol over biologically active oceans. In particular, the NE Atlantic, which is also subjected to notable anthropogenic influences via pollution transport processes, was found to contain 80% organic aerosol matter of biogenic origin directly linked to plankton emissions. The remaining carbonaceous aerosol was of fossil-fuel origin. By contrast, for polluted air advecting out from Europe into the NE Atlantic, the source apportionment is 30% marine biogenic, 40% fossil fuel, and 30% continental non-fossil fuel. The dominant marine organic aerosol source in the atmosphere has significant implications for climate change feedback processes.

Long term change in atmospheric dust absorption, dust scattering and black carbon aerosols scattering coefficient parameters over western Indian locations

Science.gov (United States)

Satoliya, Anil Kumar; Vyas, B. M.; Shekhawat, M. S.

2018-05-01

The first time satellite space based measurement of atmospheric black carbon (BC) aerosols scattering coefficient at 550nm (BC SC at 550nm), dust aerosols scattering and dust aerosols extinction coefficient (DSC at 550nm and DEC at 550nm) parameters have been used to understand their long term trend of natural and anthropogenic aerosols behavior with its close association with ground based measured precipitation parameters such as Total Rain Fall (TRF), and Total Number of Rainy Days (TNRD) for the same period over western Indian regions concerned to the primary aerosols sources of natural activities. The basic objective of this study is an attempt to investigate the inter-correlation between dust and black carbon aerosols loading characteristics with a variation of rainfall pattern parameters as indirect aerosols induced effect i.e., aerosols-cloud interaction. The black carbon aerosols generated by diverse anthropogenic or human made activities are studied by choosing of measured atmospheric BC SC at 550nm parameter, whereas desert dust mineral aerosols primarily produced by varieties of natural activities pre-dominated of dust mineral desert aerosols mainly over Thar desert influenced area of hot climate and rural tropical site are investigated by selecting DSC at 550nm and DEC at 550nm of first semi-urban site i.e., Udaipur (UDP, 24.6°N, 73.35°E, 580m above surface level (asl)) situated in southern Rajasthan part as well as over other two Great Indian Thar desert locations i.e., Jaisalmer (JSM, 26.90°N, 69.90°E, 220m asl)) and Bikaner (BKN, 28.03°N, 73.30°E, 224m asl) located in the vicinity of the Thar desert region situated in Rajasthan state of the western Indian region. The source of the present study would be collection of longer period of monthly values of the above parameters of spanning 35 years i.e., 1980 to 2015. Such types of atmospheric aerosols-cloud monsoon interaction investigation is helpful in view of understanding their direct and

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.

Elemental and organic carbon in aerosols over urbanized coastal region (southern Baltic Sea, Gdynia).

Science.gov (United States)

Lewandowska, Anita; Falkowska, Lucyna; Murawiec, Dominika; Pryputniewicz, Dorota; Burska, Dorota; Bełdowska, Magdalena

2010-09-15

Studies on PM 10, total particulate matter (TSP), elemental carbon (EC) and organic carbon (OC) concentrations were carried out in the Polish coastal zone of the Baltic Sea, in urbanized Gdynia. The interaction between the land, the air and the sea was clearly observed. The highest concentrations of PM 10, TSP and both carbon fractions were noted in the air masses moving from southern and western Poland and Europe. The EC was generally of primary origin and its contribution to TSP and PM 10 mass was on average 2.3% and 3.7% respectively. Under low wind speed conditions local sources (traffic and industry) influenced increases in elemental carbon and PM 10 concentrations in Gdynia. Elemental carbon demonstrated a pronounced weekly cycle, yielding minimum values at the weekend and maximum values on Thursdays. The role of harbors and ship yards in creating high EC concentrations was clearly observed. Concentration of organic carbon was ten times higher than that of elemental carbon, and the average OC contribution to PM 10 mass was very high (31.6%). An inverse situation was observed when air masses were transported from over the Atlantic Ocean, the North Sea and the Baltic Sea. These clean air masses were characterized by the lowest concentrations of all analysed compounds. Obtained results for organic and elemental carbon fluxes showed that atmospheric aerosols can be treated, along with water run-off, as a carbon source for the coastal waters of the Baltic Sea. The enrichment of surface water was more effective in the case of organic carbon (0.27+/-0.19 mmol m(-2) d(-1)). Elemental carbon fluxes were one order of magnitude smaller, on average 0.03+/-0.04 mmol m(-2) d(-1). We suggest that in some situations atmospheric carbon input can explain up to 18% of total carbon fluxes into the Baltic coastal waters. Copyright 2010 Elsevier B.V. All rights reserved.

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.

Relationships between Personal Measurements of 'Total' Dust, Respirable, Thoracic, and Inhalable Aerosol Fractions in the Cement Production Industry.

Science.gov (United States)

Notø, Hilde P; Nordby, Karl-Christian; Eduard, Wijnand

2016-05-01

The aims of this study were to examine the relationships and establish conversion factors between 'total' dust, respirable, thoracic, and inhalable aerosol fractions measured by parallel personal sampling on workers from the production departments of cement plants. 'Total' dust in this study refers to aerosol sampled by the closed face 37-mm Millipore filter cassette. Side-by-side personal measurements of 'total' dust and respirable, thoracic, and inhalable aerosol fractions were performed on workers in 17 European and Turkish cement plants. Simple linear and mixed model regressions were used to model the associations between the samplers. The total number of personal samples collected on 141 workers was 512. Of these 8.4% were excluded leaving 469 for statistical analysis. The different aerosol fractions contained from 90 to 130 measurements and-side-by side measurements of all four aerosol fractions were collected on 72 workers.The median ratios between observed results of the respirable, 'total' dust, and inhalable fractions relative to the thoracic aerosol fractions were 0.51, 2.4, and 5.9 respectively. The ratios between the samplers were not constant over the measured concentration range and were best described by regression models. Job type, position of samplers on left or right shoulder and plant had no substantial effect on the ratios. The ratios between aerosol fractions changed with different air concentrations. Conversion models for estimation of the fractions were established. These models explained a high proportion of the variance (74-91%) indicating that they are useful for the estimation of concentrations based on measurements of a different aerosol fraction. The calculated uncertainties at most observed concentrations were below 30% which is acceptable for comparison with limit values (EN 482, 2012). The cement industry will therefore be able to predict the health related aerosol fractions from their former or future measurements of one of the

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)

Air pollution studies in terms of particulate matters, elements and black carbon in the aerosols collected at Andravoahangy-Antananarivo

International Nuclear Information System (INIS)

HARINOELY, M.

2012-01-01

This work was performed at the Institut National des Sciences et Techniques Nucleaires (Madagascar-INSTN) in the framework of RAF/4/019 project organized by the International Atomic Energy Agency. The main objective of this work is to study the level of air pollution in terms of particulate matters, elements and black carbon in the site of Andravoahangy-Antananarivo and to transmit the results obtained to the competent authorities so that they can make decisions to reduce the impacts of air pollution on the population. The total reflection X-ray fluorescence spectrometer is used for qualitative and quantitative analyses of the elements contained in the aerosols and the reflectometer M43D for the determination of the black carbon concentrations. The results showed that the average concentrations of the particulate matters PM 2,5-10 are higher than those of PM 2,5 . The average concentrations of PM 10 in the aerosols are exceeding the World Health Organisation (WHO) and European Union guidelines, set at 50 μg.m -3 and those of PM 2,5 are higher than the 2005 WHO (25 μg.m -3 ) and the United States Environmental Protection Agency (35 μg.m -3 ) guidelines. The identified elements in the aerosols are Ti, Cr, Mn, Fe, Ni, Cu, Zn, Br, Sr and Pb. The average concentrations of these elements are also higher in the coarse particles than in the fine particles. The concentrations of black carbon are higher in the fine particles, with a maximum value of 9.12 μg.m -3 . [fr

403 nm cavity ring-down measurements of brown carbon aerosol

Science.gov (United States)

Kwon, D.; Grassian, V. H.; Kleiber, P.; Young, M. A.

2017-12-01

Atmospheric aerosol influences Earth's climate by absorbing and scattering incoming solar radiation and outgoing terrestrial radiation. One class of secondary organic aerosol (SOA), called brown carbon (BrC), has attracted attention for its wavelength dependent light absorbing properties with absorption coefficients that generally increase from the visible (Vis) to ultraviolet (UV) regions. Here we report results from our investigation of the optical properties of BrC aerosol products from the aqueous phase reaction of ammonium sulfate (AS) with methylglyoxal (MG) using cavity ring-down spectroscopy (CRDS) at 403 nm wavelength. We have measured the optical constants of BrC SOA from the AS/MG reaction as a function of reaction time. Under dry flow conditions, we observed no apparent variation in the BrC refractive index with aging over the course of 22 days. The retrieved BrC optical constants are similar to those of AS with n = 1.52 for the real component. Despite significant UV absorption observed from the bulk BrC solution, the imaginary index value at 403 nm is below our minimum detection limit which puts an upper bound of k as 0.03. These observations are in agreement with results from our recent studies of the light scattering properties of this BrC aerosol.

Sources of carbonaceous aerosol in the Amazon basin

Directory of Open Access Journals (Sweden)

S. Gilardoni

2011-03-01

Full Text Available The quantification of sources of carbonaceous aerosol is important to understand their atmospheric concentrations and regulating processes and to study possible effects on climate and air quality, in addition to develop mitigation strategies.

In the framework of the European Integrated Project on Aerosol Cloud Climate Interactions (EUCAARI fine (D_p < 2.5 μm and coarse (2.5 μm < D_p <10 μm aerosol particles were sampled from February to June (wet season and from August to September (dry season 2008 in the central Amazon basin. The mass of fine particles averaged 2.4 μg m⁻³ during the wet season and 4.2 μg m⁻³ during the dry season. The average coarse aerosol mass concentration during wet and dry periods was 7.9 and 7.6 μg m⁻³, respectively. The overall chemical composition of fine and coarse mass did not show any seasonality with the largest fraction of fine and coarse aerosol mass explained by organic carbon (OC; the average OC to mass ratio was 0.4 and 0.6 in fine and coarse aerosol modes, respectively. The mass absorbing cross section of soot was determined by comparison of elemental carbon and light absorption coefficient measurements and it was equal to 4.7 m² g⁻¹ at 637 nm. Carbon aerosol sources were identified by Positive Matrix Factorization (PMF analysis of thermograms: 44% of fine total carbon mass was assigned to biomass burning, 43% to secondary organic aerosol (SOA, and 13% to volatile species that are difficult to apportion. In the coarse mode, primary biogenic aerosol particles (PBAP dominated the carbonaceous aerosol mass. The results confirmed the importance of PBAP in forested areas.

The source apportionment results were employed to evaluate the ability of global chemistry transport models to simulate carbonaceous aerosol sources in a regional tropical background site. The comparison showed an overestimation

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

International Nuclear Information System (INIS)

Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

1990-10-01

The identity and ambient mass concentrations of radiatively important carbonaceous aerosols were measured for a boreal forest prescribed burn conducted in northern Ontario, CAN in August 1989. Nonsize-segregated airborne particles were collected for smoldering-fire and full-fire conditions using a helicopter sampling platform. Total carbon (TC), organic carbon (OC) and elemental carbon (EC) were measured. Smoke plume mass concentrations of the OC and EC particles were greatest for full-fire conditions and had ranges of 1.560 to 2.160 mg/m -1 (OC) and 0.120 to 0.160 mg/m -3 (EC) with OC:EC ratios of 10 to 18, respectively. Smoldering fire conditions showed smoke plume OC and EC levels of 0.570--1.030 mg/m -3 (OC) and 0.006--0.050 mg/m -3 (EC) and much higher ratios of OC:EC (21 to 95). These aerosol data indicate the formation of EC particles is greatest during full-fire combustion of boreal forest material relative to smoldering combustion. However, EC particles comprise a minor fraction of the particulate carbon smoke aerosols for both full-fire and smoldering conditions; the major component of carbonaceous smoke aerosols emitted during the prescribed burn is OC. Overall, the OC and EC in-plume smoke aerosol data show nonuniform production of these particles during various stages of the prescribed burn, and major differences in the type of carbonaceous aerosol that is generated (OC versus EC)

The absorption budget of fresh biomass burning aerosol from realistic laboratory fires

Science.gov (United States)

Wagner, N. L.; Adler, G. A.; Franchin, A.; Lamb, K.; Manfred, K.; Middlebrook, A. M.; Selimovic, V.; Schwarz, J. P.; Washenfelder, R. A.; Womack, C.; Yokelson, R. J.

2017-12-01

Wildfires are expected to increase globally due to climate change. The smoke from these wildfires has a highly uncertain radiative effect, largely due to the lack of detailed understanding of its optical properties. As part of the NOAA FIREX project, we have measured the optical properties of smoke primarily from laboratory burning of North American fuels at the Missoula Fire Sciences Laboratory. Here, we present a budget of the aerosol absorption from a portion of the laboratory fires. The total aerosol absorption was measured with photoacoustic spectrometers (PAS) at four wavelengths (405 nm, 532 nm, 660 nm, 870 nm) spanning the visible spectral region. The aerosol absorption is attributed to black carbon which absorbs broadly across the visible and ultraviolet (UV) spectral region and brown carbon (BrC) which absorbs in the blue and UV spectral regions. Then aerosol absorption measurements are compared with measurements of refractory black carbon (rBC) concentration by laser induced incandescence (SP2) and measurements of BrC concentration from a particle-into-liquid sampler coupled to a liquid absorption cell (BrC-PILS). Periodically, a thermodenuder was inserted upstream of all of the instruments to constrain the relationship between aerosol volatility and absorption. We synthesize these measurements to constrain the various contributors to total absorption including effects of lensing on rBC absorption, and of BrC that is not volatilized in the thermodenuder.

SCIAMACHY WFM-DOAS XCO2: comparison with CarbonTracker XCO2 focusing on aerosols and thin clouds

Directory of Open Access Journals (Sweden)

J. P. Burrows

2012-08-01

Full Text Available Carbon dioxide (CO2 is the most important greenhouse gas whose atmospheric loading has been significantly increased by anthropogenic activity leading to global warming. Accurate measurements and models are needed in order to reliably predict our future climate. This, however, has challenging requirements. Errors in measurements and models need to be identified and minimised. In this context, we present a comparison between satellite-derived column-averaged dry air mole fractions of CO2, denoted XCO2, retrieved from SCIAMACHY/ENVISAT using the WFM-DOAS (weighting function modified differential optical absorption spectroscopy algorithm, and output from NOAA's global CO2 modelling and assimilation system CarbonTracker. We investigate to what extent differences between these two data sets are influenced by systematic retrieval errors due to aerosols and unaccounted clouds. We analyse seven years of SCIAMACHY WFM-DOAS version 2.1 retrievals (WFMDv2.1 using CarbonTracker version 2010. We investigate to what extent the difference between SCIAMACHY and CarbonTracker XCO2 are temporally and spatially correlated with global aerosol and cloud data sets. For this purpose, we use a global aerosol data set generated within the European GEMS project, which is based on assimilated MODIS satellite data. For clouds, we use a data set derived from CALIOP/CALIPSO. We find significant correlations of the SCIAMACHY minus CarbonTracker XCO2 difference with thin clouds over the Southern Hemisphere. The maximum temporal correlation we find for Darwin, Australia (r2 = 54%. Large temporal correlations with thin clouds are also observed over other regions of the Southern Hemisphere (e.g. 43% for South America and 31% for South Africa. Over the Northern Hemisphere the temporal correlations are typically much lower. An exception is India, where large temporal correlations with clouds and aerosols have also been found. For all other regions the temporal correlations with

{sup 14}C content in aerosols in Mexico City

Energy Technology Data Exchange (ETDEWEB)

Gómez, V.; Solís, C.; Chávez, E.; Andrade, E.; Ortiz, M.E.; Huerta, A.; Aragón, J.; Rodríguez-Ceja, M. [Instituto de Física, Universidad Nacional Autónoma de México, Apartado Postal 20-364, México, D.F. 01000 (Mexico); Martínez, M.A. [Facultad de Ciencias, Universidad Nacional Autónoma de México (Mexico); Ortiz, E. [Universidad Autónoma Metropolitana-Azcapotzalco, Av. San Pablo 180, C. P. 02200 México, D.F. (Mexico)

2016-03-15

{sup 14}C-AMS of total carbon was determined in aerosols (PM{sub 10} fraction), collected in Mexico City during two weeks from 21 November to 3 December 2012. Other tracers such as total carbon (TC), organic carbon (OC), elemental carbon (EC) and trace element contents were also determined. F{sup 14}C values varied from 0.39 to 0.48 with an average of 0.43. These values are slightly lower than those previously obtained for PM{sub 2.5} in 2003 and 2006 and reflect a high contribution of fossil CO{sub 2} to the carbonaceous matter in aerosols from Mexico City. In contrast, from 2006 to 2012 PM{sub 10} increased; EC, Ca, Ti and Fe concentrations remained constant, while OC, TC and K concentrations decreased. The use of potassium as an indicator of biomass burning showed that this source was negligible during this campaign. Combined analytical approaches allowed us to distinguish temporal variations of anthropogenic and natural inputs to the F{sup 14}C.

Carbonaceous Aerosols in Fine Particulate Matter of Santiago Metropolitan Area, Chile

Science.gov (United States)

Toro Araya, Richard; Flocchini, Robert; Morales Segura, Rául G. E.; Leiva Guzmán, Manuel A.

2014-01-01

Measurements of carbonaceous aerosols in South American cities are limited, and most existing data are of short term and limited to only a few locations. For 6 years (2002–2007), concentrations of fine particulate matter and organic and elemental carbon were measured continuously in the capital of Chile. The contribution of carbonaceous aerosols to the primary and secondary fractions was estimated at three different sampling sites and in the warm and cool seasons. The results demonstrate that there are significant differences in the levels in both the cold (March to August) and warm (September to February) seasons at all sites studied. The percent contribution of total carbonaceous aerosol fine particulate matter was greater in the cool season (53 ± 41%) than in the warm season (44 ± 18%). On average, the secondary organic carbon in the city corresponded to 29% of the total organic carbon. In cold periods, this proportion may reach an average of 38%. A comparison of the results with the air quality standards for fine particulate matter indicates that the total carbonaceous fraction alone exceeds the World Health Organization standard (10 µg/m3) and the United States Environmental Protection Agency standard (15 µg/m3) for fine particulate matter. PMID:24587753

Carbonaceous Aerosols in Fine Particulate Matter of Santiago Metropolitan Area, Chile

Directory of Open Access Journals (Sweden)

Richard Toro Araya

2014-01-01

Full Text Available Measurements of carbonaceous aerosols in South American cities are limited, and most existing data are of short term and limited to only a few locations. For 6 years (2002–2007, concentrations of fine particulate matter and organic and elemental carbon were measured continuously in the capital of Chile. The contribution of carbonaceous aerosols to the primary and secondary fractions was estimated at three different sampling sites and in the warm and cool seasons. The results demonstrate that there are significant differences in the levels in both the cold (March to August and warm (September to February seasons at all sites studied. The percent contribution of total carbonaceous aerosol fine particulate matter was greater in the cool season (53 ± 41% than in the warm season (44 ± 18%. On average, the secondary organic carbon in the city corresponded to 29% of the total organic carbon. In cold periods, this proportion may reach an average of 38%. A comparison of the results with the air quality standards for fine particulate matter indicates that the total carbonaceous fraction alone exceeds the World Health Organization standard (10 µg/m3 and the United States Environmental Protection Agency standard (15 µg/m3 for fine particulate matter.

Carbonaceous aerosols in fine particulate matter of Santiago Metropolitan Area, Chile.

Science.gov (United States)

Toro Araya, Richard; Flocchini, Robert; Morales Segura, Rául G E; Leiva Guzmán, Manuel A

2014-01-01

Measurements of carbonaceous aerosols in South American cities are limited, and most existing data are of short term and limited to only a few locations. For 6 years (2002-2007), concentrations of fine particulate matter and organic and elemental carbon were measured continuously in the capital of Chile. The contribution of carbonaceous aerosols to the primary and secondary fractions was estimated at three different sampling sites and in the warm and cool seasons. The results demonstrate that there are significant differences in the levels in both the cold (March to August) and warm (September to February) seasons at all sites studied. The percent contribution of total carbonaceous aerosol fine particulate matter was greater in the cool season (53 ± 41%) than in the warm season (44 ± 18%). On average, the secondary organic carbon in the city corresponded to 29% of the total organic carbon. In cold periods, this proportion may reach an average of 38%. A comparison of the results with the air quality standards for fine particulate matter indicates that the total carbonaceous fraction alone exceeds the World Health Organization standard (10 µg/m(3)) and the United States Environmental Protection Agency standard (15 µg/m(3)) for fine particulate matter.

Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-07-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

Science.gov (United States)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

PM2.5 and aerosol black carbon in Suva, Fiji

Science.gov (United States)

Isley, C. F.; Nelson, P. F.; Taylor, M. P.; Mani, F. S.; Maata, M.; Atanacio, A.; Stelcer, E.; Cohen, D. D.

2017-02-01

Concentrations of particulate air pollution in Suva, Fiji, have been largely unknown and consequently, current strategies to reduce health risk from air pollution in Suva are not targeted effectively. This lack of air quality data is common across the Pacific Island Countries. A monitoring study, during 2014 and 2015, has characterised the fine particulate air quality in Suva, representing the most detailed study to date of fine aerosol air pollutants for the Pacific Islands; with sampling at City, Residential (Kinoya) and Background (Suva Point) sites. Meteorology for Suva, as it relates to pollutant dispersion for this period of time, has also been analysed. The study design enables the contribution of maritime air and the anthropogenic emissions to be carefully distinguished from each other and separately characterised. Back trajectory calculations show that a packet of air sampled at the Suva City site has typically travelled 724 km in the 24-h prior to sampling, mainly over open ocean waters; inferring that pollutants would also be rapidly transported away from Suva. For fine particulates, Suva City reported a mid-week PM2.5 of 8.6 ± 0.4 μg/m3, averaged over 13-months of gravimetric sampling. Continuous monitoring (Osiris laser photometer) suggests that some areas of Suva may experience levels exceeding the WHO PM2.5 guideline of 10 μg/m3, however, compared to other countries, Fiji's PM2.5 is low. Peak aerosol particulate levels, at all sites, were experienced at night-time, when atmospheric conditions were least favourable to dispersion of air pollutants. Suva's average ambient concentrations of black carbon in PM2.5, 2.2 ± 0.1 μg/m3, are, however, similar to those measured in much larger cities. With any given parcel of air spending only seven minutes, on average, over the land area of Suva Peninsula, these black carbon concentrations are indicative that significant combustion emissions occur within Suva. Many other communities in the Pacific Islands

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

Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

OpenAIRE

Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

2016-01-01

Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in...

Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-04-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

Light-Absorbing Brown Carbon Aerosol Constituents from Combustion of Indonesian Peat and Biomass.

Science.gov (United States)

Budisulistiorini, Sri Hapsari; Riva, Matthieu; Williams, Michael; Chen, Jing; Itoh, Masayuki; Surratt, Jason D; Kuwata, Mikinori

2017-04-18

Light-absorbing brown carbon (BrC) constituents of organic aerosol (OA) have been shown to significantly absorb ultraviolet (UV) and visible light and thus impact radiative forcing. However, molecular identification of the BrC constituents is still limited. In this study, we characterize BrC constituents at the molecular level in (i) aerosols emitted by combustion of peat, fern/leaf, and charcoal from Indonesia and (ii) ambient aerosols collected in Singapore during the 2015 haze episode. Aerosols were analyzed using ultra performance liquid chromatography instrument interfaced to a diode array detector and electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer operated in the negative ion mode. In the laboratory-generated aerosols, we identified 41 compounds that can potentially absorb near-UV and visible wavelengths, such as oxygenated-conjugated compounds, nitroaromatics, and S-containing compounds. The sum of BrC constituents in peat, fern/leaf, and charcoal burning aerosols are 16%, 35%, and 28% of the OA mass, respectively, giving an average contribution of 24%. On average, the BrC constituents account for 0.4% of the ambient OA mass; however, large uncertainties in mass closure remain because of the lack of authentic standards. This study highlights the potential of light-absorbing BrC OA constituents from peat, fern/leaf, and charcoal burning and their importance in the atmosphere.

Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign.

Science.gov (United States)

Jung, Jinsang; Lee, Hanlim; Kim, Young J; Liu, Xingang; Zhang, Yuanhang; Gu, Jianwei; Fan, Shaojia

2009-08-01

Optical and chemical aerosol measurements were obtained from 2 to 31 July 2006 at an urban site in the metropolitan area of Guangzhou (China) as part of the Program of Regional Integrated Experiment of Air Quality over Pearl River Delta (PRIDE-PRD2006) to investigate aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing. During the PRIDE-PRD2006 campaign, the average contributions of ammonium sulfate, organic mass by carbon (OMC), elemental carbon (EC), and sea salt (SS) to total PM(2.5) mass were measured to be 36.5%, 5.7%, 27.1%, 7.8%, and 3.7%, respectively. Compared with the clean marine period, (NH(4))(2)SO(4), NH(4)NO(3), and OMC were all greatly enhanced (by up to 430%) during local haze periods via the accumulation of a secondary aerosol component. The OMC dominance increased when high levels of biomass burning influenced the measurement site while (NH(4))(2)SO(4) and OMC did when both biomass burning and industrial emissions influenced it. The effect of aerosol water content on the total light-extinction coefficient was estimated to be 34.2%, of which 25.8% was due to aerosol water in (NH(4))(2)SO(4), 5.1% that in NH(4)NO(3), and 3.3% that in SS. The average mass-scattering efficiency (MSE) of PM(10) particles was determined to be 2.2+/-0.6 and 4.6+/-1.7m(2)g(-1) under dry (RHwater content, but MSE and SSA are also highly sensitive. It can be concluded that sulfate and carbonaceous aerosol, as well as aerosol water content, play important roles in the processes that determine visibility impairment and radiative forcing in the ambient atmosphere of the Guangzhou urban area.

Brown Carbon Production in Ammonium- or Amine-Containing Aerosol Particles by Reactive Uptake of Methylglyoxal and Photolytic Cloud Cycling.

Science.gov (United States)

De Haan, David O; Hawkins, Lelia N; Welsh, Hannah G; Pednekar, Raunak; Casar, Jason R; Pennington, Elyse A; de Loera, Alexia; Jimenez, Natalie G; Symons, Michael A; Zauscher, Melanie; Pajunoja, Aki; Caponi, Lorenzo; Cazaunau, Mathieu; Formenti, Paola; Gratien, Aline; Pangui, Edouard; Doussin, Jean-François

2017-07-05

The effects of methylglyoxal uptake on the physical and optical properties of aerosol containing amines or ammonium sulfate were determined before and after cloud processing in a temperature- and RH-controlled chamber. The formation of brown carbon was observed upon methylglyoxal addition, detected as an increase in water-soluble organic carbon mass absorption coefficients below 370 nm and as a drop in single-scattering albedo at 450 nm. The imaginary refractive index component k 450 reached a maximum value of 0.03 ± 0.009 with aqueous glycine aerosol particles. Browning of solid particles occurred at rates limited by chamber mixing (cloud events with chamber lights on, suggesting photosensitized brown carbon formation. Despite these changes in optical aerosol characteristics, increases in dried aerosol mass were rarely observed (<1 μg/m 3 in all cases), consistent with previous experiments on methylglyoxal. Under dry, particle-free conditions, methylglyoxal reacted (presumably on chamber walls) with methylamine with a rate constant k = (9 ± 2) × 10 -17 cm 3 molecule -1 s -1 at 294 K and activation energy E a = 64 ± 37 kJ/mol.

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...

Characterization of atmospheric aerosols using Synchroton radiation total reflection X-ray fluorescence and Fe K-edge total reflection X-ray fluorescence-X-ray absorption near-edge structure

Energy Technology Data Exchange (ETDEWEB)

Fittschen, U.E.A. [Department of Chemistry, University of Hamburg, Martin-Luther-King-Platz 6, 20146 Hamburg (Germany)], E-mail: ursula.fittschen@chemie.uni-hamburg.de; Meirer, F. [Atominstitut, Vienna University of Technology, Stadionallee 2, 1020 Wien (Austria)], E-mail: fmeirer@ati.ac.at; Streli, C. [Atominstitut, Vienna University of Technology, Stadionallee 2, 1020 Wien (Austria)], E-mail: streli@ati.ac.at; Wobrauschek, P. [Atominstitut, Vienna University of Technology, Stadionallee 2, 1020 Wien (Austria)], E-mail: wobi@ati.ac.at; Thiele, J. [Department of Chemistry, University of Hamburg, Martin-Luther-King-Platz 6, 20146 Hamburg (Germany)], E-mail: Julian.Thiele@gmx.de; Falkenberg, G. [Hamburger Synchrotronstrahlungslabor at Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22603 Hamburg (Germany)], E-mail: falkenbe@mail.desy.de; Pepponi, G. [ITC-irst, Via Sommarive 18, 38050 Povo (Trento) (Italy)], E-mail: pepponi@itc.it

2008-12-15

In this study a new procedure using Synchrotron total reflection X-ray fluorescence (SR-TXRF) to characterize elemental amounts in atmospheric aerosols down to particle sizes of 0.015 um is presented. The procedure was thoroughly evaluated regarding bounce off effects and blank values. Additionally the potential of total reflection X-ray fluorescence-X-ray absorption near edge structure (SR-TXRF-XANES) for speciation of FeII/III down to amounts of 34 pg in aerosols which were collected for 1 h is shown. The aerosols were collected in the city of Hamburg with a low pressure Berner impactor on Si carriers covered with silicone over time periods of 60 and 20 min each. The particles were collected in four and ten size fractions of 10.0-8.0 {mu}m, 8.0-2.0 {mu}m, 2.0-0.13 {mu}m 0.13-0.015 {mu}m (aerodynamic particle size) and 15-30 nm, 30-60 nm, 60-130 nm, 130-250 nm, 250-500 nm, 0.5-1 {mu}m, 1-2 {mu}m, 2-4 {mu}m, 4-8 {mu}m, 8-16 {mu}m. Prior to the sampling 'bounce off' effects on Silicone and Vaseline coated Si carriers were studied with total reflection X-ray fluorescence. According to the results silicone coated carriers were chosen for the analysis. Additionally, blank levels originating from the sampling device and the calibration procedure were studied. Blank levels of Fe corresponded to 1-10% of Fe in the aerosol samples. Blank levels stemming from the internal standard were found to be negligible. The results from the Synchroton radiation total reflection X-ray fluorescence analysis of the aerosols showed that 20 min of sampling time gave still enough sample material for elemental determination of most elements. For the determination of the oxidation state of Fe in the aerosols different Fe salts were prepared as a reference from suspensions in isopropanol. The results from the Fe K-edge Synchroton radiation total reflection X-ray fluorescence-X-ray absorption near-edge structure analysis of the aerosol samples showed that mainly Fe(III) was present in

Characterization of atmospheric aerosols using Synchroton radiation total reflection X-ray fluorescence and Fe K-edge total reflection X-ray fluorescence-X-ray absorption near-edge structure

International Nuclear Information System (INIS)

Fittschen, U.E.A.; Meirer, F.; Streli, C.; Wobrauschek, P.; Thiele, J.; Falkenberg, G.; Pepponi, G.

2008-01-01

In this study a new procedure using Synchrotron total reflection X-ray fluorescence (SR-TXRF) to characterize elemental amounts in atmospheric aerosols down to particle sizes of 0.015 um is presented. The procedure was thoroughly evaluated regarding bounce off effects and blank values. Additionally the potential of total reflection X-ray fluorescence-X-ray absorption near edge structure (SR-TXRF-XANES) for speciation of FeII/III down to amounts of 34 pg in aerosols which were collected for 1 h is shown. The aerosols were collected in the city of Hamburg with a low pressure Berner impactor on Si carriers covered with silicone over time periods of 60 and 20 min each. The particles were collected in four and ten size fractions of 10.0-8.0 μm, 8.0-2.0 μm, 2.0-0.13 μm 0.13-0.015 μm (aerodynamic particle size) and 15-30 nm, 30-60 nm, 60-130 nm, 130-250 nm, 250-500 nm, 0.5-1 μm, 1-2 μm, 2-4 μm, 4-8 μm, 8-16 μm. Prior to the sampling 'bounce off' effects on Silicone and Vaseline coated Si carriers were studied with total reflection X-ray fluorescence. According to the results silicone coated carriers were chosen for the analysis. Additionally, blank levels originating from the sampling device and the calibration procedure were studied. Blank levels of Fe corresponded to 1-10% of Fe in the aerosol samples. Blank levels stemming from the internal standard were found to be negligible. The results from the Synchroton radiation total reflection X-ray fluorescence analysis of the aerosols showed that 20 min of sampling time gave still enough sample material for elemental determination of most elements. For the determination of the oxidation state of Fe in the aerosols different Fe salts were prepared as a reference from suspensions in isopropanol. The results from the Fe K-edge Synchroton radiation total reflection X-ray fluorescence-X-ray absorption near-edge structure analysis of the aerosol samples showed that mainly Fe(III) was present in all particle size fractions

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

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

Relative importance of black carbon, brown carbon, and absorption enhancement from clear coatings in biomass burning emissions

Science.gov (United States)

Pokhrel, Rudra P.; Beamesderfer, Eric R.; Wagner, Nick L.; Langridge, Justin M.; Lack, Daniel A.; Jayarathne, Thilina; Stone, Elizabeth A.; Stockwell, Chelsea E.; Yokelson, Robert J.; Murphy, Shane M.

2017-04-01

A wide range of globally significant biomass fuels were burned during the fourth Fire Lab at Missoula Experiment (FLAME-4). A multi-channel photoacoustic absorption spectrometer (PAS) measured dry absorption at 405, 532, and 660 nm and thermally denuded (250 °C) absorption at 405 and 660 nm. Absorption coefficients were broken into contributions from black carbon (BC), brown carbon (BrC), and lensing following three different methodologies, with one extreme being a method that assumes the thermal denuder effectively removes organics and the other extreme being a method based on the assumption that black carbon (BC) has an Ångström exponent of unity. The methodologies employed provide ranges of potential importance of BrC to absorption but, on average, there was a difference of a factor of 2 in the ratio of the fraction of absorption attributable to BrC estimated by the two methods. BrC absorption at shorter visible wavelengths is of equal or greater importance to that of BC, with maximum contributions of up to 92 % of total aerosol absorption at 405 nm and up to 58 % of total absorption at 532 nm. Lensing is estimated to contribute a maximum of 30 % of total absorption, but typically contributes much less than this. Absorption enhancements and the estimated fraction of absorption from BrC show good correlation with the elemental-carbon-to-organic-carbon ratio (EC / OC) of emitted aerosols and weaker correlation with the modified combustion efficiency (MCE). Previous studies have shown that BrC grows darker (larger imaginary refractive index) as the ratio of black to organic aerosol (OA) mass increases. This study is consistent with those findings but also demonstrates that the fraction of total absorption attributable to BrC shows the opposite trend: increasing as the organic fraction of aerosol emissions increases and the EC / OC ratio decreases.

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

Science.gov (United States)

Glotfelty, Timothy; He, Jian; Zhang, Yang

2017-06-01

New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM-NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m-3 and that of primary organic aerosol (POA) decreases by 0.22 µg m-3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM-NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA-climate simulations.

Observations of black carbon aerosols characteristics over an urban environment: Radiative forcing and related implications.

Science.gov (United States)

Bibi, Samina; Alam, Khan; Chishtie, Farrukh; Bibi, Humera; Rahman, Said

2017-12-15

With observations of black carbon (BC) aerosol concentrations, optical and radiative properties were obtained over the urban city of Karachi during the period of March 2006-December 2008. BC concentrations were continuously measured using an Aethalometer, while optical and radiative properties were estimated through the Optical Properties of Aerosols and Clouds (OPAC) and Santa Barbra DISORT Atmospheric Radiative Transfer (SBDART) models, respectively. For the study period, the measured BC concentrations were higher during January, February and November, while lower during May, June, July and August. A maximum peak value was observed during January 2007 while the minimum value was observed during June 2006. The Short Wave (SW) BC Aerosol Radiative Forcing (ARF) both at Top of the Atmosphere (ToA) and within ATMOSphere (ATMOS) were positive during all the months, whereas negative SW BC ARF was found at the SurFaCe (SFC). Overall, SW BC ARF was higher during January, February and November, while relatively lower ARF was found during May, June, July and August. Conversely, the Long Wave (LW) BC ARF at ToA and SFC remained positive, whereas within ATMOS it shifted towards positive values (heating effect) during June-August. Finally, the net (SW+LW) BC ARF were found to be positive at ToA and in ATMOS, while negative at SFC. Moreover, a systematic increase in Atmospheric Heating Rate (AHR) was found during October to January. Additionally, we found highest correlation between Absorption Aerosol Optical Depth (AOD abs ) and SW BC ARF within ATMOS followed by SFC and ToA. Overall, the contribution of BC to the total ARF was found to greater than 84% for the whole observational period while contributing up to 93% during January 2007. Copyright © 2017 Elsevier B.V. All rights reserved.

Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Dron, J.; El Haddad, I.; Temime-Roussel, B.; Wortham, H.; Marchand, N. [Univ Aix Marseille, CNRS, Lab Chim Provence, Equipe Instrumentat and React Atmospher, UMR 6264, F-13331 Marseille 3 (France); Jaffrezo, J.L. [Univ Grenoble 1, CNRS, UMR 5183, Lab Glaciol and Geophys Environm, F-38402 St Martin Dheres (France)

2010-07-01

The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCIMS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R' respectively) and precursor ion (nitro groups, R-NO{sub 2}) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalization rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional

Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Directory of Open Access Journals (Sweden)

J. Dron

2010-08-01

Full Text Available The functional group composition of various organic aerosols (OA is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS. The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R´ respectively and precursor ion (nitro groups, R-NO₂ scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular to 13.5% (o-xylene photooxidation of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60

Functional characterization of the water-soluble organic carbon of size-fractionated aerosol in the southern Mississippi Valley

Science.gov (United States)

Chalbot, M.-C. G.; Brown, J.; Chitranshi, P.; Gamboa da Costa, G.; Pollock, E. D.; Kavouras, I. G.

2014-06-01

The chemical content of water-soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for periods when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp magnetic resonance (1H-NMR). The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m-3 for particles with 1.5 fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of 1H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosols and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from -26.81 ± 0.18‰ for the smallest particles to -25.93 ± 0.31‰ for the largest particles and the relative distribution of the functional groups as compared to those previously observed for marine, biomass burning and secondary organic aerosol. The latter also allowed for the differentiation of urban combustion-related aerosol and biological particles. The five types of organic hydrogen accounted for the majority of WSOC for particles with dp > 3.0 μm and dp < 0.96 μm.

Functional characterization of the water-soluble organic carbon of size fractionated aerosol in the Southern Mississippi Valley

Science.gov (United States)

Chalbot, M.-C. G.; Brown, J.; Chitranshi, P.; Gamboa da Costa, G.; Pollock, E. D.; Kavouras, I. G.

2014-02-01

The chemical content of the water soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to: (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for the period when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp magnetic resonance. The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m-3 for particles with 0.96 fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of 1H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosol and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from -26.81 ± 0.18‰ for the smallest particles to -25.93 ± 0.31‰ for the largest particles and the relative distribution of the functional groups as compared to those previously observed for marine, biomass burning and secondary organic aerosol. The latter also allowed for the differentiation of urban combustion-related aerosol and biological particles. The five types of organic hydrogen accounted for the majority of WSOC for particles with dp > 3.0 μm and dp < 0.96 μm.

Aerosol assisted synthesis of hierarchical tin–carbon composites and their application as lithium battery anode materials

KAUST Repository

Guo, Juchen

2013-01-01

We report a method for synthesizing hierarchically structured tin-carbon (Sn-C) composites via aerosol spray pyrolysis. In this method, an aqueous precursor solution containing tin(ii) chloride and sucrose is atomized, and the resultant aerosol droplets carried by an inert gas are pyrolyzed in a high-temperature tubular furnace. Owing to the unique combination of high reaction temperature and short reaction time, this method is able to achieve a hetero-structure in which small Sn particles (15 nm) are uniformly embedded in a secondary carbon particle. This procedure allows the size and size distribution of the primary Sn particles to be tuned, as well as control over the size of the secondary carbon particles by addition of polymeric surfactant in the precursor solution. When evaluated as anode materials for lithium-ion batteries, the resultant Sn-C composites demonstrate attractive electrochemical performance in terms of overall capacity, electrochemical stability, and coulombic efficiency. © 2013 The Royal Society of Chemistry.

Simulated responses of terrestrial aridity to black carbon and sulfate aerosols

Science.gov (United States)

Lin, L.; Gettelman, A.; Xu, Y.; Fu, Q.

2016-01-01

Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. Here we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate of 0.9%/°C of global mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO4-induced PET changes.

Evaluation of the carbon content of aerosols from the burn- ing of biomass in the Brazilian Amazon using thermal, op- tical and thermal-optical analysis methods

Energy Technology Data Exchange (ETDEWEB)

Soto-Garcia, Lydia L.; Andreae, Meinrat O.; Andreae, Tracey W.; taxo, Paulo Ar-; Maenhaut, Willy; Kirchstetter, Thomas; Novakov, T.; Chow, Judith C.; Mayol-Bracero, Olga L.

2011-06-03

Aerosol samples were collected at a pasture site in the Amazon Basin as part of the project LBA-SMOCC-2002 (Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate: Aerosols from Biomass Burning Perturb Global and Regional Climate). Sampling was conducted during the late dry season, when the aerosol composition was dominated by biomass burning emissions, especially in the submicron fraction. A 13-stage Dekati low-pressure impactor (DLPI) was used to collect particles with nominal aerodynamic diameters (D{sub p}) ranging from 0.03 to 0.10 m. Gravimetric analyses of the DLPI substrates and filters were performed to obtain aerosol mass concentrations. The concentrations of total, apparent elemental, and organic carbon (TC, EC{sub a}, and OC) were determined using thermal and thermal-optical analysis (TOA) methods. A light transmission method (LTM) was used to determine the concentration of equivalent black carbon (BC{sub e}) or the absorbing fraction at 880 nm for the size-resolved samples. During the dry period, due to the pervasive presence of fires in the region upwind of the sampling site, concentrations of fine aerosols (D{sub p} < 2.5 {mu}m: average 59.8 {mu}g m{sup -3}) were higher than coarse aerosols (D{sub p} > 2.5 {mu}m: 4.1 {mu}g m{sup -3}). Carbonaceous matter, estimated as the sum of the particulate organic matter (i.e., OC x 1.8) plus BC{sub e}, comprised more than 90% to the total aerosol mass. Concentrations of EC{sub a} (estimated by thermal analysis with a correction for charring) and BCe (estimated by LTM) averaged 5.2 {+-} 1.3 and 3.1 {+-} 0.8 {mu}g m{sup -3}, respectively. The determination of EC was improved by extracting water-soluble organic material from the samples, which reduced the average light absorption {angstrom} exponent of particles in the size range of 0.1 to 1.0 {mu}m from > 2.0 to approximately 1.2. The size-resolved BC{sub e} measured by the LTM showed a clear maximum between 0.4 and

Laboratory Experiments and Instrument Development for the Study of Atmospheric Aerosols

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul

2011-12-10

Soot particles are generated by incomplete combustion of fossil and biomass fuels. Through direct effects clear air aerosols containing black carbon (BC) such as soot aerosols, absorb incoming light heating the atmosphere, while most other aerosols scatter light and produce cooling. Even though BC represents only 1-2% of the total annual emissions of particulate mass to the atmosphere, it has been estimated that the direct radiative effect of BC is the second-most important contributor to global warming after absorption by CO2. Ongoing studies continue to underscore the climate forcing importance of black carbon. However, estimates of the radiative effects of black carbon on climate remain highly uncertain due to the complexity of particles containing black carbon. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. Freshly emitted soot particles are typically fractal hydrophobic aggregates. The aggregates consist of black carbon spherules with diameters typically in the range of about 15-40 nm, and they are usually coated by adsorbed polyaromatic hydrocarbons (PAHs) produced during combustion. Diesel-generated soot particles are often emitted with an organic coating composed primarily of lubricating oil and unburned fuel, as well as well as PAH compounds. Sulfuric acid has also been detected in diesel and aircraft-emitted soot particles. In the course of aging, these particle coatings may be substantially altered by chemical reactions and/or the deposition of other materials. Such processes transform the optical and CCN properties of the soot aerosols in ways that are not yet well understood. Our work over the past seven years consisted of laboratory research, instrument development and characterization, and field studies with the central focus of improving our understanding of the black carbon aerosol climate impacts. During the sixth year as well as during this seventh year (no

Total Lightning Flash Activity Response to Aerosol over China Area

Directory of Open Access Journals (Sweden)

Pengguo Zhao

2017-01-01

Full Text Available Twelve years of measurements of aerosol optical depth (AOD, cloud fraction, cloud top height, ice cloud optical thickness and lightning flash density from 2001 to 2012 have been analyzed to investigate the effect of aerosols on electrical activity over an area of China. The results show that increasing aerosol loading inspires the convective intensity, and then increases the lightning flash density. The spatial distribution of the correlation between aerosol loading and electrical activity shows a remarkable regional difference over China. The high-correlation regions embody the positive aerosol microphysical effect on the intensity of the electrical activity, while the large-scale processes may play the main role in convection development and producing lightning in low-correlation regions.

The research of a method for determination of total carbon, combination carbon and free carbon in beryllium metal

International Nuclear Information System (INIS)

Yang Xingzhong; Zhu Xiaohong

1996-02-01

A method for determination of total carbon, combination carbon and free carbon in beryllium metal with LECO CS-344 carbon/sulphur determinant has been studied. Tungsten-copper mixed pellets are used as flux to the determination of total carbon. Ratio of weight of the flux to the sample is greater than 20:1. Good analytical results are got. By this method the relative standard deviation is <10% when the content of total carbon in the range of 0.050%∼0.080% in beryllium. A standard steel sample of carbon is added into beryllium, the recoveries are 94%∼106%. For determination of free carbon, the sample are decomposed with 3 mol/L HCl, filtered and followed determination. By this method the relative standard deviation is ≤10% when the content of free carbon in the range of 0.006%∼0.020% in beryllium. the balance of total carbon and free carbon is equal to combination carbon. The method is used to determine the sample of content of total carbon in the range of 0.050%∼1.00%, free carbon in the range of 0.006%∼0.500% in metal beryllium. (6 refs., 1 fig., 13 tabs.)

Stable carbon and nitrogen isotopic composition of fine mode aerosols (PM2.5 over the Bay of Bengal: impact of continental sources

Directory of Open Access Journals (Sweden)

Srinivas Bikkina

2016-07-01

Full Text Available This study reports on stable carbon (δ13CTC and nitrogen (δ15NTN isotopic composition of total carbon and nitrogen (TC and TN in the fine mode aerosols (PM2.5; N=31 collected over the Bay of Bengal (BoB. The samples represent two distinct wind regimes during the cruise (27 December 2008–28 January 2009; one from the Indo-Gangetic Plain (referred as IGP-outflow and another from Southeast Asia (SEA-outflow. The PM2.5 samples from the IGP-outflow show higher δ13CTC (−25.0 to −22.8 ‰; −23.8±0.6 ‰ than those from the SEA-outflow (−27.4 to −24.7 ‰; −25.3±0.9 ‰. Similarly, δ15NTN varied from +11.8 to +30.6 ‰ (+20.4±5.4 ‰ and +10.4 to +31.7 ‰ (+19.4±6.1 ‰ for IGP- and SEA-outflows, respectively. Based on the literature data, MODIS-derived fire hotspots and back trajectories, we infer that higher δ13CTC in the IGP-outflow is predominantly associated with fossil fuel and biofuel combustion. In contrast, contribution of primary organic aerosols from the combustion of C3 plants or secondary organic aerosol (SOA formation from biomass/biofuel-burning emissions (BBEs can explain the lower δ13CTC values in the SEA-outflow. This inference is based on the significant linear correlations among δ13CTC, water-soluble organic carbon and non-sea-salt potassium (nss-K+, a proxy for BBEs in the SEA-outflow. A significant linear relationship of δ15N with and equivalent mass ratio of / is evident in both the continental outflows. Since abundance dominates the TN over the BoB (>90 %, atmospheric processes affecting its concentration in fine mode aerosols can explain the observed large variability of δ15NTN.

Review of brown carbon aerosols: Recent progress and perspectives.

Science.gov (United States)

Yan, Juping; Wang, Xiaoping; Gong, Ping; Wang, Chuanfei; Cong, Zhiyuan

2018-09-01

Brown carbon (BrC), a carbonaceous aerosol which absorbs solar radiation over a broad range of wavelengths, is beginning to be seen as an important contributor to global warming. BrC absorbs both inorganic and organic pollutants, leading to serious effects on human health. We review the fundamental features of BrC, including its sources, chemical composition, optical properties and radiative forcing effects. We detail the importance of including photochemical processes related to BrC in the GEOS-Chem transport model for the estimation of aerosol radiative forcing. Calculation methods for BrC emission factors are examined, including the problems and limitations of current measurement methods. We provide some insight into existing publications and recommend areas for future research, such as further investigations into the reaction mechanisms of the aging of secondary BrC, calculations of the emission factors for BrC from different sources, the absorption of large and long-lived BrC molecules and the construction of an enhanced model for the simulation of radiative forcing. This review will improve our understanding of the climatic and environmental effects of BrC. Copyright © 2018 Elsevier B.V. All rights reserved.

Total and regional deposition of inhaled aerosols in supine healthy subjects and subjects with mild-to-moderate COPD

Energy Technology Data Exchange (ETDEWEB)

Darquenne, Chantal; Lamm, Wayne J.; Fine, Janelle M.; Corley, Richard A.; Glenny, Robb W.

2016-09-01

Despite substantial development of sophisticated subject-specific computational models of aerosol transport and deposition in human lungs, experimental validation of predic- tions from these new models is sparse. We collected aerosol retention and exhalation profiles in seven healthy volunteers and six subjects with mild-to-moderate COPD (FEV1 ¼ 50–80%predicted) in the supine posture. Total deposition was measured during continuous breathing of 1 and 2.9 mm-diameter particles (tidal volume of 1 L, flow rate of 0.3 L/s and 0.75 L/s). Bolus inhalations of 1 mm particles were performed to penetration volumes of 200, 500 and 800 mL (flow rate of 0.5 L/s). Aerosol bolus dispersion (H), deposition, and mode shift (MS) were calculated from these data. There was no significant difference in total deposition between healthy subjects and those with COPD. Total deposition increased with increasing particle size and also with increasing flow rate. Similarly, there was no significant difference in aerosol bolus deposition between subject groups. Yet, the rate of increase in dispersion and of decrease in MS with increasing penetration volume was higher in subjects with COPD than in healthy volunteers (H: 0.79870.205 vs. 0.52770.122 mL/mL, p¼ 0.01; MS: - 0.27170.129 vs. - 0.145 70.076 mL/mL, p¼ 0.05) indicating larger ventilation inhomogeneities (based on H) and increased flow sequencing (based on MS) in the COPD than in the healthy group. In conclusion, in the supine posture, deposition appears to lack sensitivity for assessing the effect of lung morphology and/or ventilation distribution alteration induced by mild-to- moderate lung disease on the fate of inhaled aerosols. However, other parameters such as aerosol bolus dispersion and mode shift may be more sensitive parameters for evaluating models of lungs with moderate disease.

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

Science.gov (United States)

Glotfelty, Timothy; He, Jian

2017-01-01

Abstract New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM‐NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m−3 and that of primary organic aerosol (POA) decreases by 0.22 µg m−3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM‐NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA‐climate simulations. PMID:29104733

Preliminary characterization of submicron secondary aerosol in the amazon forest - ATTO station

Science.gov (United States)

Carbone, S.; Ferreira De Brito, J.; Andreae, M. O.; Pöhlker, C.; Chi, X.; Saturno, J.; Barbosa, H. M.; Artaxo, P.

2014-12-01

Biogenic secondary organic aerosol particles are investigated in the Amazon in the context of the GoAmazon Project. The forest naturally emits a large number of gaseous compounds; they are called the volatile organic compounds (VOCs). They are emitted through processes that are not totally understood. Part of those gaseous compounds are converted into aerosol particles, which affect the biogeochemical cycles, the radiation balance, the mechanisms involving cloud formation and evolution, among few other important effects. In this study the aerosol life-cycle is investigated at the ATTO station, which is located about 150 km northeast of Manaus, with emphasis on the natural organic component and its impacts in the ecosystem. To achieve these objectives physical and chemical aerosol properties have been investigated, such as the chemical composition with aerosol chemical speciation monitor (ACSM), nanoparticle size distribution (using the SMPS - Scanning Mobility Particle Sizer), optical properties with measurements of scattering and absorption (using nephelometers and aethalometers). Those instruments have been operating continuously since February 2014 together with trace gases (O3, CO2, CO, SO2 and NOx) analyzers and additional meteorological instruments. On average PM1 (the sum of black carbon, organic and inorganic ions) totalized 1.0±0.3 μg m-3, where the organic fraction was dominant (75%). During the beginning of the dry season (July/August) the organic aerosol presented a moderate oxygenated character with the oxygen to carbon ratio (O:C) of 0.7. In the wet season some episodes containing significant amount of chloride and backward wind trajectories suggest aerosol contribution from the Atlantic Ocean. A more comprehensive analysis will include an investigation of the different oxidized fractions of the organic aerosol and optical properties.

Aerosol Optical Depth Over India

Science.gov (United States)

David, Liji Mary; Ravishankara, A. R.; Kodros, John K.; Venkataraman, Chandra; Sadavarte, Pankaj; Pierce, Jeffrey R.; Chaliyakunnel, Sreelekha; Millet, Dylan B.

2018-04-01

Tropospheric aerosol optical depth (AOD) over India was simulated by Goddard Earth Observing System (GEOS)-Chem, a global 3-D chemical-transport model, using SMOG (Speciated Multi-pOllutant Generator from Indian Institute of Technology Bombay) and GEOS-Chem (GC) (current inventories used in the GEOS-Chem model) inventories for 2012. The simulated AODs were 80% (SMOG) and 60% (GC) of those measured by the satellites (Moderate Resolution Imaging Spectroradiometer and Multi-angle Imaging SpectroRadiometer). There is no strong seasonal variation in AOD over India. The peak AOD values are observed/simulated during summer. The simulated AOD using SMOG inventory has particulate black and organic carbon AOD higher by a factor 5 and 3, respectively, compared to GC inventory. The model underpredicted coarse-mode AOD but agreed for fine-mode AOD with Aerosol Robotic Network data. It captured dust only over Western India, which is a desert, and not elsewhere, probably due to inaccurate dust transport and/or noninclusion of other dust sources. The calculated AOD, after dust correction, showed the general features in its observed spatial variation. Highest AOD values were observed over the Indo-Gangetic Plain followed by Central and Southern India with lowest values in Northern India. Transport of aerosols from Indo-Gangetic Plain and Central India into Eastern India, where emissions are low, is significant. The major contributors to total AOD over India are inorganic aerosol (41-64%), organic carbon (14-26%), and dust (7-32%). AOD over most regions of India is a factor of 5 or higher than over the United States.

Adsorption of NO{sub 2} on carbon aerosols particles at the low ppb-level

Energy Technology Data Exchange (ETDEWEB)

Kalberer, M.; Ammann, M.; Baltensperger, U.; Gaeggeler, H.W. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1997-09-01

The adsorption of NO{sub 2} at the low ppb-level (3-40 ppb) on carbon aerosol particles was investigated. A sticking coefficient of about 2.10{sup -4} was found, similar to that in previous studies using radioactively labeled {sup 13}NO{sub 2}. (author) 2 figs., 2 refs.

Tropical intercontinental optical measurement network of aerosol, precipitable water and total column ozone

Science.gov (United States)

Holben, B. N.; Tanre, D.; Reagan, J. A.; Eck, T. F.; Setzer, A.; Kaufman, Y. A.; Vermote, E.; Vassiliou, G. D.; Lavenu, F.

1992-01-01

A new generation of automatic sunphotometers is used to systematically monitor clear sky total column aerosol concentration and optical properties, precipitable water and total column ozone diurnally and annually in West Africa and South America. The instruments are designed to measure direct beam sun, solar aureole and sky radiances in nine narrow spectral bands from the UV to the near infrared on an hourly basis. The instrumentation and the algorithms required to reduce the data for subsequent analysis are described.

Study of aerosol behavior on the basis of morphological characteristics during festival events in India

Science.gov (United States)

Agrawal, Anubha; Upadhyay, Vinay K.; Sachdeva, Kamna

2011-07-01

Two important festival events were selected to assess their impacts on atmospheric chemistry by understanding settling velocity and emission time of aerosols. Using high volume sampler, aerosols were collected in a sequential manner to understand settling velocity and emission time of aerosols on a particular day. Composition and total suspended particulate load of the aerosols collected during the festivals were used as markers for strengthening the assessment. Terminal settling velocity of the aerosols were calculated using morphological and elemental compositional data, obtained from scanning electron microcopy (SEM) and energy dispersive X-ray (EDX) study. Aerosol load, black carbon, aromatic carbon and terminal velocity calculations were correlated to obtain conclusion that aerosols collected on the festival day might have been emitted prior to the festival. Settling time of aerosols collected on 17th and 19th October'09 during Diwali were found to be 36.5 (1.5 days) and 12.8 h, respectively. Carbon concentration estimated using EDX was found to be almost double in the sample collected after 2 days of the festival event. This strengthens our inference of time calculation where carbon with high concentration of load must have settled approximately after two days of the event. Settling time of aerosols collected on Holi morning and afternoon was found to be 1.7 and 24.8 h, respectively. Further, because of the small distance of 5.4 km between the meteorological station and sampling site, observed TSP values were compared with theoretical load values, calculated by using visibility values taken from the meteorological data. And it was found that both experimental and calculated values are close to each other about 50% of the times, which proves the assumption that experimental and meteorological data are comparable.

Characterization of aerosol particles at the forested site in Lithuania

Science.gov (United States)

Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

2009-04-01

monitoring station (55˚ 26'26"N; 26˚ 03'60"E) in the eastern part of Lithuania in the Aukštaitija national park during 2-24 July, 2008. The Rugšteliškis station is located in a remote relatively clean forested area. An aerosol mass spectrometer (AMS), developed at Aerodyne Research, was used to obtain real-time quantitative information on particle size-resolved mass loadings for volatile and semi-volatile chemical components present in/on ambient aerosol. The AMS inlet system allows 100 % transmission efficiency for particles with size diameter between 60 to 600 nm and partial transmission down to 20 nm and up to 2000 nm. The aerosol sampling was also carried out using a Micro-Orifice Uniform Deposit Impactor (MOUDI) model 110. The flow rate was 30 l/min, and the 50% aerodynamic cutoff diameters of the 10 stages were 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.32, 0.18, 0.10 and 0.056 m. Aluminum foil was used as the impaction surface. The aerosol samples were analyzed for total carbon using the elemental analyzer (Flash EA1112). Besides, samples were analyzed for ^13C/12C ratio by the isotopic ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (Norman et al., 1999; Garbaras et al., 2008). During campaign the dynamic behavior of aerosols was measured and quantitatively compared with meteorological conditions and air mass transport. The submicron aerosol was predominately sulphate and organic material. The AMS was able to discriminate and quantify mixed organic/inorganic accumulation mode particles (300 - 400 nm), which appeared to be dominated by regional sources and were of the origin similar to those seen in the more remote areas. The particulate organic fraction was also investigated in detail using the mass spectral data. By combining the organic matter size distribution (measured with AMS) with the total carbon (TC) size distribution (measured with MOUDI) we were able to report organic carbon to total carbon (OC/TC) ratio in different size particles

Aerosol formation of Sea-Urchin-like nanostructures of carbon nanotubes on bimetallic nanocomposite particles

International Nuclear Information System (INIS)

Kim, S. H.; Wang, C.; Zachariah, M. R.

2011-01-01

With the advantage of continuous production of pure carbon nanotubes (CNTs), a new simple aerosol process for the formation of CNTs was developed. A combination of conventional spray pyrolysis and thermal chemical vapor deposition enabled the formation unusual sea-urchin-like carbon nanostructures composed of multi-walled CNTs and metal composite nanoparticles. The CNTs formed were relatively untangled and uniform with a diameter of less than∼10 nm. The key to the formation of CNTs in this way was to create a substrate particle containing both a catalytic and non-catalytic component, which prevented coking. The density of the CNTs grown on the spherical metal nanoparticles could be controlled by perturbing the density of the metal catalysts (Fe) in the host non-catalytic metal particle matrix (Al). Mobility size measurement was identified as a useful technique to real-time characterization of either the catalytic formation of thin carbon layer or CNTs on the surface of the metal aerosol. These materials have shown unique properties in enhancing the thermal conductivity of fluids. Other potential advantages are that the as-produced material can be manipulated easily without the concern of high mobility of conventional nanowires, and then subsequently released at the desired time in an unagglomerated state.

Aerosol-induced thermal effects increase modelled terrestrial photosynthesis and transpiration

International Nuclear Information System (INIS)

Steiner, Allison L.; Chameides, W.L.

2005-01-01

Previous studies suggest that the radiative effects of atmospheric aerosols (reducing total radiation while increasing the diffuse fraction) can enhance terrestrial productivity. Here, simulations using a regional climate/terrestrial biosphere model suggest that atmospheric aerosols could also enhance terrestrial photosynthesis and transpiration through an interaction between solar radiation, leaf temperature and stomatal conductance. During midday, clear-sky conditions, sunlit-leaf temperatures can exceed the optimum for photosynthesis, depressing both photosynthesis and transpiration. Aerosols decrease surface solar radiation, thereby reducing leaf temperatures and enhancing sunlit-leaf photosynthesis and transpiration. This modelling study finds that, under certain conditions, this thermal response of aerosols can have a greater impact on photosynthesis and transpiration than the radiative response. This implies that a full understanding of the impact of aerosols on climate and the global carbon cycle requires consideration of the biophysical responses of terrestrial vegetation as well as atmospheric radiative and thermodynamic effects

Technical Note: Molecular characterization of aerosol-derived water soluble organic carbon using ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry

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R. M. Dickhut

2008-09-01

Full Text Available Despite the acknowledged relevance of aerosol-derived water-soluble organic carbon (WSOC to climate and biogeochemical cycling, characterization of aerosol WSOC has been limited. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS was utilized in this study to provide detailed molecular level characterization of the high molecular weight (HMW; m/z>223 component of aerosol-derived WSOC collected from rural sites in Virginia and New York, USA. More than 3000 peaks were detected by ESI FT-ICR MS within a m/z range of 223–600 for each sample. Approximately 86% (Virginia and 78% (New York of these peaks were assigned molecular formulas using only carbon (C, hydrogen (H, oxygen (O, nitrogen (N, and sulfur (S as elemental constituents. H/C and O/C molar ratios were plotted on van Krevelen diagrams and indicated a strong contribution of lignin-like and lipid-like compounds to the aerosol-derived WSOC samples. Approximately 1–4% of the peaks in the aerosol-derived WSOC mass spectra were classified as black carbon (BC on the basis of double bond equivalents calculated from the assigned molecular formulas. In addition, several high-magnitude peaks in the mass spectra of samples from both sites corresponded to molecular formulas proposed in previous secondary organic aerosol (SOA laboratory investigations indicating that SOAs are important constituents of the WSOC. Overall, ESI FT-ICR MS provides a level of resolution adequate for detailed compositional and source information of the HMW constituents of aerosol-derived WSOC.

Impact of Biomass Burning Aerosols on the Biosphere over Amazonia

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Malavelle, F.; Haywood, J.; Mercado, L.; Folberth, G.; Bellouin, N.

2014-12-01

Biomass burning (BB) smoke from deforestation and the burning of agricultural waste emit a complex cocktail of aerosol particles and gases. BB emissions show a regional hotspot over South America on the edges of Amazonia. These major perturbations and impacts on surface temperature, surface fluxes, chemistry, radiation, rainfall, may have significant consequent impacts on the Amazon rainforest, the largest and most productive carbon store on the planet. There is therefore potential for very significant interaction and interplay between aerosols, clouds, radiation and the biosphere in the region. Terrestrial carbon production (i.e. photosynthesis) is intimately tied to the supply of photosynthetically active radiation (PAR - i.e. wavelengths between 300-690 nm). PAR in sufficient intensity and duration is critical for plant growth. However, if a decrease in total radiation is accompanied by an increase in the component of diffuse radiation, plant productivity may increase due to higher light use efficiency per unit of PAR and less photosynthetic saturation. This effect, sometimes referred as diffuse light fertilization effect, could have increased the global land carbon sink by approximately one quarter during the global dimming period and is expected to be a least as important locally. By directly interacting with radiation, BB aerosols significantly reduce the total amount of PAR available to plant canopies. In addition, BB aerosols also play a centre role in cloud formation because they provide the necessary cloud condensation nuclei, hence indirectly altering the water cycle and the components and quantity of PAR. In this presentation, we use the recent observations from the South American Biomass Burning Analysis (SAMBBA) to explore the impact of radiation changes on the carbon cycle in the Amazon region caused by BB emissions. A parameterisation of the impact of diffuse and direct radiation upon photosynthesis rates and net primary productivity in the

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

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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.

A risk-based framework for assessing the effectiveness of stratospheric aerosol geoengineering.

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Angus J Ferraro

Full Text Available Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth's surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth's surface area, containing 36% of its population and 60% of its gross domestic product.

A Risk-Based Framework for Assessing the Effectiveness of Stratospheric Aerosol Geoengineering

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Ferraro, Angus J.; Charlton-Perez, Andrew J.; Highwood, Eleanor J.

2014-01-01

Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth's surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth's surface area, containing 36% of its population and 60% of its gross domestic product. PMID:24533155

Seasonal variation of marine organic aerosols in the North Pacific Ocean

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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.

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

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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.

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.

Sugars in atmospheric aerosols over the Eastern Mediterranean

Science.gov (United States)

Theodosi, Christina; Panagiotopoulos, Christos; Nouara, Amel; Zarmpas, Pavlos; Nicolaou, Panagiota; Violaki, Kalliopi; Kanakidou, Maria; Sempéré, Richard; Mihalopoulos, Nikolaos

2017-04-01

The role of biomass combustion and primary bio-particles in atmospheric PM10 aerosols in the Eastern Mediterranean over a two-year period was estimated by studying sugar tracers. Sugar concentrations ranged from 6 to 334 ng m-3, while their contributions to the organic carbon (OC) and water soluble organic carbon (WSOC) pools were 3 and 11%, respectively. Over the studied period, glucose and levoglucosan were the two most abundant sugars accounting equally about 25% of the total sugar concentration in PM10 aerosols whereas fructose, sucrose, and mannitol represented 18%, 15% and 10%, respectively. Primary saccharides (glucose, fructose, and sucrose) peaked at the beginning of spring (21, 17 and 15 ng m-3, respectively), indicating significant contributions of bioaerosols to the total organic aerosol mass. On the other hand, higher concentrations of anhydrosugars (burning biomass tracers including levoglucosan, mannosan and galactosan) were recorded in winter (19, 1.4 and 0.2 ng m-3, respectively) than in summer (9.1, 1.1 and 0.5 ng m-3, respectively). Levoglucosan was the dominant monosaccharide in winter (37% of total sugars) with less contribution in summer (19%) probably in relation with enhanced photochemical oxidation reactions by hydroxyl (ṡOH) radicals impacting anhydrosugars. We estimate that atmospheric oxidation by ṡOH decreases levoglucosan levels by 54% during summer. Biomass burning, based on levoglucosan observations, was estimated to contribute up to 13% to the annual average OC measured at Finokalia. Annual OC, WSOC, and carbohydrate dry deposition fluxes for the studied period were estimated to 414, 175, and 9 mg C m-2 y-1, respectively. Glucose and levoglucosan accounted for 34% and 2% of the total sugar fluxes. According to our estimations, atmospheric OC and WSOC inputs account for ˜0.70% of the carbon produced by annual primary production (PP) in the Cretan Sea. Considering the entire Mediterranean, dry deposition of OC could provide at

Seasonal variations and sources of ambient fossil and biogenic-derived carbonaceous aerosols based on 14C measurements in Lhasa, Tibet

Science.gov (United States)

Huang, Jie; Kang, Shichang; Shen, Chengde; Cong, Zhiyuan; Liu, Kexin; Wang, Wei; Liu, Lichao

2010-06-01

A total of 30 samples of total suspended particles were collected at an urban site in Lhasa, Tibet from August 2006 to July 2007 for investigating carbonaceous aerosol features. The fractions of contemporary carbon ( fc) in total carbon (TC) of ambient aerosols are presented using radiocarbon ( 14C) measurements. The value of fc represents the biogenic contribution to TC, as the biosphere releases organic compounds with the present 14C/ 12C level ( fc = 1), whereas 14C has become extinct in anthropogenic emissions of fossil carbon ( fc = 0). The fc values in Lhasa ranging from 0.357 to 0.702, are higher than Beijing and Tokyo, but clearly lower than the rural region of Launceston, which indicates a major biogenic influence in Lhasa. Seasonal variations of fc values corresponded well with variations of pollutants concentrations (e.g. NO 2). Higher fc values appeared in winter indicating carbonaceous aerosol is more dominated by wood burning and incineration of agricultural wastes within this season. The lower fc values in summer and autumn may be caused by increased diesel and petroleum emissions related to tourism in Lhasa. δ13C values ranged from - 26.40‰ to - 25.10‰, with relative higher values in spring and summer, reflecting the increment of fossil carbon emissions.

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

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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.

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

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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.

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

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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.

Composition and sources of carbonaceous aerosols in Northern Europe during winter

NARCIS (Netherlands)

Glasius, M.; Hansen, A.M.K.; Claeys, M.; Henzing, J.S.; Jedynska, A.D.; Kasper-Giebl, A.; Kistler, M.; Kristensen, K.; Martinsson, J.; Maenhaut, W.; Nøjgaard, J.K.; Spindler, G.; Stenström, K.E.; Swietlicki, E.; Szidat, S.; Simpson, D.; Yttri, K.E.

2018-01-01

Sources of elemental carbon (EC) and organic carbon (OC) in atmospheric aerosols (carbonaceous aerosols) were investigated by collection of weekly aerosol filter samples at six background sites in Northern Europe (Birkenes, Norway; Vavihill, Sweden; Risoe, Denmark; Cabauw and Rotterdam in The

Development of a preparation system for the radiocarbon analysis of organic carbon in carbonaceous aerosols in China

International Nuclear Information System (INIS)

Zhang, Y.L.; Liu, D.; Shen, C.D.; Ding, P.; Zhang, G.

2010-01-01

Carbonaceous aerosols comprising a large fraction of elemental carbon (EC) and organic carbon (OC) are considered to affect both global climate and human health. Radiocarbon measurements have been proved to be a useful isotopic tracer for distinguishing contemporary and fossil emissions. An optimized system of a two-step thermal preparation system for radiocarbon ( 14 C) measurement of OC/TC is firstly established in China. In this system, OC/TC are converted into carbon dioxide under a pure oxygen flow at 340 o C/650 o C and then reduced to graphite for AMS target using the method of zinc reduction. Afterwards, radiocarbon measurements of the targets performed by the NEC Compact AMS System at the Institute of Heavy Ion Physics, Peking University. The measured results for estimated reference martial including HOx I, HOx II and IAEA-C6 are consistent with internationally accepted values. The radiocarbon-based source appointment of carbonaceous aerosols in China would be much more convenient and faster with the preparation system developed in this work.

Impact of Idealized Stratospheric Aerosol Injection on the Future Ocean and Land Carbon Cycles

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Tjiputra, J.; Lauvset, S.

2017-12-01

Using a state-of-the-art Earth system model, we simulate stratospheric aerosol injection (SAI) on top of the Representative Concentration Pathways 8.5 future scenario. Our idealized method prescribes aerosol concentration, linearly increasing from 2020 to 2100, and thereafter remaining constant until 2200. In one of the scenarios, the model able to project future warming below 2 degree toward 2100, despite greatier warming persists in the high latitudes. When SAI is terminated in 2100, a rapid global warming of 0.35 K yr-1 (as compared to 0.05 K yr-1 under RCP8.5) is simulated in the subsequent 10 years, and the global mean temperature rapidly returns to levels close to the reference state. In contrast to earlier findings, we show a weak response in the terrestrial carbon sink during SAI implementation in the 21st century, which we attribute to nitrogen limitation. The SAI increases the land carbon uptake in the temperate forest-, grassland-, and shrub-dominated regions. The resultant lower temperatures lead to a reduction in the heterotrophic respiration rate and increase soil carbon retention. Changes in precipitation patterns are key drivers for variability in vegetation carbon. Upon SAI termination, the level of vegetation carbon storage returns to the reference case, whereas the soil carbon remains high. The ocean absorbs nearly 10% more carbon in the geoengineered simulation than in the reference simulation, leading to a ˜15 ppm lower atmospheric CO2 concentration in 2100. The largest enhancement in uptake occurs in the North Atlantic. In both hemispheres' polar regions, SAI delays the sea ice melting and, consequently, export production remains low. Despite inducing little impact on surface acidification, in the deep water of North Atlantic, SAI-induced circulation changes accelerate the ocean acidification rate and broaden the affected area. Since the deep ocean provides vital ecosystem function and services, e.g., fish stocks, this accelerated changes

Modeling the radiative effects of biomass burning aerosols on carbon fluxes in the Amazon region

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Moreira, Demerval S.; Longo, Karla M.; Freitas, Saulo R.; Yamasoe, Marcia A.; Mercado, Lina M.; Rosário, Nilton E.; Gloor, Emauel; Viana, Rosane S. M.; Miller, John B.; Gatti, Luciana V.; Wiedemann, Kenia T.; Domingues, Lucas K. G.; Correia, Caio C. S.

2017-12-01

Every year, a dense smoke haze covers a large portion of South America originating from fires in the Amazon Basin and central parts of Brazil during the dry biomass burning season between August and October. Over a large portion of South America, the average aerosol optical depth at 550 nm exceeds 1.0 during the fire season, while the background value during the rainy season is below 0.2. Biomass burning aerosol particles increase scattering and absorption of the incident solar radiation. The regional-scale aerosol layer reduces the amount of solar energy reaching the surface, cools the near-surface air, and increases the diffuse radiation fraction over a large disturbed area of the Amazon rainforest. These factors affect the energy and CO2 fluxes at the surface. In this work, we applied a fully integrated atmospheric model to assess the impact of biomass burning aerosols in CO2 fluxes in the Amazon region during 2010. We address the effects of the attenuation of global solar radiation and the enhancement of the diffuse solar radiation flux inside the vegetation canopy. Our results indicate that biomass burning aerosols led to increases of about 27 % in the gross primary productivity of Amazonia and 10 % in plant respiration as well as a decline in soil respiration of 3 %. Consequently, in our model Amazonia became a net carbon sink; net ecosystem exchange during September 2010 dropped from +101 to -104 TgC when the aerosol effects are considered, mainly due to the aerosol diffuse radiation effect. For the forest biome, our results point to a dominance of the diffuse radiation effect on CO2 fluxes, reaching a balance of 50-50 % between the diffuse and direct aerosol effects for high aerosol loads. For C3 grasses and savanna (cerrado), as expected, the contribution of the diffuse radiation effect is much lower, tending to zero with the increase in aerosol load. Taking all biomes together, our model shows the Amazon during the dry season, in the presence of high

Modeling the radiative effects of biomass burning aerosols on carbon fluxes in the Amazon region

Directory of Open Access Journals (Sweden)

D. S. Moreira

2017-12-01

Full Text Available Every year, a dense smoke haze covers a large portion of South America originating from fires in the Amazon Basin and central parts of Brazil during the dry biomass burning season between August and October. Over a large portion of South America, the average aerosol optical depth at 550 nm exceeds 1.0 during the fire season, while the background value during the rainy season is below 0.2. Biomass burning aerosol particles increase scattering and absorption of the incident solar radiation. The regional-scale aerosol layer reduces the amount of solar energy reaching the surface, cools the near-surface air, and increases the diffuse radiation fraction over a large disturbed area of the Amazon rainforest. These factors affect the energy and CO2 fluxes at the surface. In this work, we applied a fully integrated atmospheric model to assess the impact of biomass burning aerosols in CO2 fluxes in the Amazon region during 2010. We address the effects of the attenuation of global solar radiation and the enhancement of the diffuse solar radiation flux inside the vegetation canopy. Our results indicate that biomass burning aerosols led to increases of about 27 % in the gross primary productivity of Amazonia and 10 % in plant respiration as well as a decline in soil respiration of 3 %. Consequently, in our model Amazonia became a net carbon sink; net ecosystem exchange during September 2010 dropped from +101 to −104 TgC when the aerosol effects are considered, mainly due to the aerosol diffuse radiation effect. For the forest biome, our results point to a dominance of the diffuse radiation effect on CO2 fluxes, reaching a balance of 50–50 % between the diffuse and direct aerosol effects for high aerosol loads. For C3 grasses and savanna (cerrado, as expected, the contribution of the diffuse radiation effect is much lower, tending to zero with the increase in aerosol load. Taking all biomes together, our model shows the Amazon during the dry

Impact of idealized future stratospheric aerosol injection on the large-scale ocean and land carbon cycles

Science.gov (United States)

Tjiputra, J. F.; Grini, A.; Lee, H.

2016-01-01

Using an Earth system model, we simulate stratospheric aerosol injection (SAI) on top of the Representative Concentration Pathways 8.5 future scenario. Our idealized method prescribes aerosol concentration, linearly increasing from 2020 to 2100, and thereafter remaining constant until 2200. In the aggressive scenario, the model projects a cooling trend toward 2100 despite warming that persists in the high latitudes. Following SAI termination in 2100, a rapid global warming of 0.35 K yr-1 is simulated in the subsequent 10 years, and the global mean temperature returns to levels close to the reference state, though roughly 0.5 K cooler. In contrast to earlier findings, we show a weak response in the terrestrial carbon sink during SAI implementation in the 21st century, which we attribute to nitrogen limitation. The SAI increases the land carbon uptake in the temperate forest-, grassland-, and shrub-dominated regions. The resultant lower temperatures lead to a reduction in the heterotrophic respiration rate and increase soil carbon retention. Changes in precipitation patterns are key drivers for variability in vegetation carbon. Upon SAI termination, the level of vegetation carbon storage returns to the reference case, whereas the soil carbon remains high. The ocean absorbs nearly 10% more carbon in the geoengineered simulation than in the reference simulation, leading to a ˜15 ppm lower atmospheric CO2 concentration in 2100. The largest enhancement in uptake occurs in the North Atlantic. In both hemispheres' polar regions, SAI delays the sea ice melting and, consequently, export production remains low. In the deep water of North Atlantic, SAI-induced circulation changes accelerate the ocean acidification rate and broaden the affected area.

Linking Aerosol Optical Properties Between Laboratory, Field, and Model Studies

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Murphy, S. M.; Pokhrel, R. P.; Foster, K. A.; Brown, H.; Liu, X.

2017-12-01

The optical properties of aerosol emissions from biomass burning have a significant impact on the Earth's radiative balance. Based on measurements made during the Fourth Fire Lab in Missoula Experiment, our group published a series of parameterizations that related optical properties (single scattering albedo and absorption due to brown carbon at multiple wavelengths) to the elemental to total carbon ratio of aerosols emitted from biomass burning. In this presentation, the ability of these parameterizations to simulate the optical properties of ambient aerosol is assessed using observations collected in 2017 from our mobile laboratory chasing wildfires in the Western United States. The ambient data includes measurements of multi-wavelength absorption, scattering, and extinction, size distribution, chemical composition, and volatility. In addition to testing the laboratory parameterizations, this combination of measurements allows us to assess the ability of core-shell Mie Theory to replicate observations and to assess the impact of brown carbon and mixing state on optical properties. Finally, both laboratory and ambient data are compared to the optical properties generated by a prominent climate model (Community Earth System Model (CESM) coupled with the Community Atmosphere Model (CAM 5)). The discrepancies between lab observations, ambient observations and model output will be discussed.

Sources and formation mechanisms of carbonaceous aerosol at a regional background site in the Netherlands : insights from a year-long radiocarbon study

NARCIS (Netherlands)

Dusek, Ulrike; Hitzenberger, Regina; Kasper-Giebl, Anne; Kistler, Magdalena; Meijer, Harro A. J.; Szidat, Sonke; Wacker, Lukas; Holzinger, Rupert; Rockmann, Thomas

2017-01-01

We measured the radioactive carbon isotope C-14 (radiocarbon) in various fractions of the carbonaceous aerosol sampled between February 2011 and March 2012 at the Cesar Observatory in the Netherlands. Based on the radiocarbon content in total carbon (TC), organic carbon (OC), water-insoluble organic

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.

Empirical analysis of aerosol and thin cloud optical depth effects on CO2 retrievals from GOSAT

Science.gov (United States)

Saha, A.; O'Neill, N. T.; Strong, K.; Nakajima, T.; Uchino, O.; Shiobara, M.

2014-12-01

Ground-based sunphotometer observations of aerosol and cloud optical properties at AEROCAN / AERONET sites co-located with TCCON (Total Carbon Column Observing Network) high resolution Fourier Transform Spectrometers (FTS) were used to investigate the aerosol and cloud influence on column-averaged dry-air mole fraction of carbon dioxide (XCO2) retrieved from the TANSO-FTS (Thermal And Near-infrared Sensor for carbon Observation - FTS) of GOSAT (Greenhouse gases Observing SATellite). This instrument employs high resolution spectra measured in the Short-Wavelength InfraRed (SWIR) band to retrieve XCO2estimates. GOSAT XCO2 retrievals are nominally corrected for the contaminating backscatter influence of aerosols and thin clouds. However if the satellite-retrieved aerosol and thin cloud optical depths applied to the CO2 correction is biased then the correction and the retrieved CO2 values will be biased. We employed independent ground based estimates of both cloud screened and non cloud screened AOD (aerosol optical depth) in the CO2 SWIR channel and compared this with the GOSAT SWIR-channel OD retrievals to see if that bias was related to variations in the (generally negative) CO2 bias (ΔXCO2= XCO2(GOSAT) - XCO2(TCCON)). Results are presented for a number of TCCON validation sites.

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.

Seasonal variations in size distribution, water-soluble ions, and carbon content of size-segregated aerosols over New Delhi.

Science.gov (United States)

Kumar, Pawan; Kumar, Sushil; Yadav, Sudesh

2018-02-01

Size distribution, water-soluble inorganic ions (WSII), and organic carbon (OC) and elemental carbon (EC) in size-segregated aerosols were investigated during a year-long sampling in 2010 over New Delhi. Among different size fractions of PM 10 , PM 0.95 was the dominant fraction (45%) followed by PM 3-7.2 (20%), PM 7.2-10 (15%), PM 0.95-1.5 (10%), and PM 1.5-3 (10%). All size fractions exceeded the ambient air quality standards of India for PM 2.5 . Annual average mass size distributions of ions were specific to size and ion(s); Ca 2+ , Mg 2+ , K + , NO 3 - , and Cl - followed bimodal distribution while SO 4 2- and NH 4 + ions showed one mode in PM 0.95 . The concentrations of secondary WSII (NO 3 - , SO 4 2- , and NH 4 + ) increased in winters due to closed and moist atmosphere whereas open atmospheric conditions in summers lead to dispersal of pollutants. NH 4 + and Ca 2+ were dominant neutralization ions but in different size fractions. The summer-time dust transport from upwind region by S SW winds resulted in significantly high concentrations of PM 0.95 and PM 3-7.2 and PM 7.2-10 . This indicted influence of dust generation in Thar Desert and its transport is size selective in nature in downwind direction. The mixing of different sources (geogenic, coal combustions, biomass burning, plastic burning, incinerators, and vehicular emissions sources) for soluble ions in different size fractions was noticed in principle component analysis. Total carbon (TC = EC + OC) constituted 8-31% of the total PM 0.95 mass, and OC dominated over EC. Among EC, char (EC1) dominated over soot (EC2 + EC3). High SOC contribution (82%) to OC and OC/EC ratio of 2.7 suggested possible role of mineral dust and high photochemical activity in SOC production. Mass concentrations of aerosols and WSII and their contributions to each size fraction of PM 10 are governed by nature of sources, emission strength of source(s), and seasonality in meteorological parameters.

Mercury bonds with carbon (OC and EC) in small aerosols (PM1) in the urbanized coastal zone of the Gulf of Gdansk (southern Baltic).

Science.gov (United States)

Lewandowska, A U; Bełdowska, M; Witkowska, A; Falkowska, L; Wiśniewska, K

2018-08-15

PM1 aerosols were collected at the coastal station in Gdynia between 1st January and 31st December 2012. The main purpose of the study was to determine the variability in concentrations of mercury Hg(p), organic carbon (OC) and elemental carbon (EC) in PM1 aerosols under varying synoptic conditions in heating and non-heating periods. Additionally, sources of origin and bonds of mercury with carbon species were identified. The highest concentrations of Hg(p), OC and EC were found during the heating period. Then all analyzed PM1 components had a common, local origin related to the consumption of fossil fuels for heating purposes under conditions of lower air temperatures and poor dispersion of pollutants. Long periods without precipitation also led to the increase in concentration of all measured PM1 compounds. In heating period mercury correlated well with elemental carbon and primary and secondary organic carbon when air masses were transported from over the land. At that time, the role of transportation was of minor importance. In the non-heating period, the concentration of all analyzed compounds were lower than in the heating period, which could be associated with the reduced influence of combustion processes, higher precipitation and, in the case of mercury, also the evaporation of aerosols at higher air temperatures. However, when air masses were transported from over the sea or from the port/shipyard areas the mercury concentration increased significantly. In the first case higher air humidity, solar radiation and ozone concentration as well as the presence of marine aerosols could further facilitate the conversion of gaseous mercury into particulate mercury and its concentration increase. In the second case Hg(p) could be adsorbed on particles rich in elemental carbon and primary organic carbon emitted from ships. Copyright © 2018 Elsevier Inc. All rights reserved.

Cassini CAPS-ELS observations of carbon-based anions and aerosol growth in Titan's ionosphere

Science.gov (United States)

Desai, Ravindra; Coates, Andrew; Wellbrock, Anne; Kataria, Dhiren; Jones, Geraint; Lewis, Gethyn; Waite, J.

2016-06-01

Cassini observations of Titans ionosphere revealed an atmosphere rich in positively charged ions with masses up to > 350 amu and negatively charged ions and aerosols with mass over charge ratios as high as 13,800 amu/q. The detection of negatively charged molecules by the Cassini CAPS Electron Spectrometer (CAPS-ELS) was particularly surprising and showed how the synthesis of large aerosol-size particles takes place at altitudes much greater than previously thought. Here, we present further analysis into this CAPS-ELS dataset, through an enhanced understanding of the instrument's response function. In previous studies the intrinsic E/E energy resolution of the instrument did not allow specific species to be identified and the detections were classified into broad mass ranges. In this study we use an updated fitting procedure to show how the ELS mass spectrum can be resolved into specific peaks at multiples of carbon-based anions up to > 100 amu/q. The negatively charged ions and aerosols in Titans ionosphere increase in mass with decreasing altitude, the lightest species being observed close to Titan's exobase of ˜1,450km and heaviest species observed at altitudes < 950km. We identify key stages in this apparent growth process and report on key intermediaries which appear to trigger the rapid growth of the larger aerosol-size particles.

TOMS Absorbing Aerosol Index

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Washington University St Louis — TOMS_AI_G is an aerosol related dataset derived from the Total Ozone Monitoring Satellite (TOMS) Sensor. The TOMS aerosol index arises from absorbing aerosols such...

Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

Directory of Open Access Journals (Sweden)

Y.-L. Zhang

2018-03-01

Full Text Available 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.

Influence of wildfires in the boreal forests of Eastern Siberia on atmospheric aerosol parameters

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Tomshin, Oleg A.; Solovyev, Vladimir S.

2017-11-01

The results of studies of the dynamics of forest fires in the boreal forests of Yakutia (Eastern Siberia) for 2001-2016 are presented. Variations of aerosol optical thickness (AOT), aerosol index (AI) and total carbon monoxide content during May-September were studied depending on the different forest fire activity level. It is shown that the seasonal variations of AOT, AI and CO in the most fire-dangerous years differ significantly from the fire seasons when forest fire activity was medium or low.

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.

Multiple scattering of light by water cloud droplets with external and internal mixing of black carbon aerosols

International Nuclear Information System (INIS)

Wang Hai-Hua; Sun Xian-Ming

2012-01-01

The mixture of water cloud droplets with black carbon impurities is modeled by external and internal mixing models. The internal mixing model is modeled with a two-layered sphere (water cloud droplets containing black carbon (BC) inclusions), and the single scattering and absorption characteristics are calculated at the visible wavelength of 0.55 μm by using the Lorenz—Mie theory. The external mixing model is developed assuming that the same amount of BC particles are mixed with the water droplets externally. The multiple scattering characteristics are computed by using the Monte Carlo method. The results show that when the size of the BC aerosol is small, the reflection intensity of the internal mixing model is bigger than that of the external mixing model. However, if the size of the BC aerosol is big, the absorption of the internal mixing model will be larger than that of the external mixing model. (electromagnetism, optics, acoustics, heat transfer, classical mechanics, and fluid dynamics)

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 α_380–870 values (1.27±0.09 are found over the eastern BoB. Except from the large α_380–870 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.

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.

Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

Directory of Open Access Journals (Sweden)

K. E. Yttri

2011-12-01

Full Text Available In the present study, natural and anthropogenic sources of particulate organic carbon (OC_p and elemental carbon (EC have been quantified based on weekly filter samples of PM₁₀ (particles with aerodynamic diameter <10 μm collected at four Nordic rural background sites [Birkenes (Norway, Hyytiälä (Finland, Vavihill (Sweden, Lille Valby, (Denmark] during late summer (5 August–2 September 2009. Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the ¹⁴C/¹²C ratio of total carbon (TC, have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TC_p; i.e. particulate TC was totally dominated by natural sources (69–86%, with biogenic secondary organic aerosol (BSOA being the single most important source (48–57%. Interestingly, primary biological aerosol particles (PBAP were the second most important source (20–32%. The anthropogenic contribution was mainly attributed to fossil fuel sources (OC_ff and EC_ff (10–24%, whereas no more than 3–7% was explained by combustion of biomass (OC_bb and EC_bb in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, which accounted for 4–12% of TC_p, whereas <1.5% of EC was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

Science.gov (United States)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

Aerosol absorption coefficient and Equivalent Black Carbon by parallel operation of AE31 and AE33 aethalometers at the Zeppelin station, Ny Ålesund, Svalbard

Science.gov (United States)

Eleftheriadis, Konstantinos; Kalogridis, Athina-Cerise; Vratolis, Sterios; Fiebig, Markus

2016-04-01

Light absorbing carbon in atmospheric aerosol plays a critical role in radiative forcing and climate change. Despite the long term measurements across the Arctic, comparing data obtained by a variety of methods across stations requires caution. A method for extracting the aerosol absorption coefficient from data obtained over the decades by filter based instrument is still under development. An IASOA Aerosol working group has been initiated to address this and other cross-site aerosol comparison opportunities. Continuous ambient measurements of EBC/light attenuation by means of a Magee Sci. AE-31 aethalometer operating at the Zeppelinfjellet station (474 m asl; 78°54'N, 11°53'E), Ny Ålesund, Svalbard, have been available since 2001 (Eleftheriadis et al, 2009), while a new aethalometer model (AE33, Drinovec et al, 2014) has been installed to operate in parallel from the same inlet since June 2015. Measurements are recorded by a Labview routine collecting all available parameters reported by the two instrument via RS232 protocol. Data are reported at 1 and 10 minute intervals as averages for EBC (μg m-3) and aerosol absorption coefficients (Mm-1) by means of routine designed to report Near Real Time NRT data at the EBAS WDCA database (ebas.nilu.no) Results for the first 6 month period are reported here in an attempt to evaluate comparative performance of the two instruments in terms of their response with respect to the variable aerosol load of light absorbing carbon during the warm and cold seasons found in the high arctic. The application of available conversion schemes for obtaining the absorption coefficient by the two instruments is found to demonstrate a marked difference in their output. During clean periods of low aerosol load (EBC origin was also conducted. Drinovec, L., Močnik, G., Zotter, P., Prévôt, A. S. H., Ruckstuhl, C., Coz, E., Rupakheti, M., Sciare, J., Müller, T., Wiedensohler, A., and Hansen, A. D. A. The "dual-spot" Aethalometer: an

Comprehensive characterisation of atmospheric aerosols in Budapest, Hungary: physicochemical properties of inorganic species

Science.gov (United States)

Salma, Imre; Maenhaut, Willy; Zemplén-Papp, Éva; Záray, Gyula

As part of an air pollution project in Budapest, aerosol samples were collected by stacked filter units and cascade impactors at an urban background site, two downtown sites, and within a road tunnel in field campaigns conducted in 1996, 1998 and 1999. Some criteria pollutants were also measured at one of the downtown sites. The aerosol samples were analysed by one or more of the following methods: instrumental neutron activation analysis, particle-induced X-ray emission analysis, a light reflection technique, gravimetry, thermal profiling carbon analysis and capillary electrophoresis. The quantities measured or derived include atmospheric concentrations of elements (from Na to U), of particulate matter, of black and elemental carbon, and total carbonaceous fraction, of some ionic species (e.g., nitrate and sulphate) in the fine ( EAD) or in both coarse (10- 2 μm EAD) and fine size fractions, atmospheric concentrations of NO, NO 2, SO 2, CO and total suspended particulate matter, and meteorological parameters. The analytical results were used for characterisation of the concentration levels, elemental composition, time trends, enrichment of and relationships among the aerosol species in coarse and fine size fractions, for studying their fine-to-coarse concentration ratios, spatial and temporal variability, for determining detailed elemental mass size distributions, and for examining the extent of chemical mass closure.

Characteristics and sources of carbonaceous aerosols from Shanghai, China

Science.gov (United States)

Cao, J.-J.; Zhu, C.-S.; Tie, X.-X.; Geng, F.-H.; Xu, H.-M.; Ho, S. S. H.; Wang, G.-H.; Han, Y.-M.; Ho, K.-F.

2013-01-01

An intensive investigation of carbonaceous PM2.5 and TSP (total suspended particles) from Pudong (China) was conducted as part of the MIRAGE-Shanghai (Megacities Impact on Regional and Global Environment) experiment in 2009. Data for organic and elemental carbon (OC and EC), organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs), and stable carbon isotopes OC (δ13COC) and EC (δ13CEC) were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA); high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = -24.5 ± 0.8‰ and δ13CEC = -25.1 ± 0.6‰) indicated that fossil fuels were the most important source for carbonaceous PM2.5 (particulate matter less than 2.5 micrometers in diameter), with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%; other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

Optical absorption characteristics of brown carbon aerosols during the KORUS-AQ campaign at an urban site

Science.gov (United States)

Park, Seungshik; Yu, Geun-Hye; Lee, Sangil

2018-05-01

This study investigates the absorption characteristics of brown carbon (BrC) obtained from water and methanol extracts of fine particulate matter measured at an urban site in Gwangju, Korea during the KOREA U.S. - Air Quality campaign (May 2-June 11, 2016). The measurement period was classified into two intervals: biomass burning (BB) and non-BB periods. During the non-BB period, water-soluble organic carbon (WSOC) and humic-like substances (HULIS) primarily resulted from secondary organic aerosol (SOA) formation and primary vehicle emissions. Water-soluble organic aerosols during the BB period, meanwhile, were closely related to SOA formation and regionally transported BB emissions. The light absorption coefficient measured at 365 nm (babs,365) by methanol extracts was 2.6 and 6.1 times higher than the coefficients from the water and HULIS extracts, respectively, indicating the importance of BrC absorption by water-insoluble organic carbon. This was demonstrated by a good correlation between the water-insoluble BrC absorption and the elemental carbon concentration. A comparison of babs,365 between the methanol- and water-extracted BrC indicated that water-insoluble BrC accounted for approximately 61% (33-86%) of the total BrC absorption. The contributions of SOA, primary BB emissions, and traffic emissions to the water extract babs,365 were estimated using a stepwise multiple linear regression (MLR) analysis and found to be 1.17 ± 0.55, 0.65 ± 0.62, and 0.25 ± 0.09 Mm- 1, respectively, accounting for 59.6, 26.1, and 14.3% of the absorption coefficient by the water-soluble BrC. Further, it was determined that the contribution of the BB emissions to the water-soluble BrC absorption was approximately two times higher in the BB period than in the non-BB period. The average absorption Ångstrӧm exponent was 4.8 ± 0.3, 5.3 ± 0.7, and 6.8 ± 0.8 for the methanol, water, and HULIS extracts, respectively. The average mass absorption efficiency (MAE365) of methanol

Aerosols emitted in underground mine air by diesel engine fueled with biodiesel.

Science.gov (United States)

Bugarski, Aleksandar D; Cauda, Emanuele G; Janisko, Samuel J; Hummer, Jon A; Patts, Larry D

2010-02-01

Using biodiesel in place of petroleum diesel is considered by several underground metal and nonmetal mine operators to be a viable strategy for reducing the exposure of miners to diesel particulate matter. This study was conducted in an underground experimental mine to evaluate the effects of soy methyl ester biodiesel on the concentrations and size distributions of diesel aerosols and nitric oxides in mine air. The objective was to compare the effects of neat and blended biodiesel fuels with those of ultralow sulfur petroleum diesel. The evaluation was performed using a mechanically controlled, naturally aspirated diesel engine equipped with a muffler and a diesel oxidation catalyst. The effects of biodiesel fuels on size distributions and number and total aerosol mass concentrations were found to be strongly dependent on engine operating conditions. When fueled with biodiesel fuels, the engine contributed less to elemental carbon concentrations for all engine operating modes and exhaust configurations. The substantial increases in number concentrations and fraction of organic carbon (OC) in total carbon over the baseline were observed when the engine was fueled with biodiesel fuels and operated at light-load operating conditions. Size distributions for all test conditions were found to be single modal and strongly affected by engine operating conditions, fuel type, and exhaust configuration. The peak and total number concentrations as well as median diameter decreased with an increase in the fraction of biodiesel in the fuels, particularly for high-load operating conditions. The effects of the diesel oxidation catalyst, commonly deployed to counteract the potential increase in OC emissions due to use of biodiesel, were found to vary depending upon fuel formulation and engine operating conditions. The catalyst was relatively effective in reducing aerosol number and mass concentrations, particularly at light-load conditions, but also showed the potential for an

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.

Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

Science.gov (United States)

Dreyfus, Matthew A.

. The high-time resolution data shows that rapid concentration changes of a common individual species can be lost with traditional bulk sampling, and a time resolution of 30 minutes is suggested to accurately represent these changes. Using the mass spectra collected from the extended sampling campaign, source apportionment was performed with positive matrix factorization (PMF). The resulting model features six factors either correlated to specific sources (meat cooking, car emissions/road dust, diesel exhaust) or types of compounds (phthalates, alkanes/alkanoic acids, PAHs). The high-time resolution data allowed for the observation of specific trends in each factor's behavior as a function of time and wind direction relative to the receptor site. Elemental carbon/organic carbon (EC/OC) data is used to calculate the percentages of primary and secondary organic aerosol. Primary organic aerosol (POA) constituted the vast majority of the total carbon at 91% (an average of 2.8 +/- 1.1mug/m 3); 30% of which came from combustion, and 70% from non-combustion sources. These results can be explained by the PIAMS data: the diesel factor contributes to the combustion-related POA; the car/road dust, meat cooking, and alkane/alkanoic acid factors contribute the majority of non-combustion POA. The remaining factors represent products from the ozonolysis of various monoterpenes. The product ion peaks observed indicates that both the stabilized Criegee intermediate pathway and the hydroperoxide channel are both active pathways in yielding dimers and high-order oligomer.

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

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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.

Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

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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.

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.)

Carbon isotope components of aerosol in Fukuoka, Nagoya, Suwa and Kamikochi

International Nuclear Information System (INIS)

Ikemori, Fumikazu; Higo, Hayato; Miyabara, Yuichi; Nakajima, Daisuke; Nakamura, Toshio

2013-01-01

To estimate the contributions of fossil carbon and biomass carbon in some regions in Japan, 14 C concentration of total carbon in Total suspended particles (TSP) was measured at four places (Nagoya, Fukuoka, Suwa and Kamikochi) in Japan. pMC (% Modern Carbon) showed lowest average value of pMC (50.5±5.6: n =43) in Nagoya. The average value of pMC in Fukuoka (56.7±7.7 : n=26) and Suwa (pMC=66.9±8.8 : n=12) were larger than the average value of pMC in Nagoya. In Kamikochi, the average value of pMC measured two samples only was largest pMC (102, 97.9) in four places. The correlations among organic carbon (OC), elemental carbon (EC), fossil carbon, biomass carbon and OC/EC showed different values in Nagoya, Fukuoka and Suwa. These results suggest that the carbon sources were different at three regions. (author)

Aerosol transport from Chiang Mai, Thailand to Mt. Lulin, Taiwan - Implication of aerosol aging during long-range transport

Science.gov (United States)

Chuang, Ming-Tung; Lee, Chung-Te; Chou, Charles C.-K.; Engling, Guenter; Chang, Shih-Yu; Chang, Shuenn-Chin; Sheu, Guey-Rong; Lin, Neng-Huei; Sopajaree, Khajornsak; Chang, You-Jia; Hong, Guo-Jun

2016-07-01

The transport of biomass burning (BB) aerosol from Indochina may cause a potential effect on climate change in Southeast Asia, East Asia, and the Western Pacific. Up to now, the understanding of BB aerosol composition modification during long-range transport (LRT) is still very limited due to the lack of observational data. In this study, atmospheric aerosols were collected at the Suthep/Doi Ang Khang (DAK) mountain sites in Chiang Mai, Thailand and the Lulin Atmospheric Background Station (Mt. Lulin) in central Taiwan from March to April 2010 and from February to April 2013, respectively. During the study period, an upwind and downwind relationship between the Suthep/DAK and Lulin sites (2400 km apart) was validated by backward trajectories. Comprehensive aerosol properties were resolved for PM2.5 water-soluble inorganic ions, carbonaceous content, water-soluble/insoluble organic carbon (WSOC/WIOC), dicarboxylic acids and their salts (DCAS), and anhydrosugars. A Modification Factor (MF) is proposed by employing non-sea-salt potassium ion (nss-K+) or fractionalized elemental carbon evolved at 580 °C after pyrolized OC correction (EC1-OP) as a BB aerosol tracer to evaluate the mass fraction changes of aerosol components from source to receptor regions during LRT. The MF values of nss-SO42-, NH4+, NO3-, OC1 (fractionalized organic carbon evolved from room temperature to 140 °C), OP (pyrolized OC fraction), DCAS, and WSOC were above unity, which indicated that these aerosol components were enhanced during LRT as compared with those in the near-source region. In contrast, the MF values of anhydrosugars ranged from 0.1 to 0.3, indicating anhydrosugars have degraded during LRT.

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

Automated determination of the stable carbon isotopic composition (δ13C) of total dissolved inorganic carbon (DIC) and total nonpurgeable dissolved organic carbon (DOC) in aqueous samples: RSIL lab codes 1851 and 1852

Science.gov (United States)

Révész, Kinga M.; Doctor, Daniel H.

2014-01-01

The purposes of the Reston Stable Isotope Laboratory (RSIL) lab codes 1851 and 1852 are to determine the total carbon mass and the ratio of the stable isotopes of carbon (δ13C) for total dissolved inorganic carbon (DIC, lab code 1851) and total nonpurgeable dissolved organic carbon (DOC, lab code 1852) in aqueous samples. The analysis procedure is automated according to a method that utilizes a total carbon analyzer as a peripheral sample preparation device for analysis of carbon dioxide (CO2) gas by a continuous-flow isotope ratio mass spectrometer (CF-IRMS). The carbon analyzer produces CO2 and determines the carbon mass in parts per million (ppm) of DIC and DOC in each sample separately, and the CF-IRMS determines the carbon isotope ratio of the produced CO2. This configuration provides a fully automated analysis of total carbon mass and δ13C with no operator intervention, additional sample preparation, or other manual analysis. To determine the DIC, the carbon analyzer transfers a specified sample volume to a heated (70 °C) reaction vessel with a preprogrammed volume of 10% phosphoric acid (H3PO4), which allows the carbonate and bicarbonate species in the sample to dissociate to CO2. The CO2 from the reacted sample is subsequently purged with a flow of helium gas that sweeps the CO2 through an infrared CO2 detector and quantifies the CO2. The CO2 is then carried through a high-temperature (650 °C) scrubber reactor, a series of water traps, and ultimately to the inlet of the mass spectrometer. For the analysis of total dissolved organic carbon, the carbon analyzer performs a second step on the sample in the heated reaction vessel during which a preprogrammed volume of sodium persulfate (Na2S2O8) is added, and the hydroxyl radicals oxidize the organics to CO2. Samples containing 2 ppm to 30,000 ppm of carbon are analyzed. The precision of the carbon isotope analysis is within 0.3 per mill for DIC, and within 0.5 per mill for DOC.

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

Wintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris

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M. Crippa

2013-01-01

Full Text Available The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36% and nitrate (28–29%, with lower contributions from sulfate (14–16%, ammonium (12–14% and black carbon (7–13%.

Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass, biomass burning (13–15% and cooking (up to 35% during meal hours. Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.

Aerosol processing in stratiform clouds in ECHAM6-HAM

Science.gov (United States)

Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

2013-04-01

Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the

Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer

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Y.-L. Sun

2011-02-01

Full Text Available Submicron aerosol particles (PM₁ were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM₁ mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (D_va and an accumulation mode (~550 nm that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00–02:00 p.m. EST due to photochemical production. The average (±σ oxygen-to-carbon (O/C, hydrogen-to-carbon (H/C, and nitrogen-to-carbon (N/C ratios of OA in NYC are 0.36 (±0.09, 1.49 (±0.08, and 0.012 (±0.005, respectively, corresponding to an average organic mass-to-carbon (OM/OC ratio of 1.62 (±0.11. Positive matrix factorization (PMF of the high resolution mass spectra identified two primary OA (POA sources, traffic and cooking, and three secondary OA (SOA components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63, a less oxidized, semi-volatile SV-OOA (O/C = 0.38 and a unique nitrogen-enriched OA (NOA; N/C = 0.053 characterized with prominent C_xH_{2x + 2}N⁺ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed

Organic and Elemental Carbon Aerosol Particulates at the Southern Great Plains Site Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Cary, Robert

2016-04-01

The purpose of this study was to measure the organic carbon (OC) and elemental carbon (EC) fractions of PM2.5 particulate matter at the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility Southern Great Plains (SGP) sampling site for a 6-month period during the summer of 2013. The site is in a rural location remote from any populated areas, so it would be expected to reflect carbon concentration over long-distance transport patterns. During the same period in 2012, a number of prairie fires in Oklahoma and Texas had produced large plumes of smoke particles, but OC and EC particles had not been quantified. In addition, during the summer months, other wild fires, such as forest fires in the Rocky Mountain states and other areas, can produce carbon aerosols that are transported over long distances. Both of these source types would be expected to contain mixtures of both OC and EC.

Long-term measurement of aerosol chemical composition in Athens, Greece.

Science.gov (United States)

Paraskevopoulou, Despina; Liakakou, Eleni; Theodosi, Christina; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

2014-05-01

The collection of our samples was conducted for a period of five years (2008 - 2013) in Athens, Greece. The site is situated at the premises of the National Observatory of Athens on Penteli Hill, northeast Athens suburbs, and is considered an urban background station. The aim of our study was a first long-term estimation of the chemical mass closure of aerosol. For the purposes of the study, we applied three filter samplers during the sampling period: two Partisol FRM Model 2000 air samplers (one of them collecting PM10 and the other PM2.5 fractions of aerosol) and one Dichotomous Partisol auto-sampler (with PM2.5 and PM2.5-10 inlet). Aerosols were collected on Whatman QM-A quartz fiber filters and the mass of the collected samples was estimated by weighing the pre-combusted filters before and after sampling, under controlled conditions, using a microbalance. All quartz filters were analysed for organic (OC) and elemental carbon (EC) by a thermal - optical transmission technique. The concentration of water soluble organic carbon (WSOC) was defined for each filter using a total organic carbon analyzer, while the content in main water soluble ions (Cl-, Br-, NO-3, SO4-2, PO4-3, C2O4-2, NH4+, K+, Na+, Mg+2, Ca+2) was determined by ion chromatography. Additionally the filters were analyzed for trace metals by inductively coupled plasma optical emission spectrometry (ICP-OES). Aerosol chemical mass closure calculations were conducted for the PM2.5 fraction. The area of Athens is characterized by aged aerosol that can originate from the marine boundary layer, the European mainland and occasionally from North African desert areas. The contribution of dust and particulate organic matter on PM levels was estimated taking into consideration the location of the sampling site, while identification and evaluation of sources was performed. Additionally, non-sea salt concentrations of the main ions were estimated to complete the chemical closure in the extended area. According to

Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

Science.gov (United States)

Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

2016-04-01

The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

Molecular Characterization of Organosulfates in Urban Aerosols during the Spring Festival by FT-ICR Mass Spectrometry

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Xie, Q.; Fu, P.

2017-12-01

Aerosol particles collected at daytime and nighttime in Beijing during the spring festival, including the episodes of various gradient level pollution and short-term pollution raised by fireworks, were analyzed using 15T Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS). Organosulfates (OSs), tracers for secondary organic aerosol formation, were identified through accurate mass measurements. Both the total number and the arbitrary abundance of OSs were consistent with the total OC concentrations of the aerosol samples. Nitrooxy-organosulfates were more abundant in the nighttime than those in the daytime due to high NOX concentrations at night. Although all subgroups OSs increased with the deterioration of air quality, especially for the relative abundance of aromatic OSs with high double bond equivalents, the percentage contributions of aliphatic OSs with low degree of unsaturation decreased. It was worth to note that aliphatic OSs with a wide range in carbon-chain length of C6-40 were identified in this study. The candidates for their potential precursors were alkanes and fatty acids. Moreover, a large number of aromatic OSs, about two thirds of OSs, were detected. The rapid formation of these compounds in New Year's Eve with plentiful aromatics from firework burning suggests that they may be derived from PAHs. The high carbon and oxygen contents of OSs may indicate the presence of dimmers, even polymers. Our results support the important contribution of anthropogenic precursors to OSs in ambient aerosols on the basis of aromatic and aliphatic OSs, which may have a significant impact on the hygroscopic properties of ambient aerosol particles.

The effect of aerosol on closure of the regionale short-wave radiation balance

NARCIS (Netherlands)

Henzing JS; Knap WH; Stammes P; ten Brink HM; Kos GPA; Even A; Swart DPJ; Bergwerff JP; Apituley A; NOP

2001-01-01

IPPC reports the aerosol radiative forcing per major aerosol category, like sulphate and fossil fuel derived carbon. Part of this carbon is reflective and part of the material (black carbon "soot") absorbs radiation. We find that in the Netherlands sulphate contributes some 30% to the

Apparatus for producing carbon-coated nanoparticles and carbon nanospheres

Energy Technology Data Exchange (ETDEWEB)

Perry, W. Lee; Weigle, John C.; Phillips, Jonathan

2015-10-20

An apparatus for producing carbon-coated nano- or micron-scale particles comprising a container for entraining particles in an aerosol gas, providing an inlet for carbon-containing gas, providing an inlet for plasma gas, a proximate torch for mixing the aerosol gas, the carbon-containing gas, and the plasma gas, bombarding the mixed gases with microwaves, and providing a collection device for gathering the resulting carbon-coated nano- or micron-scale particles. Also disclosed is a method and apparatus for making hollow carbon nano- or micro-scale spheres.

Studies on aerosol properties during ICARB–2006 campaign period ...

Indian Academy of Sciences (India)

Synchronous measurements of Aerosol Optical Depth (AOD), Black Carbon (BC) aerosol mass concentration and aerosol particle size distribution were carried out during the campaign period at tropical urban regions of Hyderabad, India. Daily satellite datasets of DMSP-OLS were processed for night-time forest fires over ...

Real time in situ detection of organic nitrates in atmospheric aerosols.

Science.gov (United States)

Rollins, Andrew W; Smith, Jared D; Wilson, Kevin R; Cohen, Ronald C

2010-07-15

A novel instrument is described that quantifies total particle-phase organic nitrates in real time with a detection limit of 0.11 microg m(-3) min(-1), 45 ppt min(-1) (-ONO(2)). Aerosol nitrates are separated from gas-phase nitrates with a short residence time activated carbon denuder. Detection of organic molecules containing -ONO(2) subunits is accomplished using thermal dissociation coupled to laser induced fluorescence detection of NO(2). This instrument is capable of high time resolution (seconds) measurements of particle-phase organic nitrates, without interference from inorganic nitrate. Here we use it to quantify organic nitrates in secondary organic aerosol generated from high-NO(x) photooxidation of limonene, alpha-pinene, Delta-3-carene, and tridecane. In these experiments the organic nitrate moiety is observed to be 6-15% of the total SOA mass.

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.

The influence of marine microbial activities on aerosol production: A laboratory mesocosm study

Science.gov (United States)

Alpert, Peter A.; Kilthau, Wendy P.; Bothe, Dylan W.; Radway, JoAnn C.; Aller, Josephine Y.; Knopf, Daniel A.

2015-09-01

The oceans cover most of the Earth's surface, contain nearly half the total global primary biomass productivity, and are a major source of atmospheric aerosol particles. Here we experimentally investigate links between biological activity in seawater and sea spray aerosol (SSA) flux, a relationship of potential significance for organic aerosol loading and cloud formation over the oceans and thus for climate globally. Bubbles were generated in laboratory mesocosm experiments either by recirculating impinging water jets or glass frits. Experiments were conducted with Atlantic Ocean seawater collected off the eastern end of Long Island, NY, and with artificial seawater containing cultures of bacteria and phytoplankton Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Changes in SSA size distributions occurred during all phases of bacterial and phytoplankton growth, as characterized by cell concentrations, dissolved organic carbon, total particulate carbon, and transparent exopolymer particles (gel-forming polysaccharides representing a major component of biogenic exudate material). Over a 2 week growth period, SSA particle concentrations increased by a factor of less than 2 when only bacteria were present and by a factor of about 3 when bacteria and phytoplankton were present. Production of jet-generated SSA particles of diameter less than 200 nm increased with time, while production of all particle diameters increased with time when frits were used. The implications of a marine biological activity dependent SSA flux are discussed.

Modelled radiative forcing of the direct aerosol effect with multi-observation evaluation

Directory of Open Access Journals (Sweden)

G. Myhre

2009-02-01

Full Text Available A high-resolution global aerosol model (Oslo CTM2 driven by meteorological data and allowing a comparison with a variety of aerosol observations is used to simulate radiative forcing (RF of the direct aerosol effect. The model simulates all main aerosol components, including several secondary components such as nitrate and secondary organic carbon. The model reproduces the main chemical composition and size features observed during large aerosol campaigns. Although the chemical composition compares best with ground-based measurement over land for modelled sulphate, no systematic differences are found for other compounds. The modelled aerosol optical depth (AOD is compared to remote sensed data from AERONET ground and MODIS and MISR satellite retrievals. To gain confidence in the aerosol modelling, we have tested its ability to reproduce daily variability in the aerosol content, and this is performing well in many regions; however, we also identified some locations where model improvements are needed. The annual mean regional pattern of AOD from the aerosol model is broadly similar to the AERONET and the satellite retrievals (mostly within 10–20%. We notice a significant improvement from MODIS Collection 4 to Collection 5 compared to AERONET data. Satellite derived estimates of aerosol radiative effect over ocean for clear sky conditions differs significantly on regional scales (almost up to a factor two, but also in the global mean. The Oslo CTM2 has an aerosol radiative effect close to the mean of the satellite derived estimates. We derive a radiative forcing (RF of the direct aerosol effect of −0.35 Wm⁻² in our base case. Implementation of a simple approach to consider internal black carbon (BC mixture results in a total RF of −0.28 Wm⁻². Our results highlight the importance of carbonaceous particles, producing stronger individual RF than considered in the recent IPCC estimate; however, net RF is less different

Enhanced UV Absorption in Carbonaceous Aerosols during MILAGRO and Identification of Potential Organic Contributors.

Science.gov (United States)

Mangu, A.; Kelley, K. L.; Marchany-Rivera, A.; Kilaparty, S.; Gunawan, G.; Gaffney, J. S.; Marley, N. A.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) during the month of March, 2006 by using a 7- channel aethalometer (Thermo-Anderson). These measurements, obtained at 370, 470, 520, 590, 660, 880, and 950 nm at a 5 minute time resolution, showed an enhanced absorption in the UV over that expected from carbon soot alone. Samples of fine atmospheric aerosols (less than 0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. The samples were collected on quartz fiber filters with high volume impactor samplers. The samples have been characterized for total carbon content (stable isotope ratio mass spectroscopy) and natural radionuclide tracers (210Pb, 210Po, 210Bi, 7Be, 13C, 14C, 40K, 15N). Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV-visible spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples (1). The continuous spectra also show an enhanced UV absorption over that expected from carbon soot and the general profiles are quite similar to those observed for humic and fulvic acids found as colloidal materials in surface and groundwaters (2), indicating the presence of humic-like substances (HULIS) in the fine aerosols. The spectra also show evidence of narrow band absorbers below 400 nm typical of polycyclic aromatics (PAH) and nitrated aromatic compounds. Spectra were also obtained on NIST standard diesel soot (SRM 2975), NIST standard air particulate matter (SRM 8785

Technical Report Series on Global Modeling and Data Assimilation. Volume 32; Estimates of AOD Trends (2002 - 2012) Over the World's Major Cities Based on the MERRA Aerosol Reanalysis

Science.gov (United States)

Provencal, Simon; Kishcha, Pavel; Elhacham, Emily; daSilva, Arlindo M.; Alpert, Pinhas; Suarez, Max J.

2014-01-01

NASA's Global Modeling and Assimilation Office has extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) tool with five atmospheric aerosol species (sulfates, organic carbon, black carbon, mineral dust and sea salt). This inclusion of aerosol reanalysis data is now known as MERRAero. This study analyses a ten-year period (July 2002 - June 2012) MERRAero aerosol reanalysis applied to the study of aerosol optical depth (AOD) and its trends for the aforementioned aerosol species over the world's major cities (with a population of over 2 million inhabitants). We found that a proportion of various aerosol species in total AOD exhibited a geographical dependence. Cities in industrialized regions (North America, Europe, central and eastern Asia) are characterized by a strong proportion of sulfate aerosols. Organic carbon aerosols are dominant over cities which are located in regions where biomass burning frequently occurs (South America and southern Africa). Mineral dust dominates other aerosol species in cities located in proximity to the major deserts (northern Africa and western Asia). Sea salt aerosols are prominent in coastal cities but are dominant aerosol species in very few of them. AOD trends are declining over cities in North America, Europe and Japan, as a result of effective air quality regulation. By contrast, the economic boom in China and India has led to increasing AOD trends over most cities in these two highly-populated countries. Increasing AOD trends over cities in the Middle East are caused by increasing desert dust.

Combustion characteristics of water-insoluble elemental and organic carbon in size selected ambient aerosol particles

Directory of Open Access Journals (Sweden)

K. Wittmaack

2005-01-01

Full Text Available Combustion of elemental carbon (EC and organic carbon (OC contained in ambient aerosol matter was explored using scanning electron microscopy (SEM in combination with energy dispersive X-ray analysis (EDX. To ease identification of the particles of interest and to avoid or at least reduce interaction with simultaneously sampled inorganic oxides and salts, the approach used in this work differed in two ways from commonly applied procedures. First, rather than using a mixture of particles of vastly different sizes, as in PM10 or PM2.5, aerosol matter was collected in a 5-stage impactor. Second, the water soluble fraction of the collected matter was removed prior to analysis. Diesel soot particles, which appeared in the well-known form of chain-type aggregates, constituted the major fraction of EC. In contrast, OC containing particles were observed in a variety of shapes, including a sizable amount of bioaerosol matter appearing mostly in the size range above about 1 µm. During heating in ambient air for 1h, diesel soot particles were found to be stable up to 470°C, but complete combustion occurred in a narrow temperature interval between about 480 and 510°C. After diesel soot combustion, minute quantities of 'ash' were observed in the form of aggregated tiny particles with sizes less than 10 nm. These particles could be due to elemental or oxidic contaminants of diesel soot. Combustion of OC was observed over a wide range of temperatures, from well below 200°C to at least 500°C. Incompletely burnt bioaerosol matter was still found after heating to 600°C. The results imply that the EC fraction in aerosol matter can be overestimated significantly if the contribution of OC to a thermogram is not well separated.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

Energy Technology Data Exchange (ETDEWEB)

Bluvshtein, Nir [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Lin, Peng [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Flores, J. Michel [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Segev, Lior [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Mazar, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Tas, Eran [The Robert H. Smith Faculty of Agriculture, Food and Environment, The Hebrew University of Jerusalem, Rehovot Israel; Snider, Graydon [Department of Physics and Atmospheric Science, Dalhousie University, Halifax Nova Scotia Canada; Weagle, Crystal [Department of Chemistry, Dalhousie University, Halifax Nova Scotia Canada; Brown, Steven S. [Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder Colorado USA; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder Colorado USA; Laskin, Alexander [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Rudich, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel

2017-05-23

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders of magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.

Carbonaceous and inorganic aerosols over a sub-urban site in peninsular India: Temporal variability and source characteristics

Science.gov (United States)

Aswini, A. R.; Hegde, Prashant; Nair, Prabha R.

2018-01-01

PM10 aerosol samples collected from a sub-urban site in Coimbatore during pre-monsoon, monsoon, post-monsoon and winter from 2014 to 2016 showed a large variability from 7.6 to 89 μg m- 3 with an annual average of 41 ± 21 μg m- 3 (N = 69). High abundance of PM10 and other components were recorded during winter and lowest during monsoon period. Total carbonaceous aerosols and water soluble ionic species contributed to 31% and 45% of PM10 mass respectively. SO42 - was the most abundant species (average 9.8 ± 4.8 μg m- 3) and constituted for 24% of total mass. Organic Carbon (OC) was the next most abundant species ranging from 1 to 16 μg m- 3 with an average of 7 ± 3.6 μg m- 3 accounting for 17% of PM10 mass concentration. POC (primary organic carbon) and SOC (secondary organic carbon) accounted for 56% and 44% of OC respectively. A major portion of OC ( 60%) was found to be water soluble. The correlation between OC and EC (elemental carbon) was found to be higher for night-time compared to daytime suggesting their origin from common sources during night-time. K+ was found to be strongly correlated with OC during night-time. WSOC showed good correlation with POC and K+ which was high especially during night-time. WSON (water soluble organic nitrogen) accounted for 34% of water soluble total nitrogen (WSTN). HCO3- exhibited significant positive correlation with Ca2 + during daytime indicating their crustal origin. The observations suggest that the region is influenced by biomass burning sources, however during day-time, secondary production and terrestrial sources (due to high temperature and wind) significantly influence the atmospheric aerosols over this region.

Mini Total Organic Carbon Analyzer (miniTOCA)

Data.gov (United States)

National Aeronautics and Space Administration — The objective of this development is to create a prototype hand-held, 1 to 2 liter size battery-powered Total Organic Carbon Analyzer (TOCA). The majority of...

Direct measurement of aerosol shape factors

International Nuclear Information System (INIS)

Zeller, W.

1983-12-01

The dynamic shape factor whereas the coagulation shape factor is an average over the total examined size range. The experiments have shown that the results of experiments with a certain aerosol system cannot be transferred to other aerosol systems without further consideration. The outer shape of particles of a certain size depends on the specific properties of the material as well as on the experimental conditions during the aerosol generation. For both aerosol systems examined the mean dynamic shape factor, averaged over the total examined size range, agrees roughly with the coagulation shape factor. (Description of aerosol centrifuge and of differential mobility analyzer). (orig./HP) [de

Observation of carbonaceous aerosols and carbon monoxide in Mid-Atlantic region: Seasonal and inter-annual variations

Science.gov (United States)

Chen, L. A.; Doddridge, B. G.; Doddridge, B. G.; Dickerson, R. R.; Dickerson, R. R.

2001-05-01

As part of Maryland Aerosol Research and Characterization (MARCH-Atlantic) study, a long-term monitoring of ambient elemental and organic carbon (EC and OC) aerosols has been made at Fort Meade, MD (39.16° N 76.51° W; elevation 46 m MSL), a suburban site within the Baltimore-Washington (B-W) corridor, since July 1999. 24-hr average EC and OC are measured every day during the season-representative months (July 1999, October 1999, January 2000, April 2000 and July 2000). Carbon monoxide (CO) was also measured nearly continuously over the period. Strong correlation between EC and CO (r = 0.7 ~ 0.9) in every month suggests common or proximate sources, likely traffic emissions. The EC versus CO slope, however, varies in different seasons and is found to increase nonlinearly with the ambient temperature. EC source strength may peak in summer. OC shows strong correlation with EC (r ~ 0.95) only in winter, suggesting that OC is also of the same primary sources during wintertime. The Interagency Monitoring of Protected Visual Environments (IMPROVE) network has been measuring EC and OC around the United States since 1988. The FME data during July 1999 are also compared with simultaneous measurements at nearby IMPROVE sites, showing B-W corridor could be a major contributor to the carbonaceous aerosols in the Mid-Atlantic region. A decreasing trend of EC level is found in three IMPROVE sites in this region. This actually agrees with the decreasing trend of CO observed previously at Big Meadow, Shenandoah National Park if CO and EC are both influenced by traffic emissions.

Spatiotemporal variability and contribution of different aerosol types to the aerosol optical depth over the Eastern Mediterranean

Directory of Open Access Journals (Sweden)

A. K. Georgoulias

2016-11-01

Full Text Available This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the aerosol optical depth (AOD over the Eastern Mediterranean as derived from MODIS (Moderate Resolution Imaging Spectroradiometer Terra (March 2000–December 2012 and Aqua (July 2002–December 2012 satellite instruments. For this purpose, a 0.1° × 0.1° gridded MODIS dataset was compiled and validated against sun photometric observations from the AErosol RObotic NETwork (AERONET. The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium-sized cities, industrial zones and power plant complexes, seasonal variabilities and decadal averages. The average AOD at 550 nm (AOD550 for the entire region is ∼ 0.22 ± 0.19, with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in central and eastern Europe and transport of dust from the Sahara and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine-mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine-mode natural aerosols account for ∼ 51, ∼ 34 and ∼ 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account ∼ 40, ∼ 34

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.

Characterization of distinct Arctic aerosol accumulation modes and their sources

Science.gov (United States)

Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

2018-06-01

In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Science.gov (United States)

Ulevicius, Vidmantas; Byčenkienė, Steigvilė; Bozzetti, Carlo; Vlachou, Athanasia; Plauškaitė, Kristina; Mordas, Genrik; Dudoitis, Vadimas; Abbaszade, Gülcin; Remeikis, Vidmantas; Garbaras, Andrius; Masalaite, Agne; Blees, Jan; Fröhlich, Roman; Dällenbach, Kaspar R.; Canonaco, Francesco; Slowik, Jay G.; Dommen, Josef; Zimmermann, Ralf; Schnelle-Kreis, Jürgen; Salazar, Gary A.; Agrios, Konstantinos; Szidat, Sönke; El Haddad, Imad; Prévôt, André S. H.

2016-05-01

In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m-3 and black carbon (BC) up to 17 µg m-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26-44 % and 13-23 % to the total carbon (TC), respectively. 5-8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4-13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13-24 and 7-13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Source apportionment of submicron organic aerosol collected from Atlanta, Georgia, during 2014-2015 using the aerosol chemical speciation monitor (ACSM)

Science.gov (United States)

Rattanavaraha, Weruka; Canagaratna, Manjula R.; Budisulistiorini, Sri Hapsari; Croteau, Philip L.; Baumann, Karsten; Canonaco, Francesco; Prevot, Andre S. H.; Edgerton, Eric S.; Zhang, Zhenfa; Jayne, John T.; Worsnop, Douglas R.; Gold, Avram; Shaw, Stephanie L.; Surratt, Jason D.

2017-10-01

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was redeployed at the Jefferson Street (JST) site in downtown Atlanta, Georgia (GA) for 1 year (March 20, 2014-February 08, 2015) to chemically characterize non-refractory submicron particulate matter (NR-PM1) in near real-time and to assess whether organic aerosol (OA) types and amounts change from year-to-year. Submicron organic aerosol (OA) mass spectra were analyzed by season using multilinear engine (ME-2) to apportion OA subtypes to potential sources and chemical processes. A suite of real-time collocated measurements from the Southeastern Aerosol Research and Characterization (SEARCH) network was compared with ME-2 factor solutions to aid in the interpretation of OA subtypes during each season. OA tracers measured from high-volume filter samples using gas chromatography interfaced with electron ionization-mass spectrometry (GC/EI-MS) also aided in identifying OA sources. The initial application of ME-2 to the yearlong ACSM dataset revealed that OA source apportionment by season was required to better resolve sporadic OA types. Spring and fall OA mass spectral datasets were separated into finer periods to capture potential OA sources resulting from non-homogeneous emissions during transitioning periods. NR-PM1 was highest in summer (16.7 ± 8.4 μg m-3) and lowest in winter (8.0 ± 5.7 μg m-3), consistent with prior studies. OA dominated NR-PM1 mass (56-74% on average) in all seasons. Hydrocarbon-like OA (HOA) from primary emissions was observed in all seasons, averaging 5-22% of total OA mass. Strong correlations of HOA with carbon monoxide (CO) (R = 0.71-0.88) and oxides of nitrogen (NOx) (R = 0.55-0.79) indicated that vehicular traffic was the likely source. Biomass burning OA (BBOA) was observed in all seasons, with lower contributions (2%) in summer and higher in colder seasons (averaging 8-20% of total OA mass). BBOA correlated strongly with levoglucosan (R = 0.78-0.95) during colder seasons

An improved method for quantitatively measuring the sequences of total organic carbon and black carbon in marine sediment cores

Science.gov (United States)

Xu, Xiaoming; Zhu, Qing; Zhou, Qianzhi; Liu, Jinzhong; Yuan, Jianping; Wang, Jianghai

2018-01-01

Understanding global carbon cycle is critical to uncover the mechanisms of global warming and remediate its adverse effects on human activities. Organic carbon in marine sediments is an indispensable part of the global carbon reservoir in global carbon cycling. Evaluating such a reservoir calls for quantitative studies of marine carbon burial, which closely depend on quantifying total organic carbon and black carbon in marine sediment cores and subsequently on obtaining their high-resolution temporal sequences. However, the conventional methods for detecting the contents of total organic carbon or black carbon cannot resolve the following specific difficulties, i.e., (1) a very limited amount of each subsample versus the diverse analytical items, (2) a low and fluctuating recovery rate of total organic carbon or black carbon versus the reproducibility of carbon data, and (3) a large number of subsamples versus the rapid batch measurements. In this work, (i) adopting the customized disposable ceramic crucibles with the microporecontrolled ability, (ii) developing self-made or customized facilities for the procedures of acidification and chemothermal oxidization, and (iii) optimizing procedures and carbon-sulfur analyzer, we have built a novel Wang-Xu-Yuan method (the WXY method) for measuring the contents of total organic carbon or black carbon in marine sediment cores, which includes the procedures of pretreatment, weighing, acidification, chemothermal oxidation and quantification; and can fully meet the requirements of establishing their highresolution temporal sequences, whatever in the recovery, experimental efficiency, accuracy and reliability of the measurements, and homogeneity of samples. In particular, the usage of disposable ceramic crucibles leads to evidently simplify the experimental scenario, which further results in the very high recovery rates for total organic carbon and black carbon. This new technique may provide a significant support for

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

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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

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

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J. Wang

2016-07-01

Full Text Available In this work, the Aerodyne soot particle – aerosol mass spectrometer (SP-AMS was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD of China, for online characterization of the submicron aerosols (PM1. The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics. The average PM1 concentration was found to be 28.2 µg m−3, with organics (45 % as the most abundant component, following by sulfate (19.3 %, nitrate (13.6 %, ammonium (11.1 %, rBC (9.7 %, and chloride (1.3 %. These PM1 species together can reconstruct ∼ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA yielded four OA subcomponents, including hydrocarbon-like OA (HOA, cooking-related OA (COA, semi-volatile oxygenated OA (SV-OOA, and low-volatility oxygenated OA (LV-OOA. Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA dominated the total OA mass (55.5 %, but primary organic aerosol (POA, equal to the sum of HOA and COA can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand

Seasonal dependence of aerosol processing in urban Philadelphia

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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

TOMS/Earth-Probe Total Ozone Aerosol Index UV-Reflectivity UV-B Erythemal Irradiance Daily L3 Global 1x1.25 deg V008

Data.gov (United States)

National Aeronautics and Space Administration — The Total Ozone Mapping Spectrometer (TOMS) version 8 daily global gridded data consist of total column ozone, aerosol index, Lambertian effective surface...

Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

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L. Hildebrandt

2010-05-01

Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM₁, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM₁ sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM₁ such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×10¹¹ molecules cm⁻³ s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

Characteristics and sources of carbonaceous aerosols from Shanghai, China

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J.-J. Cao

2013-01-01

Full Text Available An intensive investigation of carbonaceous PM_2.5 and TSP (total suspended particles from Pudong (China was conducted as part of the MIRAGE-Shanghai (Megacities Impact on Regional and Global Environment experiment in 2009. Data for organic and elemental carbon (OC and EC, organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs, and stable carbon isotopes OC (δ¹³C_OC and EC (δ¹³C_EC were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA; high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ¹³C_OC = −24.5 ± 0.8‰ and δ¹³C_EC = −25.1 ± 0.6‰ indicated that fossil fuels were the most important source for carbonaceous PM_2.5 (particulate matter less than 2.5 micrometers in diameter, with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%; other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

The aerosol optical properties and PM2.5 components over the world's largest industrial zone in Tangshan, North China

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Zhang, Kequan; Ma, Yongjing; Xin, Jinyuan; Liu, Zirui; Ma, Yining; Gao, Dongdong; Wu, Junsong; Zhang, Wenyu; Wang, Yuesi; Shen, Pengke

2018-03-01

To achieve an in-depth understanding of the aerosol optical properties in the highly-industrial region of Tangshan, we provided systematic aerosol optical properties analysis in this largest industrial zone for the first time. The aerosol optical datasets (2013.05-2015.04) and chemical component data of PM2.5 (2014-2015) obtained from the Tangshan site of the campaign on atmospheric aerosol research (CARE-China) network were analyzed. The results showed that the Tangshan region was seriously affected by fine-mode industrial aerosols all year, which would promote the accumulation of pollutants and influence the atmospheric circulation through changing the vertical temperature gradient. The annual average aerosol optical depth (AOD) and Ångstrӧm exponent (α) were 0.80 ± 0.26 and 1.05 ± 0.10, respectively. The aerosol optical properties revealed significant seasonal characteristics. The maximum seasonal average AOD (1.03 ± 0.62) and α (1.12 ± 0.19) accompanied the highest seasonal secondary inorganic aerosol concentrations (SIA: SO42 -, NO3-, NH4+), 53.33 μg/m3, occurred in summer, and this phenomenon was attributed to the photochemical reactions favored by the high temperature and humidity. During the spring, frequent dust events led to the maximum Ca2 + concentration of 6.57 μg/m3 and the lowest seasonal α of 0.98 ± 0.31. Coal was used for generating heat in winter, resulting in the highest levels of pollutant emissions (Cl-, Elemental carbon (EC) and organic carbon (OC)). The aerosol type classifications showed that the industrial aerosols were the main controls in the summer and fall, representing 56%-58% of the total aerosols. While for spring and winter, mixed aerosols represented 53%-54% of the total aerosols. Hygroscopic growth effect of aerosols existed all year, which could enhance the negative radiative forcing and eventually cool the earth-atmosphere system. The classification Wing for Tangshan data showed high AOD values (> 0.70) were mainly

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

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Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

2016-07-01

In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The

Characterization of Black and Brown Carbon Concentrations and Sources during winter in Beijing

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Yan, Caiqing; Liu, Yue; Hansen, Anthony D. A.; Močnik, Griša; Zheng, Mei

2017-04-01

Carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), play important roles in air quality, human health, and climate change. A better understanding of sources of light-absorbing carbonaceous aerosol (including black carbon and brown carbon) is particular critical for formulating emission-based control strategies and reducing uncertainties in current aerosol radiative forcing estimates. Beijing, the capital of China, has experienced serious air pollution problems and high concentrations of carbonaceous aerosols in recent years, especially during heating seasons. During November and December of 2016, several severe haze episodes occurred in Beijing, with hourly average PM2.5 mass concentration up to 400 μg/m3. In this study, concentration levels and sources of black carbon and brown carbon were investigated based on 7-wavelength Aethalometer (AE-33) with combination of other PM2.5 chemical composition information. Contributions of traffic and non-traffic emissions (e.g., coal combustion, biomass burning) were apportioned, and brown carbon was separated from black carbon. Our preliminary results showed that (1) Concentrations of BC were around 5.3±4.2 μg/m3 during the study period, with distinct diurnal variations during haze and non-haze days. (2) Traffic emissions contributed to about 37±17% of total BC, and exhibited higher contributions during non-haze days compared to haze days. (3) Coal combustion was a major source of black carbon and brown carbon in Beijing, which was more significant compared to biomass burning. Sources and the relative contributions to black carbon and brown carbon during haze and non-haze days will be further discussed.

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

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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

Long-term (2001-2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

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Boreddy, Suresh K. R.; Mozammel Haque, M.; Kawamura, Kimitaka

2018-01-01

The present study reports on long-term trends of carbonaceous aerosols in total suspended particulate (TSP) samples collected at Chichijima in the western North Pacific during 2001-2012. Seasonal variations of elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) concentrations showed maxima in winter to spring and minima in summer. These seasonal differences in the concentrations of carbonaceous aerosols were associated with the outflows of polluted air masses from East Asia, which are clearly distinguishable from pristine air masses from the central Pacific. The higher concentrations of carbonaceous aerosols during winter to spring are associated with long-range atmospheric transport of East Asian continental polluted air masses, whereas lower concentrations may be due to pristine air masses from the central Pacific in summer. The annual trends of OC / EC (+0.46 % yr-1), WSOC (+0.18 % yr-1) and WSOC / OC (+0.08 % yr-1) showed significant (p Asia.

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

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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

Vertical profiles of aerosol and black carbon in the Arctic: a seasonal phenomenology along 2 years (2011–2012 of field campaigns

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L. Ferrero

2016-10-01

Full Text Available We present results from a systematic study of vertical profiles of aerosol number size distribution and black carbon (BC concentrations conducted in the Arctic, over Ny-Ålesund (Svalbard. The campaign lasted 2 years (2011–2012 and resulted in 200 vertical profiles measured by means of a tethered balloon (up to 1200 m a.g.l. during the spring and summer seasons. In addition, chemical analysis of filter samples, aerosol size distribution and a full set of meteorological parameters were determined at ground. The collected experimental data allowed a classification of the vertical profiles into different typologies, which allowed us to describe the seasonal phenomenology of vertical aerosol properties in the Arctic. During spring, four main types of profiles were found and their behavior was related to the main aerosol and atmospheric dynamics occurring at the measuring site. Background conditions generated homogenous profiles. Transport events caused an increase of aerosol concentration with altitude. High Arctic haze pollution trapped below thermal inversions promoted a decrease of aerosol concentration with altitude. Finally, ground-based plumes of locally formed secondary aerosol determined profiles with decreasing aerosol concentration located at different altitude as a function of size. During the summer season, the impact from shipping caused aerosol and BC pollution plumes to be constrained close to the ground, indicating that increasing shipping emissions in the Arctic could bring anthropogenic aerosol and BC in the Arctic summer, affecting the climate.

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

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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

TOMS/Nimbus-7 Total Ozone Aerosol Index UV-Reflectivity UV-B Erythemal Irradiances Daily L3 Global 1x1.25 deg V008

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National Aeronautics and Space Administration — The Total Ozone Mapping Spectrometer (TOMS) version 8 Daily Gridded Data consist of daily, global coverage of total column ozone, aerosol index, Lambertian effective...

Regional Responses to Black Carbon Aerosols: The Importance of Air-Sea Interaction

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Gnanadesikan, A.; Scott, A. A.; Pradal, M.-A.; Seviour, W. J. M.; Waugh, D. W.

2017-12-01

The impact of modern black carbon aerosols on climate via their changes in radiative balance is studied using a coupled model where sea surface temperatures (SSTs) are allowed to vary and an atmosphere-only version of the same model where SSTs are held fixed. Allowing the ocean to respond is shown to have a profound impact on the pattern of temperature change. Particularly, large impacts are found in the North Pacific (which cools by up to 1 K in the coupled model) and in north central Asia (which warms in the coupled simulation and cools in the fixed SST simulation). Neither set of experiments shows large changes in surface temperatures in the Southeast Asian region where the atmospheric burden of black carbon is highest. These results are related to the stabilization of the atmosphere and changes in oceanic heat transport. Over the North Pacific, atmospheric stabilization results in an increase in stratiform clouds. The resulting shading reduces evaporation, freshening the surface layer of the ocean and reducing the inflow of warm subtropical waters. Over the land, a delicate balance between greater atmospheric absorption, shading of the surface and changes in latent cooling of the surface helps to determine whether warming or cooling is seen. Our results emphasize the importance of coupling in determining the response of the climate system to black carbon and suggest that black carbon may play an important role in modulating climate change over the North Pacific.

Composition and sources of carbonaceous aerosols in Northern Europe during winter

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Glasius, M.; Hansen, A. M. K.; Claeys, M.; Henzing, J. S.; Jedynska, A. D.; Kasper-Giebl, A.; Kistler, M.; Kristensen, K.; Martinsson, J.; Maenhaut, W.; Nøjgaard, J. K.; Spindler, G.; Stenström, K. E.; Swietlicki, E.; Szidat, S.; Simpson, D.; Yttri, K. E.

2018-01-01

Sources of elemental carbon (EC) and organic carbon (OC) in atmospheric aerosols (carbonaceous aerosols) were investigated by collection of weekly aerosol filter samples at six background sites in Northern Europe (Birkenes, Norway; Vavihill, Sweden; Risoe, Denmark; Cabauw and Rotterdam in The Netherlands; Melpitz, Germany) during winter 2013. Analysis of 14C and a set of molecular tracers were used to constrain the sources of EC and OC. During the four-week campaign, most sites (in particular those in Germany and The Netherlands) were affected by an episode during the first two weeks with high concentrations of aerosol, as continental air masses were transported westward. The analysis results showed a clear, increasing north to south gradient for most molecular tracers. Total carbon (TC = OC + EC) at Birkenes showed an average concentration of 0.5 ± 0.3 μg C m-3, whereas the average concentration at Melpitz was 6.0 ± 4.3 μg C m-3. One weekly mean TC concentration as high as 11 μg C m-3 was observed at Melpitz. Average levoglucosan concentrations varied by an order of magnitude from 25 ± 13 ng m-3 (Birkenes) to 249 ± 13 ng m-3 (Melpitz), while concentrations of tracers of fungal spores (arabitol and mannitol) and vegetative debris (cellulose) were very low, showing a minor influence of primary biological aerosol particles during the North European winter. The fraction of modern carbon generally varied from 0.57 (Melpitz) to 0.91 (Birkenes), showing an opposite trend compared to the molecular tracers and TC. Total concentrations of 10 biogenic and anthropogenic carboxylic acids, mainly of secondary origin, were 4-53 ng m-3, with the lowest concentrations observed at Birkenes and the highest at Melpitz. However, the highest relative concentrations of carboxylic acids (normalized to TC) were observed at the most northern sites. Levels of organosulphates and nitrooxy organosulphates varied more than two orders of magnitude, from 2 to 414 ng m-3, between

Contribution of Seawater Surfactants to Generated Primary Marine Aerosol Particles

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Frossard, A. A.; Gerard, V.; Duplessis, P.; Kinsey, J. D.; Lu, X.; Zhu, Y.; Bisgrove, J.; Maben, J. R.; Long, M. S.; Chang, R.; Beaupre, S. R.; Kieber, D. J.; Keene, W. C.; Noziere, B.; Cohen, R. C.

2017-12-01

Surfactants account for minor fractions of total organic carbon in the ocean but may have major impacts on the surface tension of bursting bubbles at the sea surface that drive the production of primary marine aerosol particles (PMA). Surfactants associated with marine aerosol may also significantly reduce the surface tension of water thereby increasing the potential for cloud droplet activation and growth. During September and October 2016, PMA were produced from bursting bubbles in seawater using a high capacity generator at two biologically productive and two oligotrophic stations in the western North Atlantic, as part of a cruise on the R/V Endeavor. Surfactants were extracted from paired PMA and seawater samples, and their ionic compositions, total concentrations, and critical micelle concentrations (CMC) were quantified and compared for the four hydrographic stations. Higher surfactant concentrations were determined in the aerosol produced from biologically productive seawater compared to oligotrophic seawater, and the surfactants extracted from productive seawater were stronger (had lower CMCs) than those in the oligotrophic seawater. Surfactants associated with PMA and seawater in productive regions also varied over diel cycles, whereas those in the oligotrophic regions did not. This work demonstrates a direct link between surfactants in seawater and those in PMA.

Carbonaceous Aerosol Characterization during 2016 KOR-US 2016

Science.gov (United States)

Rodriguez, B.; Santos, G. M.; Sanchez, D.; Jeong, D.; Czimczik, C. I.; Kim, S.

2017-12-01

Atmospheric carbonaceous aerosols are a major component of fine particulate matter and assume important roles in Earth's climate and human health. Because atmospheric carbonaceous aerosols exist as a continuum ranging from small, light-scattering organic carbon (OC), to highly-condensed, light-absorbing elemental carbon (EC) they have contrasting effects on interaction with incoming and outgoing radiation, cloud formation, and snow/ice albedo. By strengthening our understanding of the relative contribution and sources of OC and EC we will be able to further describe aerosol formation and mixing at the regional level. To understand the relative anthropogenic and biogenic contributions to carbonaceous aerosol, 12 PM10 aerosols samples were collected on quartz fiber filters at the Mt. Taewha Research Forest in South Korea during the KORUS-AQ 2016 campaign over periods of 24-48 hours with a high-volume air sampler. Analysis of bulk C and N concentrations and absorption properties of filter extracts interspersed with HYSPLIT model results indicated that continental outflow across the Yellow Sea in enriched in bulk nitrogen loading and enhanced bulk absorptive properties of the aerosols. Bulk radiocarbon analysis also indicated enriched values in all samples indicating contamination from a nuclear power plant or the combustion of biomedical waste nearby. Here, we aim to investigate further the chemical characterization of VOCs adsorbed unto the aerosol through TD-GC-TOFMS. With this dataset we aim to determine the relative contribution of anthropogenic and biogenic aerosols by utilizing specific chemical tracers for source apportionment.

Stratospheric aerosols

International Nuclear Information System (INIS)

Rosen, J.; Ivanov, V.A.

1993-01-01

Stratospheric aerosol measurements can provide both spatial and temporal data of sufficient resolution to be of use in climate models. Relatively recent results from a wide range of instrument techniques for measuring stratospheric aerosol parameters are described. Such techniques include impactor sampling, lidar system sensing, filter sampling, photoelectric particle counting, satellite extinction-sensing using the sun as a source, and optical depth probing, at sites mainly removed from tropospheric aerosol sources. Some of these techniques have also had correlative and intercomparison studies. The main methods for determining the vertical profiles of stratospheric aerosols are outlined: lidar extinction measurements from satellites; impactor measurements from balloons and aircraft; and photoelectric particle counter measurements from balloons, aircraft, and rockets. The conversion of the lidar backscatter to stratospheric aerosol mass loading is referred to. Absolute measurements of total solar extinction from satellite orbits can be used to extract the aerosol extinction, and several examples of vertical profiles of extinction obtained with the SAGE satellite are given. Stratospheric mass loading can be inferred from extinction using approximate linear relationships but under restrictive conditions. Impactor sampling is essentially the only method in which the physical nature of the stratospheric aerosol is observed visually. Vertical profiles of stratospheric aerosol number concentration using impactor data are presented. Typical profiles using a dual-size-range photoelectric dustsonde particle counter are given for volcanically disturbed and inactive periods. Some measurements of the global distribution of stratospheric aerosols are also presented. Volatility measurements are described, indicating that stratospheric aerosols are composed primarily of about 75% sulfuric acid and 25% water

Characterization of atmospheric aerosol in Buenos Aires, Argentina

International Nuclear Information System (INIS)

Jasan, R.C.; Pla, R.R.; Invernizzi, R.; Dos Santos, M.

2009-01-01

PM10 and PM2.5 samples were taken using a Gent sampler to characterize the atmospheric aerosol of Buenos Aires metropolitan area. A total of 114 samples were collected from October 2005 to October 2006 at one urban site, every third day, for 24 h. Samples were analyzed by neutron activation, and black carbon and mass concentration were determined. In both fractions, elemental and gravimetric mass concentrations were compared with historical data. Enrichment factors, backward trajectories and factor analysis were calculated. The attribution of pollution sources is discussed. (author)

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

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

Science.gov (United States)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Directory of Open Access Journals (Sweden)

V. Ulevicius

2016-05-01

Full Text Available In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1 was measured by an Aerodyne aerosol chemical speciation monitor (ACSM and a source apportionment with the multilinear engine (ME-2 running the positive matrix factorization (PMF model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m−3 and black carbon (BC up to 17 µg m−3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C measurements of the elemental (EC and organic (OC carbon fractions. Non-fossil organic carbon (OCnf was the dominant fraction of PM1, with the primary (POCnf and secondary (SOCnf fractions contributing 26–44 % and 13–23 % to the total carbon (TC, respectively. 5–8 % of the TC had a primary fossil origin (POCf, whereas the contribution of fossil secondary organic carbon (SOCf was 4–13 %. Non-fossil EC (ECnf and fossil EC (ECf ranged from 13–24 and 7–13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Nitrate radical oxidation of γ-terpinene: hydroxy nitrate, total organic nitrate, and secondary organic aerosol yields

Science.gov (United States)

Slade, Jonathan H.; de Perre, Chloé; Lee, Linda; Shepson, Paul B.

2017-07-01

Polyolefinic monoterpenes represent a potentially important but understudied source of organic nitrates (ONs) and secondary organic aerosol (SOA) following oxidation due to their high reactivity and propensity for multi-stage chemistry. Recent modeling work suggests that the oxidation of polyolefinic γ-terpinene can be the dominant source of nighttime ON in a mixed forest environment. However, the ON yields, aerosol partitioning behavior, and SOA yields from γ-terpinene oxidation by the nitrate radical (NO3), an important nighttime oxidant, have not been determined experimentally. In this work, we present a comprehensive experimental investigation of the total (gas + particle) ON, hydroxy nitrate, and SOA yields following γ-terpinene oxidation by NO3. Under dry conditions, the hydroxy nitrate yield = 4(+1/-3) %, total ON yield = 14(+3/-2) %, and SOA yield ≤ 10 % under atmospherically relevant particle mass loadings, similar to those for α-pinene + NO3. Using a chemical box model, we show that the measured concentrations of NO2 and γ-terpinene hydroxy nitrates can be reliably simulated from α-pinene + NO3 chemistry. This suggests that NO3 addition to either of the two internal double bonds of γ-terpinene primarily decomposes forming a relatively volatile keto-aldehyde, reconciling the small SOA yield observed here and for other internal olefinic terpenes. Based on aerosol partitioning analysis and identification of speciated particle-phase ON applying high-resolution liquid chromatography-mass spectrometry, we estimate that a significant fraction of the particle-phase ON has the hydroxy nitrate moiety. This work greatly contributes to our understanding of ON and SOA formation from polyolefin monoterpene oxidation, which could be important in the northern continental US and the Midwest, where polyolefinic monoterpene emissions are greatest.

Evaluating Carbonate System Algorithms in a Nearshore System: Does Total Alkalinity Matter?

Science.gov (United States)

Jones, Jonathan M; Sweet, Julia; Brzezinski, Mark A; McNair, Heather M; Passow, Uta

2016-01-01

Ocean acidification is a threat to many marine organisms, especially those that use calcium carbonate to form their shells and skeletons. The ability to accurately measure the carbonate system is the first step in characterizing the drivers behind this threat. Due to logistical realities, regular carbonate system sampling is not possible in many nearshore ocean habitats, particularly in remote, difficult-to-access locations. The ability to autonomously measure the carbonate system in situ relieves many of the logistical challenges; however, it is not always possible to measure the two required carbonate parameters autonomously. Observed relationships between sea surface salinity and total alkalinity can frequently provide a second carbonate parameter thus allowing for the calculation of the entire carbonate system. Here, we assessed the rigor of estimating total alkalinity from salinity at a depth sampling water from a pier in southern California for several carbonate system parameters. Carbonate system parameters based on measured values were compared with those based on estimated TA values. Total alkalinity was not predictable from salinity or from a combination of salinity and temperature at this site. However, dissolved inorganic carbon and the calcium carbonate saturation state of these nearshore surface waters could both be estimated within on average 5% of measured values using measured pH and salinity-derived or regionally averaged total alkalinity. Thus we find that the autonomous measurement of pH and salinity can be used to monitor trends in coastal changes in DIC and saturation state and be a useful method for high-frequency, long-term monitoring of ocean acidification.

Ambient Observations of Aerosols, Novel Aerosol Structures, And Their Engineering Applications

Science.gov (United States)

Beres, Nicholas D.

The role of atmospheric aerosols remains a crucial issue in understanding and mitigating climate change in our world today. These particles influence the Earth by altering the Earth's delicate radiation balance, human health, and visibility. In particular, black carbon particulate matter remains the key driver in positive radiative forcing (i.e., warming) due to aerosols. Produced from the incomplete combustion of hydrocarbons, these compounds can be found in many different forms around the globe. This thesis provides an overview of three research topics: (1) the ambient characterization of aerosols in the Northern Indian Ocean, measurement techniques used, and how these aerosols influence local, regional, and global climate; (2) the exploration of novel soot superaggregate particles collected in the Northern Indian Ocean and around the globe and how the properties of these particles relate to human health and climate forcing; and (3) how aerogelated soot can be produced in a novel, one-step method utilizing an inverted flame reactor and how this material could be used in industrial settings.

Aerosol effects on UV radiation

International Nuclear Information System (INIS)

Koepke, P.; Reuder, J.; Schwander, H.

2000-01-01

The reduction of erythemally weighted UV-irradiance (given as UV index, UVI) due to aerosols is analyzed by variation of the tropospheric particles in a wide, but realistic range. Varied are amount and composition of the particles and relative humidity and thickness of the mixing layer. The reduction of UVI increases with aerosol optical depth and the UV change is around 10% for a change aerosol optical depth from 0.25 to 0.1 and 0.4 respectively. Since both aerosol absorption and scattering are of relevance, the aerosol effect depends besides total aerosol amount on relative amount of soot and on relative humidity

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

(>75%. The correlation between OA and an anthropogenic tracer does not necessarily identify the source of the carbon as being anthropogenic but instead suggests a coupling between the anthropogenic and biogenic components in the air mass that might be related to the source of the oxidant and/or the aerosol sulfate. Observations of organosulfates of isoprene and α-pinene provided evidence for the likely importance of aerosol sulfate in spite of neutralized aerosol although acidic plumes might have played a role upwind of the site. This is in contrast to laboratory studies where strongly acidic seed aerosols were needed in order to form these compounds. These compounds together represented only a minor fraction (<1% of the total OA mass, which may be the result of the neutralized aerosol at the site or because only a small number of organosulfates were quantified. The low contribution of organosulfates to total OA suggests that other mechanisms, e.g. NO_x enhancement of oxidant levels, are likely responsible for the majority of the anthropogenic enhancement of biogenic secondary organic aerosol observed at this site.

Onshore Wind Speed Modulates Microbial Aerosols along an Urban Waterfront

Directory of Open Access Journals (Sweden)

M. Elias Dueker

2017-11-01

Full Text Available Wind blowing over aquatic and terrestrial surfaces produces aerosols, which include microbial aerosols. We studied the effect of onshore wind speeds on aerosol concentrations as well as total and culturable microbial aerosols (bacterial and viral at an urban waterfront (New York, NY, United States of America. We used two distinct methods to characterize microbial aerosol responses to wind speed: A culture-based exposure-plate method measuring viable bacterial deposition near-shore (CFU accumulation rate; and a culture-independent aerosol sampler-based method measuring total bacterial and viral aerosols (cells m−3 air. While ambient coarse (>2 µm and fine (0.3–2 µm aerosol particle number concentrations (regulated indicators of air quality decreased with increasing onshore wind speeds, total and depositing culturable bacterial aerosols and total viral aerosols increased. Taxonomic identification of the 16S rDNA of bacterial aerosol isolates suggested both terrestrial and aquatic sources. Wind appears to increase microbial aerosol number concentrations in the near-shore environment by onshore transport at low wind speeds (<4 m s−1, and increased local production and transport of new microbial aerosols from adjacent water surfaces at higher wind speeds (>4 m s−1. This study demonstrates a wind-modulated microbial connection between water and air in the coastal urban environment, with implications for public health management and urban microbial ecology.

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.

Modeling ozone and aerosol formation and transport in the pacific northwest with the community Multi-Scale Air Quality (CMAQ) modeling system.

Science.gov (United States)

O'Neill, Susan M; Lamb, Brian K; Chen, Jack; Claiborn, Candis; Finn, Dennis; Otterson, Sally; Figueroa, Cristiana; Bowman, Clint; Boyer, Mike; Wilson, Rob; Arnold, Jeff; Aalbers, Steven; Stocum, Jeffrey; Swab, Christopher; Stoll, Matt; Dubois, Mike; Anderson, Mary

2006-02-15

The Community Multi-Scale Air Quality (CMAQ) modeling system was used to investigate ozone and aerosol concentrations in the Pacific Northwest (PNW) during hot summertime conditions during July 1-15, 1996. Two emission inventories (El) were developed: emissions for the first El were based upon the National Emission Trend 1996 (NET96) database and the BEIS2 biogenic emission model, and emissions for the second El were developed through a "bottom up" approach that included biogenic emissions obtained from the GLOBEIS model. The two simulations showed that elevated PM2.5 concentrations occurred near and downwind of the Interstate-5 corridor along the foothills of the Cascade Mountains and in forested areas of central Idaho. The relative contributions of organic and inorganic aerosols varied by region, but generally organic aerosols constituted the largest fraction of PM2.5. In wilderness areas near the 1-5 corridor, organic carbon from anthropogenic sources contributed approximately 50% of the total organic carbon with the remainder from biogenic precursors, while in wilderness areas in Idaho, biogenic organic carbon accounted for 80% of the total organic aerosol. Regional analysis of the secondary organic aerosol formation in the Columbia River Gorge, Central Idaho, and the Olympics/Puget Sound showed that the production rate of secondary organic carbon depends on local terpene concentrations and the local oxidizing capacity of the atmosphere, which was strongly influenced by anthropogenic emissions. Comparison with observations from 12 IMPROVE sites and 21 ozone monitoring sites showed that results from the two El simulations generally bracketed the average observed PM parameters and that errors calculated for the model results were within acceptable bounds. Analysis across all statistical parameters indicated that the NW-AIRQUEST El solution performed better at predicting PM2.5, PM1, and beta(ext) even though organic carbon PM was over-predicted, and the NET96 El

Warming-induced increase in aerosol number concentration likely to moderate climate change

NARCIS (Netherlands)

Paasonen, P.; Asmi, A.; Petäjä, T.; Kajos, M.K.; Äijälä, M.; Junninen, H.; Holst, T.; Abbatt, J.P.D.; Arneth, A.; Birmili, W.; Denier van der Gon, H.A.C.; Hamed, A.; Hoffer, A.; Laakso, L.; Laaksonen, A.; Richard Leaitch, W.; Plass-Dülmer, C.; Pryor, S.C.; Räisänen, P.; Swietlicki, E.; Wiedensohler, A.; Worsnop, D.R.; Kerminen, V.-M.; Kulmala, M.

2013-01-01

Atmospheric aerosol particles influence the climate system directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. Apart from black carbon aerosol, aerosols cause a negative radiative forcing at the top of the atmosphere and substantially mitigate

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

GRIP LANGLEY AEROSOL RESEARCH GROUP EXPERIMENT (LARGE) V1

Data.gov (United States)

National Aeronautics and Space Administration — Langley Aerosol Research Group Experiment (LARGE) measures ultrafine aerosol number density, total and non-volatile aerosol number density, dry aerosol size...

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.

UV-Vis-IR spectral complex refractive indices and optical properties of brown carbon aerosol from biomass burning

Science.gov (United States)

Sumlin, Benjamin J.; Heinson, Yuli W.; Shetty, Nishit; Pandey, Apoorva; Pattison, Robert S.; Baker, Stephen; Hao, Wei Min; Chakrabarty, Rajan K.

2018-02-01

Constraining the complex refractive indices, optical properties and size of brown carbon (BrC) aerosols is a vital endeavor for improving climate models and satellite retrieval algorithms. Smoldering wildfires are the largest source of primary BrC, and fuel parameters such as moisture content, source depth, geographic origin, and fuel packing density could influence the properties of the emitted aerosol. We measured in situ spectral (375-1047 nm) optical properties of BrC aerosols emitted from smoldering combustion of Boreal and Indonesian peatlands across a range of these fuel parameters. Inverse Lorenz-Mie algorithms used these optical measurements along with simultaneously measured particle size distributions to retrieve the aerosol complex refractive indices (m = n + iκ). Our results show that the real part n is constrained between 1.5 and 1.7 with no obvious functionality in wavelength (λ), moisture content, source depth, or geographic origin. With increasing λ from 375 to 532 nm, κ decreased from 0.014 to 0.003, with corresponding increase in single scattering albedo (SSA) from 0.93 to 0.99. The spectral variability of κ follows the Kramers-Kronig dispersion relation for a damped harmonic oscillator. For λ ≥ 532 nm, both κ and SSA showed no spectral dependency. We discuss differences between this study and previous work. The imaginary part κ was sensitive to changes in FPD, and we hypothesize mechanisms that might help explain this observation.

Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Lin, Peng; Aiona, Paige K.; Li, Ying; Shiraiwa, Manabu; Laskin, Julia; Nizkorodov, Sergey A.; Laskin, Alexander

2016-11-01

Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly-emitted biomass burning organic aerosol (BBOA) samples collected during test burns of selected biomass fuels: sawgrass, peat, ponderosa pine, and black spruce. We characterize individual BrC chromophores present in these samples using high performance liquid chromatography coupled to a photodiode array detector and a high-resolution mass spectrometer. We demonstrate that both the overall BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels and burning conditions. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as potential markers of BrC originating from different biomass burning sources. On average, ~50% of the light absorption above 300 nm can be attributed to a limited number of strong BrC chromophores, which may serve as representative light-absorbing species for studying atmospheric processing of BrC aerosol. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of 16 hours. A “molecular corridors” analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low volatility (<1 g m-1) and will be retained in the particle phase under atmospherically relevant conditions.

Spectroscopic study of the water-soluble organic matter isolated from atmospheric aerosols collected under different atmospheric conditions

International Nuclear Information System (INIS)

Duarte, Regina M.B.O.; Pio, Casimiro A.; Duarte, Armando C.

2005-01-01

The composition of the water-soluble organic matter from fine aerosols collected in a rural location during two different meteorological conditions (summer and autumn) was investigated by UV-vis, synchronous fluorescence (with Δλ = 20 nm), FT-IR and CPMAS- 13 C NMR spectroscopies. A seasonal variation in the concentration of total carbon, organic carbon and water-soluble organic carbon was confirmed, with higher values during the autumn and lower values during the summer season. The chemical characterisation of the water-soluble organic matter showed that both samples are dominated by a high content of aliphatic structures, carboxyl groups and aliphatic carbons single bonded to one oxygen or nitrogen atom. However, the autumn sample exhibits a higher aromatic content than the summer sample, plus signals due to carbons of phenol, ketones and methoxyl groups. These signals were attributed to lignin breakdown products which are likely to be released during wood combustion processes. The obtained results put into evidence the major contribution of biomass burning processes in domestic fireplaces during low temperature conditions into both the concentration and the bulk chemical properties of the WSOC from fine aerosols

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.

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential

Origin and radiative forcing of black carbon aerosol: production and consumption perspectives.

Science.gov (United States)

Meng, Jing; Liu, Junfeng; Yi, Kan; Yang, Haozhe; Guan, Dabo; Liu, Zhu; Zhang, Jiachen; Ou, Jiamin; Dorling, Stephen; Mi, Zhifu; Shen, Huizhong; Zhong, Qirui; Tao, Shu

2018-04-24

Air pollution, a threat to air quality and human health, has attracted ever-increasing attention in recent years. In addition to having local influence, air pollutants can also travel the globe via atmospheric circulation and international trade. Black carbon (BC), emitted from incomplete combustion, is a unique but representative particulate pollutant. This study tracked down the BC aerosol and its direct radiative forcing to the emission sources and final consumers using the global chemical transport model (MOZART-4), the rapid radiative transfer model for general circulation simulations (RRTM) and a multiregional input-output analysis (MRIO). BC is physically transported (i.e., atmospheric transport) from western to eastern countries in the mid-latitude westerlies, but its magnitude is near an order of magnitude higher if the virtual flow embodied in international trade is considered. The transboundary effects on East and South Asia by other regions increased from about 3% (physical transport only) to 10% when considering both physical and virtual transport. The influence efficiency on East Asia is also large because of the comparatively large emission intensity and emission-intensive exports (e.g., machinery and equipment). The radiative forcing in Africa imposed by consumption from Europe, North America and East Asia (0.01Wm-2) was even larger than the total forcing in North America. Understanding the supply chain and incorporating both atmospheric and virtual transport may improve multilateral cooperation on air pollutant mitigation both domestically and internationally.

Influence of sample composition on aerosol organic and black carbon determinations

Energy Technology Data Exchange (ETDEWEB)

Novakov, T.; Corrigan, C.E.

1995-07-01

In this paper we present results on characterization of filter-collected redwood (Sequoia sempevirens)-needle and eucalyptus smoke particles by thermal, optical, and solvent extraction methods. Our results demonstrate that organic and black carbon concentrations determined by thermal and optical methods are not only method dependent, but also critically influenced by the overall chemical composition of the samples. These conclusions are supported by the following: (1) the organic fraction of biomass smoke particles analyzed includes a component, ranging in concentration from about 6-20% of total carbon or from 16-30% of organic carbon, that is relatively non-volatile and has a combustion temperature close to that of black carbon; (2) presence of K or Na in biomass smoke samples lowers the combustion temperatures of this organic component and of black carbon, making their combustion properties indistinguishable; (3) about 20% of total organic material is nonvolatile when heated to 550{degrees}C in an inert atmosphere. Consequently, thermal methods that rely on a specific temperature to separate organic from black carbon may either underestimate or overestimate the black and organic carbon concentrations, depending on the amounts of Na and K and on the composition and concentration of organic material present in a sample. These analytical uncertainties and, under some conditions, absorption by organic material may contribute to the variability of empirically derived proportionality between light transmission through filter deposits and black carbon concentrations.

Influence of sample composition on aerosol organic and black carbon determinations

International Nuclear Information System (INIS)

Novakov, T.; Corrigan, C.E.

1995-07-01

In this paper we present results on characterization of filter-collected redwood (Sequoia sempevirens)-needle and eucalyptus smoke particles by thermal, optical, and solvent extraction methods. Our results demonstrate that organic and black carbon concentrations determined by thermal and optical methods are not only method dependent, but also critically influenced by the overall chemical composition of the samples. These conclusions are supported by the following: (1) the organic fraction of biomass smoke particles analyzed includes a component, ranging in concentration from about 6-20% of total carbon or from 16-30% of organic carbon, that is relatively non-volatile and has a combustion temperature close to that of black carbon; (2) presence of K or Na in biomass smoke samples lowers the combustion temperatures of this organic component and of black carbon, making their combustion properties indistinguishable; (3) about 20% of total organic material is nonvolatile when heated to 550 degrees C in an inert atmosphere. Consequently, thermal methods that rely on a specific temperature to separate organic from black carbon may either underestimate or overestimate the black and organic carbon concentrations, depending on the amounts of Na and K and on the composition and concentration of organic material present in a sample. These analytical uncertainties and, under some conditions, absorption by organic material may contribute to the variability of empirically derived proportionality between light transmission through filter deposits and black carbon concentrations

Mexico city aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0 – Part 2: Analysis of the biomass burning contribution and the non-fossil carbon fraction

Directory of Open Access Journals (Sweden)

A. C. Aiken

2010-06-01

does not show an increase during the fire periods or a correlation with fire counts, FLEXPART-predicted FIFs or fire tracers, indicating that it is dominated by urban and/or regional sources and not by the fires near the MCMA.

A new ¹⁴C aerosol dataset is presented. Both this new and a previously published dataset of ¹⁴C analysis suggest a similar BBOA contribution as the AMS and chemical mass balance (CMB, resulting in 13% higher non-fossil carbon during the high vs. low regional fire periods. The new dataset has ~15% more fossil carbon on average than the previously published one, and possible reasons for this discrepancy are discussed. During the low regional fire period, 38% of organic carbon (OC and 28% total carbon (TC are from non-fossil sources, suggesting the importance of urban and regional non-fossil carbon sources other than the fires, such as food cooking and regional biogenic SOA. The ambient BBOA/ΔCH₃CN ratio is much higher in the afternoon when the wildfires are most intense than during the rest of the day. Also, there are large differences in the contributions of the different OA components to the surface concentrations vs. the integrated column amounts. Both facts may explain some apparent disagreements between BB impacts estimated from afternoon aircraft flights vs. those from 24-h ground measurements.

We show that by properly accounting for the non-BB sources of K, all of the BB PM estimates from MILAGRO can be reconciled. Overall, the fires from the region near the MCMA are estimated to contribute 15–23% of the OA and 7–9% of the fine PM at T0 during MILAGRO, and 2–3% of the fine PM as an annual average. The 2006 MCMA emissions inventory contains a substantially lower impact of the forest fire emissions, although a fraction of these emissions occur just outside of the MCMA inventory area.

Carbon pool densities and a first estimate of the total carbon pool in the Mongolian forest-steppe.

Science.gov (United States)

Dulamsuren, Choimaa; Klinge, Michael; Degener, Jan; Khishigjargal, Mookhor; Chenlemuge, Tselmeg; Bat-Enerel, Banzragch; Yeruult, Yolk; Saindovdon, Davaadorj; Ganbaatar, Kherlenchimeg; Tsogtbaatar, Jamsran; Leuschner, Christoph; Hauck, Markus

2016-02-01

The boreal forest biome represents one of the most important terrestrial carbon stores, which gave reason to intensive research on carbon stock densities. However, such an analysis does not yet exist for the southernmost Eurosiberian boreal forests in Inner Asia. Most of these forests are located in the Mongolian forest-steppe, which is largely dominated by Larix sibirica. We quantified the carbon stock density and total carbon pool of Mongolia's boreal forests and adjacent grasslands and draw conclusions on possible future change. Mean aboveground carbon stock density in the interior of L. sibirica forests was 66 Mg C ha(-1) , which is in the upper range of values reported from boreal forests and probably due to the comparably long growing season. The density of soil organic carbon (SOC, 108 Mg C ha(-1) ) and total belowground carbon density (149 Mg C ha(-1) ) are at the lower end of the range known from boreal forests, which might be the result of higher soil temperatures and a thinner permafrost layer than in the central and northern boreal forest belt. Land use effects are especially relevant at forest edges, where mean carbon stock density was 188 Mg C ha(-1) , compared with 215 Mg C ha(-1) in the forest interior. Carbon stock density in grasslands was 144 Mg C ha(-1) . Analysis of satellite imagery of the highly fragmented forest area in the forest-steppe zone showed that Mongolia's total boreal forest area is currently 73 818 km(2) , and 22% of this area refers to forest edges (defined as the first 30 m from the edge). The total forest carbon pool of Mongolia was estimated at ~ 1.5-1.7 Pg C, a value which is likely to decrease in future with increasing deforestation and fire frequency, and global warming. © 2015 John Wiley & Sons Ltd.

Supercritical Water Oxidation Total Organic Carbon (TOC) Analysis

Science.gov (United States)

The work presented here is the evaluation of the modified wet‐oxidation method described as Supercritical Water Oxidation (SCWO) for the analysis of total organic carbon (TOC) in very difficult oil/gas produced water sample matrices.

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

Stable carbon isotopic compositions of low-molecular-weight dicarboxylic acids, glyoxylic acid and glyoxal in tropical aerosols: implications for photochemical processes of organic aerosols

Directory of Open Access Journals (Sweden)

Stelyus L. Mkoma

2014-10-01

Full Text Available Tropical aerosols of PM2.5 and PM10 were collected at a rural site in Morogoro, Tanzania (East Africa, and analysed for stable carbon isotopic composition (δ13C of dicarboxylic acids (C2–C9, glyoxylic acid (ωC2 and glyoxal (Gly using gas chromatography/isotope ratio mass spectrometer. PM2.5 samples showed that δ13C of oxalic (C2 acid are largest (mean, −18.3±1.7‰ followed by malonic (C3, −19.6±1.0‰ and succinic (C4, −21.8±2.2‰ acids, whereas those in PM10 are a little smaller: −19.9±3.1‰ (C2, −20.2±2.7‰ (C3 and −23.3±3.2‰ (C4. The δ13C of C2–C4 diacids showed a decreasing trend with an increase in carbon numbers. The higher δ13C values of oxalic acid can be explained by isotopic enrichment of 13C in the remaining C2 due to the atmospheric decomposition of oxalic acid or its precursors. δ13C of ωC2 and Gly that are precursors of oxalic acid also showed larger values (mean, −22.5‰ and −20.2‰, respectively in PM2.5 than those (−26.7‰ and −23.7‰ in PM10. The δ13C values of ωC2 and Gly are smaller than those of C2 in both PM2.5 and PM10. On the other hand, azelaic acid (C9; mean, −28.5‰ is more depleted in 13C, which is consistent with the previous knowledge; that is, C9 is produced by the oxidation of unsaturated fatty acids emitted from terrestrial higher plants. A significant enrichment of 13C in oxalic acid together with its negative correlations with relative abundance of C2 in total diacids and ratios of water-soluble organic carbon and organic carbon further support that a photochemical degradation of oxalic acid occurs during long-range transport from source regions.

An advanced technique for speciation of organic nitrogen in atmospheric aerosols

Science.gov (United States)

Samy, S.; Robinson, J.; Hays, M. D.

2011-12-01

The chemical composition of organic nitrogen (ON) in the environment is a research topic of broad significance. The topic intersects the branches of atmospheric, aquatic, and ecological science; thus, a variety of instrumentation, analytical methods, and data interpretation tools have evolved for determination of ON. Recent studies that focus on atmospheric particulate nitrogen (N) suggest a significant fraction (20-80%) of total N is bound in organic compounds. The sources, bioavailability and transport mechanisms of these N-containing compounds can differ, producing a variety of environmental consequences. Amino acids (AA) are a key class of atmospheric ON compounds that can contribute to secondary organic aerosol (SOA) formation and potentially influence water cycles, air pollutant scavenging, and the radiation balance. AA are water-soluble organic compounds (WSOC) that can significantly alter the acid-base chemistry of aerosols, and may explain the buffering capacity that impacts heterogeneous atmospheric chemistry. The chemical transformations that N-containing organic compounds (including AA) undergo can increase the light-absorbing capacity of atmospheric carbon via formation of 'brown carbon'. Suggested sources of atmospheric AA include: marine surface layer transport from bursting sea bubbles, the suspension of bacteria, fungi, algae, pollen, spores, or biomass burning. Methodology for detection of native (underivatized) amino acids (AA) in atmospheric aerosols has been developed and validated (Samy et al., 2011). This presentation describes the use of LC-MS (Q-TOF) and microwave-assisted gas phase hydrolysis for detection of free and combined amino acids in aerosols collected in a Southeastern U.S. forest environment. Accurate mass detection and the addition of isotopically labeled surrogates prior to sample preparation allows for sensitive quantitation of target AA in a complex aerosol matrix. A total of 16 native AA were detected above the reporting

Measurements and Analysis of Black Carbon Aerosols in the Eastern Mediterranean Megacity

Science.gov (United States)

Unal, A.; Ozdemir, H.; Kindap, T.; Demir, G.; Karaca, M.; Khan, M. N.

2010-12-01

In a world where at least 50 percent of the population is living in urban environments, air pollution and specifically particulate matter became one of the most critical issues. There have been many studies that focused on mass concentration measurements of PM10 and PM2.5. Recent studies suggest that chemical composition is critical in understanding the effects of PM on health as well as climate. For example, public health studies reveal that, components of the atmospheric aerosols have different impacts on human health. Smith et al. (2009) stated that; on the basis of the 1μg/m3 contrast, the percentage increase in all-cause mortality for PM2.5 was 0.58; sulfate effects were about twice those of PM2.5, and effects of elemental carbon (an indicator of black carbon mass) about ten times greater. To date, many studies and national inventories have been based on particulate matter (PM10 and PM2.5), and the major greenhouse pollutants, but not speciated emissions, especially in the developing world (Smith et al., 2009; Chow et al., 2010). But air quality standards will soon need to include particulate black carbon (BC), as it directly afffects climate, visibility, and human health. Anthropogenic emissions are increasing dramatically worldwide and recent estimates of global BC emissions range from 8 to 24 Tg (1012 g) per year. In this study, we investigated BC pollution for the first time in Istanbul, Turkey. Istanbul is a megacity of over 15 million inhabitants (OECD, 2008). On-road traffic is also increasing rapidly in the city (over 3 million vehicles on the road). Hence, the city has a potential to be an important source for both local and regional pollution in the Eastern Mediterranean. In our study, an Aethalometer (<0.1μg/m3 sensitivity) was used for continuous and real-time measurements of BC concentration. Measurements were carried out at the selected five different locations throughout the city. 1st and 2nd sites were near high-traffic streets; in the city

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

1.5 °C carbon budget dependent on carbon cycle uncertainty and future non-CO2 forcing.

Science.gov (United States)

Mengis, Nadine; Partanen, Antti-Ilari; Jalbert, Jonathan; Matthews, H Damon

2018-04-11

Estimates of the 1.5 °C carbon budget vary widely among recent studies, emphasizing the need to better understand and quantify key sources of uncertainty. Here we quantify the impact of carbon cycle uncertainty and non-CO 2 forcing on the 1.5 °C carbon budget in the context of a prescribed 1.5 °C temperature stabilization scenario. We use Bayes theorem to weight members of a perturbed parameter ensemble with varying land and ocean carbon uptake, to derive an estimate for the fossil fuel (FF) carbon budget of 469 PgC since 1850, with a 95% likelihood range of (411,528) PgC. CO 2 emissions from land-use change (LUC) add about 230 PgC. Our best estimate of the total (FF + LUC) carbon budget for 1.5 °C is therefore 699 PgC, which corresponds to about 11 years of current emissions. Non-CO 2 greenhouse gas and aerosol emissions represent equivalent cumulative CO 2 emissions of about 510 PgC and -180 PgC for 1.5 °C, respectively. The increased LUC, high non-CO 2 emissions and decreased aerosols in our scenario, cause the long-term FF carbon budget to decrease following temperature stabilization. In this scenario, negative emissions would be required to compensate not only for the increasing non-CO 2 climate forcing, but also for the declining natural carbon sinks.

Aerosol observation using multi-wavelength Mie-Raman lidars of the Ad-Net and aerosol component analysis

Directory of Open Access Journals (Sweden)

Nishizawa Tomoaki

2018-01-01

Full Text Available We deployed multi-wavelength Mie-Raman lidars (MMRL at three sites of the AD-Net and have conducted continuous measurements using them since 2013. To analyze the MMRL data and better understand the externally mixing state of main aerosol components (e.g., dust, sea-salt, and black carbon in the atmosphere, we developed an integrated package of aerosol component retrieval algorithms, which have already been developed or are being developed, to estimate vertical profiles of the aerosol components. This package applies to the other ground-based lidar network data (e.g., EARLINET and satellite-borne lidar data (e.g., CALIOP/CALIPSO and ATLID/EarthCARE as well as the other lidar data of the AD-Net.

Aerosol observation using multi-wavelength Mie-Raman lidars of the Ad-Net and aerosol component analysis

Science.gov (United States)

Nishizawa, Tomoaki; Sugimoto, Nobuo; Shimizu, Atsushi; Uno, Itsushi; Hara, Yukari; Kudo, Rei

2018-04-01

We deployed multi-wavelength Mie-Raman lidars (MMRL) at three sites of the AD-Net and have conducted continuous measurements using them since 2013. To analyze the MMRL data and better understand the externally mixing state of main aerosol components (e.g., dust, sea-salt, and black carbon) in the atmosphere, we developed an integrated package of aerosol component retrieval algorithms, which have already been developed or are being developed, to estimate vertical profiles of the aerosol components. This package applies to the other ground-based lidar network data (e.g., EARLINET) and satellite-borne lidar data (e.g., CALIOP/CALIPSO and ATLID/EarthCARE) as well as the other lidar data of the AD-Net.

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.

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

Science.gov (United States)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Corr, C. A.; Dibb, J. E.; Greenslade, M. E.; Martin, R. F.; Moore, R. H.; Scheuer, E.; Shook, M. A.;

Carbonaceous content of atmospheric aerosols in Lisbon urban atmosphere

Science.gov (United States)

Mirante, Fátima; Oliveira, C.; Martins, N.; Pio, C.; Caseiro, A.; Cerqueira, M.; Alves, C.; Oliveira, C.; Oliveira, J.; Camões, F.; Matos, M.; Silva, H.

2010-05-01

Lisbon is the capital city of Portugal with about 565,000 residents and a population density of 6,600 inhabitants per square kilometre. The town is surrounded by satellite cities, forming together a region known as "Lisbon Metropolitan Area" with about 3 million inhabitants. It is estimated that more than one million citizens come into the Lisbon area every day from the outskirts, leading to elevated traffic densities and intense traffic jams. Airborne particulate matter limit values are frequently exceeded, with important consequences on air pollution levels and obvious negative impacts on human health. Atmospheric aerosols are known to have in their structure significant amounts of carbonaceous material. The knowledge of the aerosols carbon content, particularly on their several carbon forms (as TC, EC and OC, meaning respectively Total, Elemental and Organic carbon) is often required to provide information for source attribution. In order to assess the vehicles PM input, two sampling campaigns (summer and winter periods) were carried out in 2008 in Lisbon in two contrasting sites, a roadside and an urban background site. Particulate matter was collected in two fractions on quartz fibre filters using Hi-Vol samplers (coarse fraction, 2.5µmwork was performed under Project PAHLIS (Polycyclic Aromatic Hydrocarbons Contamination in Lisbon Urban Atmosphere - PTDC/AMB/65699/2006) financed by "Fundação para a Ciência e a Tecnologia" - FCT. Fátima Mirante acknowledges FCT her PhD grant (SFRH/BD/45473/2008).

Water soluble organic carbon in aerosols (PM1, PM2.5, PM10) and various precipitation forms (rain, snow, mixed) over the southern Baltic Sea station.

Science.gov (United States)

Witkowska, Agnieszka; Lewandowska, Anita U

2016-12-15

In the urbanized coastal zone of the Southern Baltic, complex measurements of water soluble organic carbon (WSOC) were conducted between 2012 and 2015, involving atmospheric precipitation in its various forms (rain, snow, mixed) and PM1, PM2.5 and PM10 aerosols. WSOC constituted about 60% of the organic carbon mass in aerosols of various sizes. The average concentration of WSOC was equal to 2.6μg∙m -3 in PM1, 3.6μg∙m -3 in PM2.5 and 4.4μg∙m -3 in PM10. The lowest concentration of WSOC was noted in summer as a result of effective removal of this compound with rainfall. The highest WSOC concentrations in PM2.5 and PM10 aerosols were measured in spring, which should be associated with developing vegetation on land and in the sea. On the other hand, the highest WSOC concentrations in PM1 occurred in winter at low air temperatures and greatest atmospheric stability, when there were increased carbon emissions from fuel combustion in the communal-utility sector and from transportation. WSOC concentrations in precipitation were determined by its form. Mixed precipitation turned out to be the richest in soluble organic carbon (5.1mg·dm -3 ), while snow contained the least WSOC (1.7mg·dm -3 ). Snow and rain cleaned carbon compounds from the atmosphere more effectively when precipitation lasted longer than 24h, while in the case of mixed precipitation WSOC was removed most effectively within the first 24h. Copyright © 2016 Elsevier B.V. All rights reserved.

Sources and characteristics of carbonaceous aerosol in two largest cities in Pearl River Delta Region, China

Science.gov (United States)

Duan, Jingchun; Tan, Jihua; Cheng, Dingxi; Bi, Xinhui; Deng, Wenjing; Sheng, Guoying; Fu, Jiamo; Wong, M. H.

PM 2.5 samples were collected at five sites in Guangzhou and Hong Kong, Pearl River Delta Region (PRDR), China in both summer and winter during 2004-2005. Elemental carbon (EC) and organic carbon (OC) in these samples were measured. The OC and EC concentrations ranked in the order of urban Guangzhou > urban Hong Kong > background Hong Kong. Total carbonaceous aerosol (TCA) contributed less to PM 2.5 in urban Guangzhou (32-35%) than that in urban Hong Kong (43-57%). The reason may be that, as an major industrial city in South China, Guangzhou would receive large amount of inorganic aerosol from all kinds of industries, however, as a trade center and seaport, urban Hong Kong would mainly receive organic aerosol and EC from container vessels and heavy-duty diesel trucks. At Hong Kong background site Hok Tsui, relatively lower contribution of TCA to PM 2.5 may result from contributions of marine inorganic aerosol and inland China pollutant. Strong correlation ( R2=0.76-0.83) between OC and EC indicates minor fluctuation of emission and the secondary organic aerosol (SOA) formation in urban Guangzhou. Weak correlation between OC and EC in Hong Kong can be related to the impact of the long-range transported aerosol from inland China. Averagely, secondary OC (SOC) concentrations were 3.8-5.9 and 10.2-12.8 μg m -3, respectively, accounting for 21-32% and 36-42% of OC in summer and winter in Guangzhou. The average values of 4.2-6.8% for SOA/ PM 2.5 indicate that SOA was minor component in PM 2.5 in Guangzhou.

Study of total column atmospheric aerosol optical depth, ozone and ...

Indian Academy of Sciences (India)

R. Narasimhan (Krishtel eMaging) 1461 1996 Oct 15 13:05:22

general circulation models. ... at all wavelengths from initial to later part of observation period due to cloud-scavenging and rain-washout effects as well as signature of coastal aerosol loading. ... important roles in the study of the Earth's climate.

Comparison of structural features of water-soluble organic matter from atmospheric aerosols with those of aquatic humic substances

Science.gov (United States)

Duarte, Regina M. B. O.; Santos, Eduarda B. H.; Pio, Casimiro A.; Duarte, Armando C.

Elemental analysis, Fourier transform infrared coupled to attenuated total reflectance (FTIR-ATR) and solid-state cross polarization with magic angle spinning- 13C-nuclear magnetic resonance (CPMAS 13C NMR) spectroscopies were used to compare the chemical features of water-soluble organic compounds (WSOC) from atmospheric aerosols with those of aquatic humic and fulvic acids. The influence of different meteorological conditions on the structural composition of aerosol WSOC was also evaluated. Prior to the structural characterisation, the WSOC samples were separated into hydrophobic acids and hydrophilic acids fractions by using a XAD-8/XAD-4 isolation procedure. Results showed that WSOC hydrophobic acids are mostly aliphatic (40-62% of total NMR peak area), followed by oxygenated alkyls (15-21%) and carboxylic acid (5.4-13.4%) functional groups. Moreover, the aromatic content of aerosol WSOC samples collected between autumn and winter seasons is higher (˜18-19%) than that of samples collected during warmer periods (˜6-10%). The presence of aromatic signals typical of lignin-derived structures in samples collected during low-temperature conditions highlights the major contribution of wood burning processes in domestic fireplaces into the bulk chemical properties of WSOC from aerosols. According to our investigations, aerosol WSOC hydrophobic acids and aquatic fulvic and humic acids hold similar carbon functional groups; however, they differ in terms of the relative carbon distribution. Elemental analysis indicates that H and N contents of WSOC hydrophobic acids samples surpass those of aquatic fulvic and humic acids. In general, the obtained results suggest that WSOC hydrophobic acids have a higher aliphatic character and a lower degree of oxidation than those of standard fulvic and humic acids. The study here reported suggests that aquatic fulvic and humic acids may not be good models for WSOC from airborne particulate matter.

Characterization of fresh and aged organic aerosol emissions from meat charbroiling

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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.

Sensitivity of aerosol loading and properties to cloudiness

Science.gov (United States)

Iversen, T.; Seland, O.; Kirkevag, A.; Kristjansson, J. E.

2005-12-01

Clouds influence aerosols in various ways. Sulfate is swiftly produced in liquid phase provided there is both sulfur dioxide and oxidants available. Nucleation and Aitken mode aerosol particles efficiently grow in size by collision and coagulation with cloud droplets. When precipitation is formed, aerosol and precursor gases may be quickly removed bay rainout. The dynamics associated with clouds in some cases may swiftly mix aerosols deeply into the troposphere. In some cases Aitken-mode particles may be formed in cloud droplets by splitting agglomerates of particulate matter such as black carbon In this presentation we will discuss how global cloudiness may influence the burden, residence time, and spatial distribution of sulfate, black carbon and particulate organic matter. A similar physico-chemical scheme for there compounds has been implemented in three generations of the NCAR community climate model (CCM3, CAM2 and CAM3). The scheme is documented in the literature and is a part of the Aerocom-intercomparison. There are many differences between these models. With respect to aerosols, a major difference is that CAM3 has a considerably higher global cloud volume and more then twice the amount of cloud water than CAM2 and CCM3. Atmospheric simulations have been made with prescribed ocean temperatures. It is slightly surprising to discover that certain aspects of the aerosols are not particularly sensitive to these differences in cloud availability. This sensitivity will be compared to sensitivities with respect to processing in deep convective clouds.

Estimation of atmospheric columnar organic matter (OM) mass concentration from remote sensing measurements of aerosol spectral refractive indices

Science.gov (United States)

Zhang, Ying; Li, Zhengqiang; Sun, Yele; Lv, Yang; Xie, Yisong

2018-04-01

Aerosols have adverse effects on human health and air quality, changing Earth's energy balance and lead to climate change. The components of aerosol are important because of the different spectral characteristics. Based on the low hygroscopic and high scattering properties of organic matter (OM) in fine modal atmospheric aerosols, we develop an inversion algorithm using remote sensing to obtain aerosol components including black carbon (BC), organic matter (OM), ammonium nitrate-like (AN), dust-like (DU) components and aerosol water content (AW). In the algorithm, the microphysical characteristics (i.e. volume distribution and complex refractive index) of particulates are preliminarily separated to fine and coarse modes, and then aerosol components are retrieved using bimodal parameters. We execute the algorithm using remote sensing measurements of sun-sky radiometer at AERONET site (Beijing RADI) in a period from October of 2014 to January of 2015. The results show a reasonable distribution of aerosol components and a good fit for spectral feature calculations. The mean OM mass concentration in atmospheric column is account for 14.93% of the total and 56.34% of dry and fine-mode aerosol, being a fairly good correlation (R = 0.56) with the in situ observations near the surface layer.

Radioactive content in aerosols and rainwater; Contenido radiactivo en aerosoles y agua de lluvia

Energy Technology Data Exchange (ETDEWEB)

Rodriguez Perestelo, N.; Lopez Perez, M.; Rodriguez, S.; Duarte, X.; Catalan, A.; Fernandez de Aldecoa, J. C.; Hernandez, J.

2013-07-01

The environmental radiological characterization of a place requires knowledge of the radioactive contents of its components, such as air (aerosol), rain, soil, etc ... Inhalation of radioactive aerosols in the air remains the main component of the total dose to the world population. This work focuses on its determination. (Author)

Radiative effects of absorbing aerosols over northeastern India: Observations and model simulations

Science.gov (United States)

Gogoi, Mukunda M.; Babu, S. Suresh; Moorthy, K. Krishna; Bhuyan, Pradip Kumar; Pathak, Binita; Subba, Tamanna; Chutia, Lakhima; Kundu, Shyam Sundar; Bharali, Chandrakala; Borgohain, Arup; Guha, Anirban; De, Barin Kumar; Singh, Brajamani; Chin, Mian

2017-01-01

Multiyear measurements of spectral properties of aerosol absorption are examined over four geographically distinct locations of northeastern India. Results indicated significant spatiotemporal variation in aerosol absorption coefficients (σabs) with highest values in winter and lowest in monsoon. The western parts of the region, close to the outflow of Indo-Gangetic Plains, showed higher values of σabs and black carbon (BC) concentration—mostly associated with fossil fuel combustion. But, the eastern parts showed higher contributions from biomass-burning aerosols, as much as 20-25% to the total aerosol absorption, conspicuously during premonsoon season. This is attributed to a large number of burning activities over the Southeast Asian region, as depicted from Moderate Resolution Imaging Spectroradiometer fire count maps, whose spatial extent and magnitude peaks during March/April. The nearly consistent high values of aerosol index (AI) and layer height from Ozone Monitoring Instrument indicate the presence of absorbing aerosols in the upper atmosphere. The observed seasonality has been captured fairly well by Goddard Chemistry Aerosol Radiation and Transport (GOCART) as well as Weather Research and Forecasting-Chemistry (WRF-Chem) model simulations. The ratio of column-integrated optical depths due to particulate organic matter and BC from GOCART showed good coincidence with satellite-based observations, indicating the increased vertical dispersion of absorbing aerosols, probably by the additional local convection due to higher fire radiative power caused by the intense biomass-burning activities. In the WRF-Chem though underperformed by different magnitude in winter, the values are closer or overestimated near the burnt areas. Atmospheric forcing due to BC was highest ( 30 Wm-2) over the western part associated with the fossil fuel combustion.

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.

Climate Impacts of CALIPSO-Guided Corrections to Black Carbon Aerosol Vertical Distributions in a Global Climate Model

International Nuclear Information System (INIS)

Kovilakam, Mahesh; Mahajan, Salil; Saravanan, R.; Chang, Ping

2017-01-01

Here, we alleviate the bias in the tropospheric vertical distribution of black carbon aerosols (BC) in the Community Atmosphere Model (CAM4) using the Cloud-Aerosol and Infrared Pathfinder Satellite Observations (CALIPSO)-derived vertical profiles. A suite of sensitivity experiments are conducted with 1x, 5x, and 10x the present-day model estimated BC concentration climatology, with (corrected, CC) and without (uncorrected, UC) CALIPSO-corrected BC vertical distribution. The globally averaged top of the atmosphere radiative flux perturbation of CC experiments is ~8–50% smaller compared to uncorrected (UC) BC experiments largely due to an increase in low-level clouds. The global average surface temperature increases, the global average precipitation decreases, and the ITCZ moves northward with the increase in BC radiative forcing, irrespective of the vertical distribution of BC. Further, tropical expansion metrics for the poleward extent of the Northern Hemisphere Hadley cell (HC) indicate that simulated HC expansion is not sensitive to existing model biases in BC vertical distribution.

Estimation of the mass absorption cross-section of the black and brown carbon aerosols during GoPoEx 2014

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Cho, C.; Kim, S. W.; Lee, M.; Gustafsson, O.; Fang, W.

2017-12-01

Black carbon (BC) is a major contributor to the atmospheric heating by absorbing the solar radiation. According to recent studies, the solar absorption of brown carbon (BrC) is not negligible and even comparable to that of BC at visible to UV wavelengths, but most optical instruments that quantify light absorption are unable to distinguish each other. Thus, light absorption properties of BC or BrC usually have been studied through modeling researches by using mass absorption cross-section (MAC). Although MAC has a large spatial and temporal variability, most modeling studies have used a specific value of BC MAC and even the absorption by BrC is seldom considered in most chemical and climate models. The generalization of modeling research can lead to serious errors of radiative forcing by BC and BrC. In this study, MAC of BC and BrC are separately determined and the contribution of BC and BrC on aerosol light absorption are estimated from co-located simultaneous in-situ measurements, COSMOS, CLAP and Sunset EC/OC analyzer, at Gosan climate observatory, Korea during Gosan Pollution Experiment in January 2014 (GoPoEx 2014). At 565 nm, MAC of BC is found to be about 6.4±1.5 m2 g-1 from COSMOS and Sunset EC/OC analyzer measurements. This value is similar to those from previous studies in China (Cui et al., STE, 2016), but lower than those observed to be ranged 10-18 m2 g-1 in America or Europe (Lack et al., PNAS, 2012). Aerosol absorption coefficient (AAC) and BC mass concentration from COSMOS, meanwhile, are approximately 15-20% lower than those of CLAP. This difference can be attributable to the contribution of BrC. The MAC of BrC was calculated using the absorption coefficient of BrC and by the following three methods: (1) the difference of mass concentration from Aethalometer and COSMOS applied new BC MAC of this study, (2) The mass concentration of water-soluble organic carbon, (3) a method using the mass concentration of organic carbon suggested by Chung et al

CV-Dust: Atmospheric aerosol in the Cape Verde region: carbon and soluble fractions of PM10

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Pio, C.; Nunes, T.; Cardoso, J.; Caseiro, A.; Custódio, D.; Cerqueira, M.; Patoilo, D.; Almeida, S. M.; Freitas, M. C.

2012-04-01

than 100 PM10 samples, addressing mainly their mass concentrations and the chemical composition of water soluble ions and carbon species (carbonates and organic and elemental carbon). Different PM10 samplers worked simultaneously in order to collect enough mass to make the aerosol characterization through the different methodologies and to collect aerosols in different filter matrixes, which have to be appropriated to the chemical and mineralogical analysis. The sampling site was located at Santiago Island, in the surroundings of Praia City (14° 55' N e 23° 29' W, 98 m at sea level). High concentrations, up to more than 400 μg m-3, are connected to north-east and north-northeast winds, and it was identified several dust events characteristic of "bruma seca", whose duration is on average of two to four days. Backward trajectories analysis confirms that the high concentrations in Cape Verde are associated with air masses passing over the Sahara. During dust events the percentage of inorganic water soluble ions for the total PM10 mass concentration decreased significantly to values lower than 10% in comparison with remainder data that range around 45±10%. Acknowledgement: This work was funded by the Portuguese Science Foundation (FCT) through the project PTDD/AAC-CLI/100331/2008 and FCOMP-01-0124-FEDER-008646 (CV-Dust). J. Cardoso acknowledges the PhD grant SFRH-BD-6105-2009 from FCT.

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

Science.gov (United States)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

Science.gov (United States)

Persad, Geeta Gayatri

' surface versus atmospheric forcing. Future aerosol emissions patterns will affect the distribution of regional climate impacts. This dissertation interrogates how international trade affects existing assumptions about East Asia's future black carbon aerosol emissions, using integrated assessment modeling, emissions and economic data, and AM3 simulations. Exports emerge as a uniquely large and potentially growing source of Chinese black carbon emissions that could impede projected regional emissions reductions, with substantial climate and health consequences. The findings encourage greater emissions projection sophistication and illustrate how societal decisions may influence future aerosol forcing heterogeneity.

Cloud albedo increase from carbonaceous aerosol

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W. R. Leaitch

2010-08-01

Full Text Available Airborne measurements from two consecutive days, analysed with the aid of an aerosol-adiabatic cloud parcel model, are used to study the effect of carbonaceous aerosol particles on the reflectivity of sunlight by water clouds. The measurements, including aerosol chemistry, aerosol microphysics, cloud microphysics, cloud gust velocities and cloud light extinction, were made below, in and above stratocumulus over the northwest Atlantic Ocean. On the first day, the history of the below-cloud fine particle aerosol was marine and the fine particle sulphate and organic carbon mass concentrations measured at cloud base were 2.4 μg m⁻³ and 0.9 μg m⁻³ respectively. On the second day, the below-cloud aerosol was continentally influenced and the fine particle sulphate and organic carbon mass concentrations were 2.3 μg m⁻³ and 2.6 μg m⁻³ respectively. Over the range 0.06–0.8 μm diameter, the shapes of the below-cloud size distributions were similar on both days and the number concentrations were approximately a factor of two higher on the second day. The cloud droplet number concentrations (CDNC on the second day were approximately three times higher than the CDNC measured on the first day. Using the parcel model to separate the influence of the differences in gust velocities, we estimate from the vertically integrated cloud light scattering measurements a 6% increase in the cloud albedo principally due to the increase in the carbonaceous components on the second day. Assuming no additional absorption by this aerosol, a 6% albedo increase translates to a local daytime radiative cooling of ∼12 W m⁻². This result provides observational evidence that the role of anthropogenic carbonaceous components in the cloud albedo effect can be much larger than that of anthropogenic sulphate, as some global simulations have indicated.

Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

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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

The regional aerosol-climate model REMO-HAM

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J.-P. Pietikäinen

2012-11-01

Full Text Available REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km² and 10 × 10 km². Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.

Evaluating inter-continental transport of fine aerosols:(2) Global health impact

Science.gov (United States)

Liu, Junfeng; Mauzerall, Denise L.; Horowitz, Larry W.

In this second of two companion papers, we quantify for the first time the global impact on premature mortality of the inter-continental transport of fine aerosols (including sulfate, black carbon, organic carbon, and mineral dust) using the global modeling results of (Liu et al., 2009). Our objective is to estimate the number of premature mortalities in each of ten selected continental regions resulting from fine aerosols transported from foreign regions in approximately year 2000. Our simulated annual mean population-weighted (P-W) concentrations of total PM2.5 (aerosols with diameter less than 2.5 μm) are highest in East Asia (EA, 30 μg m -3) and lowest in Australia (3.6 μg m -3). Dust is the dominant component of PM2.5 transported between continents. We estimate global annual premature mortalities (for adults age 30 and up) due to inter-continental transport of PM2.5 to be nearly 380 thousand (K) in 2000. Approximately half of these deaths occur in the Indian subcontinent (IN), mostly due to aerosols transported from Africa and the Middle East (ME). Approximately 90K deaths globally are associated with exposure to foreign (i.e., originating outside a receptor region) non-dust PM2.5. More than half of the premature mortalities associated with foreign non-dust aerosols are due to aerosols originating from Europe (20K), ME (18K) and EA (15K); and nearly 60% of the 90K deaths occur in EA (21K), IN (19K) and Southeast Asia (16K). The lower and higher bounds of our estimated 95% confidence interval (considering uncertainties from the concentration-response relationship and simulated aerosol concentrations) are 18% and 240% of the estimated deaths, respectively, and could be larger if additional uncertainties were quantified. We find that in 2000 nearly 6.6K premature deaths in North America (NA) were associated with foreign PM2.5 exposure (5.5K from dust PM2.5). NA is least impacted by foreign PM2.5 compared to receptors on the Eurasian continent. However, the

Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands

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P. Schlag

2016-07-01

Full Text Available Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM at the Cabauw Experimental Site for Atmospheric Research (CESAR in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted nearly 1 year from July 2012 to June 2013 as part of the EU-FP7-ACTRIS project (Q-ACSM Network. Including equivalent black carbon an average particulate mass concentration of 9.50 µg m−3 was obtained during the whole campaign with dominant contributions from ammonium nitrate (45 %, organic aerosol (OA, 29 %, and ammonium sulfate (19 %. There were 12 exceedances of the World Health Organization (WHO PM2.5 daily mean limit (25 µg m−3 observed at this rural site using PM1 instrumentation only. Ammonium nitrate and OA represented the largest contributors to total particulate matter during periods of exceedance. Source apportionment of OA was performed season-wise by positive matrix factorization (PMF using the multilinear engine 2 (ME-2 controlled via the source finder (SoFi. Primary organic aerosols were attributed mainly to traffic (8–16 % contribution to total OA, averaged season-wise and biomass burning (0–23 %. Secondary organic aerosols (SOAs, 61–84 % dominated the organic fraction during the whole campaign, particularly on days with high mass loadings. A SOA factor which is attributed to humic-like substances (HULIS was identified as a highly oxidized background aerosol in Cabauw. This shows the importance of atmospheric aging processes for aerosol concentration at this rural site. Due to the large secondary fraction, the reduction of particulate mass at this rural site is challenging on a local scale.

Water-soluble ions and carbon content of size-segregated aerosols in New Delhi, India: direct and indirect influences of firework displays.

Science.gov (United States)

Kumar, Pawan; Kumar, Rakesh; Yadav, Sudesh

2016-10-01

The particle size distribution and water-soluble inorganic ion (WSII) and carbonaceous species in size-segregated aerosols, Dp firework displays in New Delhi, India. The firework activity had the maximum contribution to the mass loading of PM 0.95 (786 μg/m 3 ) followed by PM 0.95-1.5 (216 μg/m 3 ) with all other three fractions accounting to a total of 214 μg/m 3 . The percentage contributions of WSII to the total mass of aerosols were highest in first two size fractions (39 and 40 %, respectively), compared to other fractions. The firework marker ion (Mg 2+ , Cl - , and K + ) mass concentration shows higher values in PM 0.95 during Diwali compared to before Diwali period. The mass size distribution of particles, NH 4 + , K + , Cl - , SO 4 2- , Mg 2+ , and NO 3 - , also showed changes on the Diwali night compared to previous and after days. The high Cl - /Na + (5.6) and OC/EC (3.4) ratio of PM 0.95 can be used as the indicators of firework displays. The lowering of mixing height on Diwali night to 50 m compared to before (277 mts) and after (269 mts) Diwali period further concentrated the aerosols in ambient atmosphere. Therefore, the firework display not only released the gaseous or elemental constituent but also influenced the temperature profile and both put together result in high aerosol concentrations, WSII, OC, and BC contents in ambient atmosphere. The alveolar, respirable, and inhalable fractions accounted for 64.6, 90.8, and 97.8 %, respectively, of the total PM 10 mass. People stay exposed to such high pollution level in short span of 6-8 h and experience adverse health impacts due to high mass concentrations and the chemical components of fine aerosols.

Rural continental aerosol properties and processes observed during the Hohenpeissenberg Aerosol Characterization Experiment (HAZE2002

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N. Hock

2008-02-01

Full Text Available Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD in Southern Germany.

Online measurements included: Size-resolved chemical composition of submicron particles; total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm; gas-phase concentration of monoterpenes, CO, O₃, OH, and H₂SO₄. Filter sampling and offline analytical techniques were used to determine: Fine particle mass (PM2.5, organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5, and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins.

Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m⁻³, arithmetic mean and standard deviation accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m⁻³. The relative proportions of non-refractory submicron particle components were: (23±39% ammonium nitrate, (27±23% ammonium sulfate, and (50±40% organics (OM1. OM1 was closely correlated with PM1 (r²=0.9 indicating a near-constant ratio of non-refractory organics and inorganics.

The average ratio of OM1 to OC2.5 was 2.1±1.4, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA over hydrocarbon-like organic aerosol (HOA inferred from the AMS results (4:1, and also with the high abundance of proteins (~3% indicating a high proportion of primary biological material (~30% in PM2.5. This finding was confirmed by low abundance of PAHs (<1 ng m⁻³ and EC (<1 μg m⁻³ in PM2.5 and detection of several

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

Science.gov (United States)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

Two-Column Aerosol Project (TCAP) Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Berg, Larry K [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2016-05-01

This study included the deployment of the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Mobile Facility (AMF), ARM Mobile Aerosol Observing System (MAOS) and the ARM Aerial Facility (AAF). The study was a collaborative effort involving scientists from DOE national laboratories, NOAA, NASA, and universities. The AAF and MAOS were deployed for two approximately month-long Intensive Operational Periods (IOPs) conducted in June 2012 and February 2013. Seasonal differences in the aerosol chemical and optical properties observed using the AMF, AAF, and MAOS are presented in this report. The total mass loading of aerosol is found to be much greater in the summer than in the winter, with the difference associated with greater amounts of organic aerosol. The mass fraction of organic aerosol is much reduced in the winter, when sulfate is the dominant aerosol type. Surprisingly, very little sea-salt aerosol was observed in the summer. In contrast, much more sea salt aerosol was observed in the winter. The mass loading of black carbon is nearly the same in both seasons. These differences lead to a relative increase in the aerosol light absorption in the winter and an associated decrease in observed single-scattering albedo. Measurements of aerosol mixing state were made using a single-particle mass spectrometer, which showed that the majority of the summertime aerosol consisted of organic compounds mixed with various amounts of sulfate. A number of other findings are also summarized in the report, including: impact of aerosol layers aloft on the column aerosol optical depth; documentation of the aerosol properties at the AMF; differences in the aerosol properties associated with both columns, which are not systematic but reflect the complicated meteorological and chemical processes that impact aerosol as it is advected away from North America; and new instruments and data-processing techniques for measuring both aerosol and

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

Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

Science.gov (United States)

Marley, N. A.; Marchany-Rivera, A.; Kelley, K. L.; Mangu, A.; Gaffney, J. S.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (Petroleo (IMP) and CENICA.

Carbonaceous aerosol at two rural locations in New York State: Characterization and behavior

Science.gov (United States)

Sunder Raman, Ramya; Hopke, Philip K.; Holsen, Thomas M.

2008-06-01

Fine particle samples were collected to determine the chemical constituents in PM2.5 at two rural background sites (Potsdam and Stockton, N. Y.) in the northeastern United States from November 2002 to August 2005. Samples were collected every third day for 24 h with a speciation network sampler. The measured carbonaceous species included thermal-optical organic carbon (OC), elemental carbon (EC), pyrolytic carbon (OP), black carbon (BC), and water-soluble, short-chain (WSSC) organic acids. Concentration time series, autocorrelations, and seasonal variations of the carbonaceous species were examined. During this multiyear period, the contributions of the total carbon (OC + EC) to the measured fine particle mass were 31.2% and 31.1% at Potsdam and Stockton, respectively. The average sum of the WSSC acids carbon accounted for approximately 2.5% of the organic carbon at Potsdam and 3.0% at Stockton. At Potsdam, the seasonal differences in the autocorrelation function (ACF) and partial autocorrelation function (PACF) values for carbonaceous species suggest that secondary formation may be an important contributor to the observed concentrations of species likely to be secondary in origin, particularly during the photochemically active time of the year (May to October). This study also investigated the relationships between carbonaceous species to better understand the behavior of carbonaceous aerosol and to assess the contribution of secondary organic carbon (SOC) to the total organic carbon mass (the EC tracer method was used to estimate SOC). At Potsdam the average SOC contribution to total OC varied between 66% and 72%, while at Stockton it varied between 58% and 64%.

Workplace aerosol mass concentration measurement using optical particle counters.

Science.gov (United States)

Görner, Peter; Simon, Xavier; Bémer, Denis; Lidén, Göran

2012-02-01

Direct-reading aerosol measurement usually uses the optical properties of airborne particles to detect and measure particle concentration. In the case of occupational hygiene, mass concentration measurement is often required. Two aerosol monitoring methods are based on the principle of light scattering: optical particle counting (OPC) and photometry. The former analyses the light scattered by a single particle, the latter by a cloud of particles. Both methods need calibration to transform the quantity of scattered light detected into particle concentration. Photometers are simpler to use and can be directly calibrated to measure mass concentration. However, their response varies not only with aerosol concentration but also with particle size distribution, which frequently contributes to biased measurement. Optical particle counters directly measure the particle number concentration and particle size that allows assessment of the particle mass provided the particles are spherical and of known density. An integrating algorithm is used to calculate the mass concentration of any conventional health-related aerosol fraction. The concentrations calculated thus have been compared with simultaneous measurements by conventional gravimetric sampling to check the possibility of field OPC calibration with real workplace aerosols with a view to further monitoring particle mass concentration. Aerosol concentrations were measured in the food industry using the OPC GRIMM® 1.108 and the CIP 10-Inhalable and CIP 10-Respirable (ARELCO®) aerosol samplers while meat sausages were being brushed and coated with calcium carbonate. Previously, the original OPC inlet had been adapted to sample inhalable aerosol. A mixed aerosol of calcium carbonate and fungi spores was present in the workplace. The OPC particle-size distribution and an estimated average particle density of both aerosol components were used to calculate the mass concentration. The inhalable and respirable aerosol fractions

Impact of cloud-borne aerosol representation on aerosol direct and indirect effects

Directory of Open Access Journals (Sweden)

S. J. Ghan

2006-01-01

Full Text Available Aerosol particles attached to cloud droplets are much more likely to be removed from the atmosphere and are much less efficient at scattering sunlight than if unattached. Models used to estimate direct and indirect effects of aerosols employ a variety of representations of such cloud-borne particles. Here we use a global aerosol model with a relatively complete treatment of cloud-borne particles to estimate the sensitivity of simulated aerosol, cloud and radiation fields to various approximations to the representation of cloud-borne particles. We find that neglecting transport of cloud-borne particles introduces little error, but that diagnosing cloud-borne particles produces global mean biases of 20% and local errors of up to 40% for aerosol, droplet number, and direct and indirect radiative forcing. Aerosol number, aerosol optical depth and droplet number are significantly underestimated in regions and seasons where and when wet removal is primarily by stratiform rather than convective clouds (polar regions during winter, but direct and indirect effects are less biased because of the limited sunlight there and then. A treatment that predicts the total mass concentration of cloud-borne particles for each mode yields smaller errors and runs 20% faster than the complete treatment. The errors are much smaller than current estimates of uncertainty in direct and indirect effects of aerosols, which suggests that the treatment of cloud-borne aerosol is not a significant source of uncertainty in estimates of direct and indirect effects.

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

Science.gov (United States)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.;

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

Energy Technology Data Exchange (ETDEWEB)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, John; Hostetler, Chris A.; Hubbe, John M.; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, K.; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail S.; Rogers, Ray; Russell, P.; Redemann, Jens; Sedlacek, Art; Segal Rozenhaimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline; Volkamer, Rainer M.; Zelenyuk, Alla; Berkowitz, Carl M.

2016-01-08

The Two-Column Aerosol Project (TCAP), which was conducted from June 2012 through June 2013, was a unique field study that was designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere at a number of altitudes, from near the surface to as high as 8 km, within two atmospheric columns; one located near the coast of North America (over Cape Cod, MA) and a second over the Atlantic Ocean several hundred kilometers from the coast. TCAP included the yearlong deployment of the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) that was located at the base of the Cape Cod column, as well as summer and winter aircraft intensive observation periods of the ARM Aerial Facility. One important finding from TCAP is the relatively common occurrence (on four of six nearly cloud-free flights) of elevated aerosol layers in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total aerosol optical depth (AOD) observed in the column. Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning aerosol and nitrate compared to the aerosol found near the surface.

The Two-Column Aerosol Project: Phase I—Overview and impact of elevated aerosol layers on aerosol optical depth

Science.gov (United States)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

2016-01-01

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

Aerosol Climate Time Series Evaluation In ESA Aerosol_cci

Science.gov (United States)

Popp, T.; de Leeuw, G.; Pinnock, S.

2015-12-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. By the end of 2015 full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which are also validated. The paper will summarize and discuss the results of major reprocessing and validation conducted in 2015. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension with successor instruments of the Sentinel family will be described and the complementarity of the different satellite aerosol products

Laboratory experiments on the formation and recoil jet transport of aerosol by laser ablation

Science.gov (United States)

Hirooka, Yoshi; Tanaka, Kazuo A.; Imamura, Keisuke; Okazaki, Katsuya

2016-05-01

In a high-repetition rate inertial fusion reactor, the first wall will be subjected to repeated ablation along with pellet implosions, which then leads to the formation of aerosol to scatter and/or deflect laser beams for the subsequent implosion, affecting the overall reactor performance. Proposed in the present work is a method of in-situ directed transport of aerosol particles by the use of laser ablation-induced jet recoil momenta. Lithium and carbon are used as the primary ablation targets, the former of which is known to form aerosol in the form of droplet, and the latter of which tends to form carbon nanotubes. Laboratory-scale experiments have been conducted to irradiate airborne aerosol particles with high-intensity laser to produce ablation-induced jet. Data have indicated a change in aerosol flow direction, but only in the case of lithium.

IMAA (Integrated Measurements of Aerosol in Agri valley) campaign: Multi-instrumental observations at the largest European oil/gas pre-treatment plant area

Science.gov (United States)

Calvello, Mariarosaria; Caggiano, Rosa; Esposito, Francesco; Lettino, Antonio; Sabia, Serena; Summa, Vito; Pavese, Giulia

2017-11-01

A short-term intensive multi-instrumental measurement campaign (Integrated Measurements of Aerosol in Agri valley - IMAA) was carried out near the largest European oil and gas pre-treatment plant (Centro Olio Val d'Agri - COVA) in a populated area, where, so far, ample characterization of aerosol loading is missing. As such, between the 2 and 17 July in 2013, using a number of instruments analyses were carried out on physical, chemical, morphological and optical properties of aerosol at this distinctive site, at both ground and over the atmospheric column, including the investigation of the mixing and transformation of particles. The observation of slag silicates with a rough surface texture is consistent with the presence of oil-related activities which represent the only industrial activity in the area. Desulfurization/sulfur liquefaction processes occurring at COVA can explain the peculiar morphology of calcium-sodium-aluminum particles. The common COVA source was associated with high concentrations of sulfur, nickel and zinc, and with significant correlations between zinc-sulfur and zinc-nickel. The Optical Particle Sizer (OPS) data, hygroscopicity and optical properties of atmospheric aerosol are consistent with the typical oil-derived gaseous emissions (e.g. sulfur dioxide and methane) that strongly influence the mixing state of particles and their size distributions. Continuous combustion processes at COVA were found to be responsible for Equivalent Black Carbon (EBC) concentrations from their relevant contribution to the total number of fine particles. The expected significant contribution of WS (water soluble) and BC (Black Carbon) components to the total Aerosol Optical Depth (AOD) are consistent with the results from the radiometric model especially for July 3 and 16.

Inferring brown carbon content from UV aerosol absorption measurements during biomass burning season

Science.gov (United States)

Mok, J.; Krotkov, N. A.; Arola, A. T.; Torres, O.; Jethva, H. T.; Andrade, M.; Labow, G. J.; Eck, T. F.; Li, Z.; Dickerson, R. R.; Stenchikov, G. L.; Osipov, S.

2015-12-01

Measuring spectral dependence of light absorption by colored organic or "brown" carbon (BrC) is important, because of its effects on photolysis rates of ozone and surface ultraviolet (UV) radiation. Enhanced UV spectral absorption by BrC can in turn be exploited for simultaneous retrievals of BrC and black carbon (BC) column amounts in field campaigns. We present an innovative ground-based retrieval of BC and BrC volume fractions and their mass absorption efficiencies during the biomass burning season in Santa Cruz, Bolivia in September-October 2007. Our method combines retrieval of BC volume fraction using AERONET inversion in visible wavelengths with the inversion of total BC+BrC absorption (i.e., column effective imaginary refractive index, kmeas) using Diffuse/Direct irradiance measurements in UV wavelengths. First, we retrieve BrC volume fraction by fitting kmeas at 368nm using Maxwell-Garnett (MG) mixing rules assuming: (1) flat spectral dependence of kBC, (2) known value of kBrC at 368nm from laboratory absorption measurements or smoke chamber experiments, and (3) known BC volume fraction from AERONET inversion. Next, we derive kBrC in short UVB wavelengths by fitting kmeas at 305nm, 311nm, 317nm, 325nm, and 332nm using MG mixing rules and fixed volume fractions of BC and BrC. Our retrievals show larger than expected spectral dependence of kBrC in UVB wavelengths, implying reduced surface UVB irradiance and inhibited photolysis rates of surface ozone destruction. We use a one-dimensional chemical box model to show that the observed strong wavelength dependence of BrC absorption leads to inhibited photolysis of ozone to O(1D), a loss mechanism, while having little impact or even accelerating photolysis of NO2, an ozone production mechanism. Although BC only absorption in biomass burning aerosols is important for climate radiative forcing in the visible wavelengths, additional absorption by BrC is important because of its impact on surface UVB radiation

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.

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,...

Aerosol Climate Time Series in ESA Aerosol_cci

Science.gov (United States)

Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon

2016-04-01

with successor instruments of the Sentinel family will be described and the complementarity of the different satellite aerosol products (e.g. dust vs. total AOD, ensembles from different algorithms for the same sensor) will be discussed.

The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore–Washington, D.C. region

Directory of Open Access Journals (Sweden)

A. J. Beyersdorf

2016-01-01

Full Text Available In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites and mass measurements of aerosol loading (PM2.5 used for air quality monitoring must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH, and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 % and organics (57 %. A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs. The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35�

Functional group analysis by H NMR/chemical derivatization for the characterization of organic aerosol from the SMOCC field campaign

Directory of Open Access Journals (Sweden)

E. Tagliavini

2006-01-01

Full Text Available Water soluble organic compounds (WSOC in aerosol samples collected in the Amazon Basin in a period encompassing the middle/late dry season and the beginning of the wet season, were investigated by H NMR spectroscopy. HiVol filter samples (PM2.5 and PM>2.5 and size-segregated samples from multistage impactor were subjected to H NMR characterization. The H NMR methodology, recently developed for the analysis of organic aerosol samples, has been improved by exploiting chemical methylation of carboxylic groups with diazomethane, which allows the direct determination of the carboxylic acid content of WSOC. The content of carboxylic carbons for the different periods and sizes ranged from 12% to 20% of total measured carbon depending on the season and aerosol size, with higher contents for the fine particles in the transition and wet periods with respect to the dry period. A comprehensive picture is presented of WSOC functional groups in aerosol samples representative of the biomass burning period, as well as of transition and semi-clean atmospheric conditions. A difference in composition between fine (PM2.5 and coarse (PM>2.5 size fractions emerged from the NMR data, the former showing higher alkylic content, the latter being largely dominated by R-O-H (or R-O-R' functional groups. Very small particles (<0.14 μm, however, present higher alkyl-chain content and less oxygenated carbons than larger fine particles (0.42–1.2 μm. More limited variations were found between the average compositions in the different periods of the campaign.

Laboratory studies of the chemical composition and cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA

Directory of Open Access Journals (Sweden)

A. T. Lambe

2011-09-01

Full Text Available Secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O₃ in a Potential Aerosol Mass (PAM flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS. The fraction of AMS signal at m/z = 43 and m/z = 44 (f₄₃, f₄₄, the hydrogen-to-carbon (H/C ratio, and the oxygen-to-carbon (O/C ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA. The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f₄₄–f₄₃ composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κ_org, ranged from 8.4×10⁻⁴ to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κ_org and O/C ratio is significantly wider than has been previously obtained. To first order, the κ_org-to-O/C relationship is well represented by a linear function of the form κ_org = (0.18±0.04 ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and

Total Belowground Carbon Allocation in a Fast-growing Eucalyptus Plantation Estimated Using a Carbon Balance Approach

Science.gov (United States)

Christian P. Giardina; Michael G. Ryan

2002-01-01

Trees allocate a large portion of gross primary production belowground for the production and maintenance of roots and mycorrhizae. The difficulty of directly measuring total belowground carbon allocation (TBCA) has limited our understanding of belowground carbon (C) cycling and the factors that control this important flux. We measured TBCA over 4 years using a...

Ice nucleation in sulfuric acid/organic aerosols: implications for cirrus cloud formation

Directory of Open Access Journals (Sweden)

M. R. Beaver

2006-01-01

Full Text Available Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10 and ketones (C3 and C9 on ice nucleation in sulfuric acid aerosols. Mixed aerosols were prepared by combining an organic vapor flow with a flow of sulfuric acid aerosols over a small mixing time (~60 s at room temperature. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. In these experiments, aerosol organic content, determined by a Mie scattering analysis, was found to vary with the partial pressure of organic, the flow tube temperature, and the identity of the organic compound. The physical properties of the organic compounds (primarily the solubility and melting point were found to play a dominant role in determining the inferred mode of nucleation (homogenous or heterogeneous and the specific freezing temperatures observed. Overall, very soluble, low-melting organics, such as acetone and propanal, caused a decrease in aerosol ice nucleation temperatures when compared with aqueous sulfuric acid aerosol. In contrast, sulfuric acid particles exposed to organic compounds of eight carbons and greater, of much lower solubility and higher melting temperatures, nucleate ice at temperatures above aqueous sulfuric acid aerosols. Organic compounds of intermediate carbon chain length, C4-C7, (of intermediate solubility and melting temperatures nucleated ice at the same temperature as aqueous sulfuric acid aerosols. Interpretations and implications of these results for cirrus cloud formation are discussed.

In vivo measurement of total body carbon using 238Pu/Be neutron sources

International Nuclear Information System (INIS)

Sutcliffe, J.F.; Mitra, S.; Hill, G.L.

1990-01-01

Total body carbon has been measured by in vivo neutron activation analysis (IVNAA) in 278 surgical gastroenterological patients and 29 normal volunteers. This is based on the inelastic scattering reaction { 12 C(n,n') 12 C*} for neutrons with energy above 4.8MeV, producing 4.43 MeV gamma rays. Since only part of the body is scanned, total body carbon is estimated as the ratio of the gamma ray emission from carbon to the emission from hydrogen, using hydrogen as the internal standard. The precision of the estimate is ±1.6kg for a whole body dose of 0.3mSv. There is a significant difference between the estimates of total body water from IVNAA measurements of carbon and nitrogen and measurements of body water in these subjects by tritium dilution (t=3.1, p < 0.005). (author)

Secondary organic aerosols: Formation potential and ambient data

DEFF Research Database (Denmark)

Barthelmie, R.J.; Pryor, S.C.

1997-01-01

Organic aerosols comprise a significant fraction of the total atmospheric particle loading and are associated with radiative forcing and health impacts. Ambient organic aerosol concentrations contain both a primary and secondary component. Herein, fractional aerosol coefficients (FAC) are used...... in conjunction with measurements of volatile organic compounds (VOC) to predict the formation potential of secondary organic aerosols (SOA) in the Lower Fraser Valley (LEV) of British Columbia. The predicted concentrations of SOA show reasonable accord with ambient aerosol measurements and indicate considerable...

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.

Reservoir patterns of soot, organic particles, total carbon, soluble substances and aerosols (numbers and mass) in the droplet and interstitial phase of clouds; Reservoiraufteilung von Russ, organischen Bestandteilen, Gesamtkohlenstoff, loeslichen Substanzen und Aerosolpartikeln (Anzahl und Masse) in der Tropfen- und Zwischenraumphase von Wolken. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Wieprecht, W.; Acker, K.; Moeller, D.; Auel, R.; Hofmeister, J.; Kalass, D.

2002-07-01

The reservoir patterns of the constitutents of representative clouds over Germany were investigated for a better characterisation of their optical, microphysical and chemical properties. One of the key points of interest was the distribution of carbonaceous aerosol particles in the droplet and interstitial phase, which was to provide information on the role of absorbing (soot or BC) and organic carbon (OC) in cloud formation. Data about the effects of potential CCN on cloud characteristics and about the changes in aerosol particles induced by cloud processes are required as input for models of the chemical and climate effects of atmospheric aerosol. [German] Ziel des Projektes war eine moeglichst umfassende experimentelle Ermittlung der Reservoiraufteilung der Inhaltsstoffe repraesentativer Wolken ueber der Bundesrepublik Deutschland, um ihre optischen, mikrophysikalischen und chemischen Eigenschaften besser zu charakterisieren. Ein besonderer Schwerpunkt des Gesamtprojekts lag auf der Bestimmung der Verteilung kohlenstoffhaltiger Aerosolpartikel auf die Tropfen- und interstitielle Phase, um Aufschluesse ueber die Rolle von absorbierendem (Russ oder BC) und organischem Kohlenstoff (OC) bei der Wolkenbildung zu erhalten. Erkenntnisse sowohl ueber die Beeinflussung potentieller CCN auf Wolkeneigenschaften als auch ueber die Veraenderung der Aerosolpartikel durch Wolkenprozesse sind erforderlich als Eingangsdaten in entsprechende Modelle, um die chemischen und klimatischen Effekte des atmosphaerischen Aerosols zu bestimmen. (orig.)

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Carbonaceous components, levoglucosan and inorganic ions in tropical aerosols from Tanzania, East Africa: implication for biomass burning contribution to organic aerosols

Science.gov (United States)

Mkoma, S. L.; Kawamura, K.; Fu, P.

2012-11-01

Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania in 2011 during wet and dry seasons and they were analysed for carbonaceous components, levoglucosan and water-soluble inorganic ions. The mean mass concentrations of PM2.5 and PM10 were 28.2±6.4 μg m-3 and 47±8.2 μg m-3 in wet season, and 39.1±9.8 μg m-3 and 61.4±19.2 μg m-3 in dry season, respectively. Total carbon (TC) accounted for 16-19% of the PM2.5 mass and 13-15% of the PM10 mass. On average, 85.9 to 88.7% of TC in PM2.5 and 87.2 to 90.1% in PM10 was organic carbon (OC), of which 67-72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. Water-soluble potassium (K+) and sulphate (SO42-) in PM2.5 and, sodium (Na+) and SO42- in PM10 were the dominant ionic species. We found, that concentrations of biomass burning tracers (levoglucosan and mannosan) well correlated with non-sea-salt-K+, WSOC and OC in the aerosols from Tanzania, East Africa. Mean contributions of levoglucosan to OC ranged between 3.9-4.2% for PM2.5 and 3.5-3.8% for PM10. This study demonstrates that emissions from biomass- and biofuel-burning activities followed by atmospheric photochemical processes mainly control the air quality in Tanzania.

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

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.

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

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

Method of producing carbon coated nano- and micron-scale particles

Science.gov (United States)

Perry, W. Lee; Weigle, John C; Phillips, Jonathan

2013-12-17

A method of making carbon-coated nano- or micron-scale particles comprising entraining particles in an aerosol gas, providing a carbon-containing gas, providing a plasma gas, mixing the aerosol gas, the carbon-containing gas, and the plasma gas proximate a torch, bombarding the mixed gases with microwaves, and collecting resulting carbon-coated nano- or micron-scale particles.

Impact of OH Heterogenous Oxidation on the Evolution of Brown Carbon Aerosol Optical Properties

Science.gov (United States)

Schnitzler, E.; Abbatt, J.

2017-12-01

The effects of varying relative humidity (RH) on the evolution of brown carbon (BrC) optical properties induced by heterogeneous OH oxidation were investigated in a series of photooxidation chamber experiments. A BrC surrogate was generated from aqueous 1,3-dihydroxybenzene (10 mM) and H2O2 (10 mM) exposed to >300 nm radiation, atomized, passed through a series of trace gas denuders, and injected into the chamber, which was conditioned to about 10 or 60% RH. Following aerosol injection, H2O2 was continuously bubbled into the chamber; an hour later, the chamber was irradiated with black-lights (UV-B) to produce OH. Before irradiation, aerosol absorption and scattering at 405 nm, measured using a photoacoustic spectrometer, decreased due only to deposition and dilution, and single scattering albedo (SSA) was relatively steady. In the presence of gas-phase OH, absorption first increased, despite continued particle losses, and SSA decreased. Subsequently, absorption decreased faster than scattering, and SSA increased uniformly. At 60% RH, colour enhancement, likely associated with functionalization, was greatest after only minutes of reaction. In contrast, at 10% RH, peak colour enhancement occurred after about two hours of reaction, indicating that the decrease in RH and the attendant increase in particle viscosity significantly impeded heterogeneous OH oxidation of the BrC surrogate.

Impacts of springtime biomass burning in the northern Southeast Asia on marine organic aerosols over the Gulf of Tonkin, China.

Science.gov (United States)

Zheng, Lishan; Yang, Xiaoyang; Lai, Senchao; Ren, Hong; Yue, Siyao; Zhang, Yingyi; Huang, Xin; Gao, Yuanguan; Sun, Yele; Wang, Zifa; Fu, Pingqing

2018-06-01

Fine particles (PM 2.5 ) samples, collected at Weizhou Island over the Gulf of Tonkin on a daytime and nighttime basis in the spring of 2015, were analyzed for primary and secondary organic tracers, together with organic carbon (OC), elemental carbon (EC), and stable carbon isotopic composition (δ 13 C) of total carbon (TC). Five organic compound classes, including saccharides, lignin/resin products, fatty acids, biogenic SOA tracers and phthalic acids, were quantified by gas chromatography/mass spectrometry (GC/MS). Levoglucosan was the most abundant organic species, indicating that the sampling site was under strong influence of biomass burning. Based on the tracer-based methods, the biomass-burning-derived fraction was estimated to be the dominant contributor to aerosol OC, accounting for 15.7% ± 11.1% and 22.2% ± 17.4% of OC in daytime and nighttime samples, respectively. In two episodes E1 and E2, organic aerosols characterized by elevated concentrations of levoglucosan as well as its isomers, sugar compounds, lignin products, high molecular weight (HMW) fatty acids and β-caryophyllinic acid, were attributed to the influence of intensive biomass burning in the northern Southeast Asia (SEA). However, the discrepancies in the ratios of levoglucosan to mannosan (L/M) and OC (L/OC) as well as the δ 13 C values suggest the type of biomass burning and the sources of organic aerosols in E1 and E2 were different. Hardwood and/or C 4 plants were the major burning materials in E1, while burning of softwood and/or C 3 plants played important role in E2. Furthermore, more complex sources and enhanced secondary contribution were found to play a part in organic aerosols in E2. This study highlights the significant influence of springtime biomass burning in the northern SEA to the organic molecular compositions of marine aerosols over the Gulf of Tonkin. Copyright © 2018 Elsevier Ltd. All rights reserved.

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

Strong impacts on aerosol indirect effects from historical oxidant changes

Science.gov (United States)

Hafsahl Karset, Inger Helene; Koren Berntsen, Terje; Storelvmo, Trude; Alterskjær, Kari; Grini, Alf; Olivié, Dirk; Kirkevåg, Alf; Seland, Øyvind; Iversen, Trond; Schulz, Michael

2018-06-01

Uncertainties in effective radiative forcings through aerosol-cloud interactions (ERFaci, also called aerosol indirect effects) contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from -1.32 to -1.07 W m-2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3). The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

Spectral dependence of aerosol light absorption at an urban and a remote site over the Tibetan Plateau.

Science.gov (United States)

Zhu, Chong-Shu; Cao, Jun-Ji; Hu, Ta-Feng; Shen, Zhen-Xing; Tie, Xue-Xi; Huang, Hong; Wang, Qi-Yuan; Huang, Ru-Jin; Zhao, Zhu-Zi; Močnik, Griša; Hansen, Anthony D A

2017-07-15

We present a study of aerosol light absorption by using a 7-wavelength Aethalometer model AE33 at an urban site (Lhasa) and a remote site (Lulang) in the Tibetan Plateau. Approximately 5 times greater aerosol absorption values were observed at Lhasa (53±46Mm -1 at 370nm and 20±18Mm -1 at 950nm, respectively) in comparison to Lulang (15±19Mm -1 at 370nm and 4±5Mm -1 at 950nm, respectively). Black carbon (BC) was the dominant light absorbing aerosol component at all wavelengths. The brown carbon (BrC) absorption at 370nm is 32±15% of the total aerosol absorption at Lulang, whereas it is 8±6% at Lhasa. Higher value of absorption Ångström exponent (AAE, 370-950nm) was obtained for Lulang (1.18) than that for Lhasa (1.04) due to the presence of BrC. The AAEs (370-950nm) of BrC were directly extracted at Lulang (3.8) and Lhasa (3.3). The loading compensation parameters (k) increased with wavelengths for both sites, and lower values were obtained at Lulang than those observed at Lhasa for all wavelengths. This study underlines the relatively high percentage of BrC absorption contribution in remote area compared to urban site over the Tibetan Plateau. Copyright © 2017 Elsevier B.V. All rights reserved.

Microphysical processing of aerosol particles in orographic clouds

Science.gov (United States)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

Microphysical processing of aerosol particles in orographic clouds

Directory of Open Access Journals (Sweden)

S. Pousse-Nottelmann

2015-08-01

aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener–Bergeron–Findeisen (WBF process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number

Scavenging of particulate elemental carbon into stratus cloud

Energy Technology Data Exchange (ETDEWEB)

Kaneyasu, Naoki; Maeda, Takahisa [National Inst. for Resources and Environment, Tsukuba (Japan)

1995-12-31

The role of atmospheric aerosols on the alternation of cloud radiative properties has widely been recognized since 1977 when Tomey and his coworkers have numerically demonstrated the effect of increased cloud condensation nuclei (CCN). At the same time, cloud processes are one of the most important factor in controlling the residence time of atmospheric aerosols through the wet removal process. The redistribution of the size and the composition of pre-cloud aerosols is also the important role of cloud process on the nature of atmospheric aerosols. In order to study these cloud-aerosol interaction phenomena, the incorporation of aerosols into cloud droplets is the first mechanism to be investigated. Among the several mechanisms for the incorporation of aerosols into cloud droplets, nucleation scavenging, is the potentially important process in the view of cloud-aerosol interactions. This critical supersaturation for a given radius of a particle can be theoretically calculated only for pure species, e.g., NaCl. However, a significant portion of the atmospheric aerosols is in the form of internal mixture of multiple components, such as SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, NH{sub 4}{sup +} and particulate elemental carbon. The knowledge acquired by field measurements is therefore essential on this subject. The present study focuses on the scavenging of major components of urban atmospheric aerosols, in particular the incorporation of particulate elemental carbon into stratus cloud. Particulate elemental carbon is the strongest light absorbing species in visible region, and has potential to change the optical property of cloud. On the basis of the measurements conducted at a mountain located in the suburb of Tokyo Metropolitan area, Japan, some insights on the scavenging of particulate elemental carbon into cloud droplet will be presented

Scavenging of particulate elemental carbon into stratus cloud

Energy Technology Data Exchange (ETDEWEB)

Kaneyasu, Naoki; Maeda, Takahisa [National Inst. for Resources and Environment, Tsukuba (Japan)

1996-12-31

The role of atmospheric aerosols on the alternation of cloud radiative properties has widely been recognized since 1977 when Tomey and his coworkers have numerically demonstrated the effect of increased cloud condensation nuclei (CCN). At the same time, cloud processes are one of the most important factor in controlling the residence time of atmospheric aerosols through the wet removal process. The redistribution of the size and the composition of pre-cloud aerosols is also the important role of cloud process on the nature of atmospheric aerosols. In order to study these cloud-aerosol interaction phenomena, the incorporation of aerosols into cloud droplets is the first mechanism to be investigated. Among the several mechanisms for the incorporation of aerosols into cloud droplets, nucleation scavenging, is the potentially important process in the view of cloud-aerosol interactions. This critical supersaturation for a given radius of a particle can be theoretically calculated only for pure species, e.g., NaCl. However, a significant portion of the atmospheric aerosols is in the form of internal mixture of multiple components, such as SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, NH{sub 4}{sup +} and particulate elemental carbon. The knowledge acquired by field measurements is therefore essential on this subject. The present study focuses on the scavenging of major components of urban atmospheric aerosols, in particular the incorporation of particulate elemental carbon into stratus cloud. Particulate elemental carbon is the strongest light absorbing species in visible region, and has potential to change the optical property of cloud. On the basis of the measurements conducted at a mountain located in the suburb of Tokyo Metropolitan area, Japan, some insights on the scavenging of particulate elemental carbon into cloud droplet will be presented

Oxalate metal complexes in aerosol particles: implications for the hygroscopicity of oxalate-containing particles

Directory of Open Access Journals (Sweden)

T. Furukawa

2011-05-01

Full Text Available Atmospheric aerosols have both a direct and an indirect cooling effect that influences the radiative balance at the Earth's surface. It has been estimated that the degree of cooling is large enough to weaken the warming effect of carbon dioxide. Among the cooling factors, secondary organic aerosols (SOA play an important role in the solar radiation balance in the troposphere as SOA can act as cloud condensation nuclei (CCN and extend the lifespan of clouds because of their high hygroscopic and water soluble nature. Oxalic acid is an important component of SOA, and is produced via several formation pathways in the atmosphere. However, it is not certain whether oxalic acid exists as free oxalic acid or as metal oxalate complexes in aerosols, although there is a marked difference in their solubility in water and their hygroscopicity. We employed X-ray absorption fine structure spectroscopy to characterize the calcium (Ca and zinc (Zn in aerosols collected at Tsukuba in Japan. Size-fractionated aerosol samples were collected for this purpose using an impactor aerosol sampler. It was shown that 10–60% and 20–100% of the total Ca and Zn in the finer particles (<2.1 μm were present as Ca and Zn oxalate complexes, respectively. Oxalic acid is hygroscopic and can thus increase the CCN activity of aerosol particles, while complexes with various polyvalent metal ions such as Ca and Zn are not hygroscopic, which cannot contribute to the increase of the CCN activity of aerosols. Based on the concentrations of noncomplexed and metal-complexed oxalate species, we found that most of the oxalic acid is present as metal oxalate complexes in the aerosols, suggesting that oxalic acid does not always increase the hygroscopicity of aerosols in the atmosphere. Similar results are expected for other dicarboxylic acids, such as malonic and succinic acids. Thus, it is advisable that the cooling effect of organic aerosols should be estimated by including the

Distinguishing Aerosol Impacts on Climate Over the Past Century

Energy Technology Data Exchange (ETDEWEB)

Koch, Dorothy; Menon, Surabi; Del Genio, Anthony; Ruedy, Reto; Alienov, Igor; Schmidt, Gavin A.

2008-08-22

Aerosol direct (DE), indirect (IE), and black carbon-snow albedo (BAE) effects on climate between 1890 and 1995 are compared using equilibrium aerosol-climate simulations in the Goddard Institute for Space Studies General Circulation Model coupled to a mixed layer ocean. Pairs of control(1890)-perturbation(1995) with successive aerosol effects allow isolation of each effect. The experiments are conducted both with and without concurrent changes in greenhouse gases (GHG's). A new scheme allowing dependence of snow albedo on black carbon snow concentration is introduced. The fixed GHG experiments global surface air temperature (SAT) changed -0.2, -1.0 and +0.2 C from the DE, IE, and BAE. Ice and snow cover increased 1.0% from the IE and decreased 0.3% from the BAE. These changes were a factor of 4 larger in the Arctic. Global cloud cover increased by 0.5% from the IE. Net aerosol cooling effects are about half as large as the GHG warming, and their combined climate effects are smaller than the sum of their individual effects. Increasing GHG's did not affect the IE impact on cloud cover, however they decreased aerosol effects on SAT by 20% and on snow/ice cover by 50%; they also obscure the BAE on snow/ice cover. Arctic snow, ice, cloud, and shortwave forcing changes occur mostly during summer-fall, but SAT, sea level pressure, and long-wave forcing changes occur during winter. An explanation is that aerosols impact the cryosphere during the warm-season but the associated SAT effect is delayed until winter.

Radioactive content in aerosols and rainwater

International Nuclear Information System (INIS)

Rodriguez Perestelo, N.; Lopez Perez, M.; Rodriguez, S.; Duarte, X.; Catalan, A.; Fernandez de Aldecoa, J. C.; Hernandez, J.

2013-01-01

The environmental radiological characterization of a place requires knowledge of the radioactive contents of its components, such as air (aerosol), rain, soil, etc ... Inhalation of radioactive aerosols in the air remains the main component of the total dose to the world population. This work focuses on its determination. (Author)

Design, demonstration and performance of a versatile electrospray aerosol generator for nanomaterial research and applications

International Nuclear Information System (INIS)

Jennerjohn, Nancy; Fung, David C; Hirakawa, Karen S; Hinds, William; Kennedy, Nola J; Eiguren-Fernandez, Arantzazu; Prikhodko, Sergey; Zavala-Mendez, Jose D

2010-01-01

Carbon nanotubes are difficult to aerosolize in a controlled manner. We present a method for generating aerosols not only of carbon nanotubes, but also of many reference and proprietary materials including quantum dots, diesel particulate matter, urban dust, and their mixtures, using electrospraying. This method can be used as a teaching tool, or as the starting point for advanced research, or to deliver nanomaterials in animal exposure studies. This electrospray system generates 180 μg of nanotubes per m 3 of carrier gas, and thus aerosolizes an occupationally relevant mass concentration of nanotubes. The efficiency achievable for single-walled carbon nanotubes is 9.4%. This system is simple and quick to construct using ordinary lab techniques and affordable materials. Since it is easy to replace soiled parts with clean ones, experiments on different types of nanomaterial can be performed back to back without contamination from previous experiments. In this paper, the design, fabrication, operation and characterization of our versatile electrospray method are presented. Also, the morphological changes that carbon nanotubes undergo as they make the transition from dry powders to aerosol particles are presented.

Transport of dust and anthropogenic aerosols across Alexandria, Egypt

Energy Technology Data Exchange (ETDEWEB)

El-Askary, H. [Chapman Univ., Orange, CA (United States). Dept. of Physics Computational Science and Engineering; Chapman Univ., Orange, CA (United States). Center of Excellence in Earth Observing; Alexandria Univ. (Egypt). Dept. of Environmental Sciences; National Authority for Remote Sensing and Space Science (NARSS), Cairo (Egypt); Farouk, R. [Alexandria Univ. (Egypt). Dept. of Environmental Sciences; Ichoku, C. [NASA Goddard Space Flight Center, Greenbelt, MD (United States). Climate and Radiation Branch; Kafatos, M. [Chapman Univ., Orange, CA (United States). Dept. of Physics Computational Science and Engineering; Chapman Univ., Orange, CA (United States). Center of Excellence in Earth Observing

2009-07-01

The flow of pollutants from Europe and desert dust to Europe from the Sahara desert both affects the air quality of the coastal regions of Egypt. As such, measurements from both ground and satellite observations assume great importance to ascertain the conditions and flow affecting the Nile Delta and the large city of Alexandria. We note that special weather conditions prevailing in the Mediterranean Sea result in a westerly wind flow pattern during spring and from North to South during the summer. Such flow patterns transport dust-loaded and polluted air masses from the Sahara desert and Europe, respectively, through Alexandria, and the Nile Delta in Egypt. We have carried out measurements acquired with a ground- based portable sun photometer (Microtops II) and the satellite-borne TERRA/Moderate Resolution Imaging Spectroradiometer (MODIS) sensor during the periods of October 1999-August 2001 and July 2002-September 2003. These measurements show a seasonal variability in aerosol optical depth (AOD) following these flow patterns. Maximum aerosol loadings accompanied by total precipitable water vapor (W) enhancements are observed during the spring and summer seasons. Pronounced changes have been observed in the Aangstroem exponent ({alpha}) derived from ground-based measurements over Alexandria (31.14 N, 29.59 E) during both dust and pollution periods. We have followed up the observations with a 3-day back-trajectories model to trace the probable sources and pathways of the air masses causing the observed aerosol loadings. We have also used other NASA model outputs to estimate the sea salt, dust, sulfates and black carbon AOD spatial distributions during different seasons. Our results reveal the probable source regions of these aerosol types, showing agreement with the trajectory and Aangstroem exponent analysis results. It is confirmed that Alexandria is subjected to different atmospheric conditions involving dust, pollution, mixed aerosols and clean sky. (orig.)

Tracing carbon fixation in phytoplankton—compound specific and total

NARCIS (Netherlands)

Grosse, J.; Van Breugel, P.; Boschker, H.T.S.

2015-01-01

Measurement of total primary production using 13C incorporation is a widely established tool. However, these bulk measurements lack information about the fate of fixed carbon: the production of major cellular compounds (carbohydrates, amino acids, fatty acids, and DNA/RNA) is affected by for

Aerosol characterization study using multi-spectrum remote sensing measurement techniques.

Energy Technology Data Exchange (ETDEWEB)

Glen, Crystal Chanea; Sanchez, Andres L.; Lucero, Gabriel Anthony; Schmitt, Randal L.; Johnson, Mark S.; Tezak, Matthew S; Servantes, Brandon Lee

2013-09-01

A unique aerosol flow chamber coupled with a bistatic LIDAR system was implemented to measure the optical scattering cross sections and depolarization ratio of common atmospheric particulates. Each of seven particle types (ammonium sulfate, ammonium nitrate, sodium chloride, potassium chloride, black carbon and Arizona road dust) was aged by three anthropogenically relevant mechanisms: 1. Sulfuric acid deposition, 2. Toluene ozonolysis reactions, and 3. m-Xylene ozonolysis reactions. The results of pure particle scattering properties were compared with their aged equivalents. Results show that as most particles age under industrial plume conditions, their scattering cross sections are similar to pure black carbon, which has significant impacts to our understanding of aerosol impacts on climate. In addition, evidence emerges that suggest chloride-containing aerosols are chemically altered during the organic aging process. Here we present the direct measured scattering cross section and depolarization ratios for pure and aged atmospheric particulates.

A study of the mixing state of black carbon in urban zone

Science.gov (United States)

Mallet, M.; Roger, J. C.; Despiau, S.; Putaud, J. P.; Dubovik, O.

2004-02-01

The knowledge of the mixing state of black carbon particle with other aerosol species is critical for adequate simulations of the direct radiative effect of black carbon particles and its effect on climate. This paper reports the investigation of the mixing state of black carbon aerosol in the urban zone. The study uses a combination of in situ and ground-based remote sensing observations conducted during the ESCOMPTE experiment, which took place in industrialized region in France in summer of 2001. The criteria we used for identifying mixing state relies on the known enhancement of absorption for aerosol composed by internal versus external mixtures of black carbon with weakly absorbing aerosol components. First, using in situ aerosol data, we performed Mie computations and reconstructed the single scattering albedo of aerosol for the two different mixing assumptions: black carbon mixed externally or internally with other aerosol species. Then, we compared the obtained values ωo,int and ωo,ext with the retrievals of ωo from independent AERONET Sun-photometric measurements. The aerosol single scattering albedo (ωo,aer.) derived from the AERONET photometer observations (with the mean value equal to 0.84 ± 0.04) was found to be close to ωo,ext reconstructed from in situ observation under assumptions of external mixture. This similarity between AERONET values and external mixture simulations was observed during all the days studied. Our conclusion on external mixture of black carbon aerosol with other particles in urban zone during ESCOMPTE (close to the pollution source) is coherent with observations made during other independent studies reported in a number of recent publications.

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

Science.gov (United States)

Mazurek, Monica A.; Cofer, Wesley R., III; Levine, Joel S.

1991-01-01

During the boreal forest burn studied, the ambient concentrations for the particle carbon smoke aerosol are highest for the full-fire burn conditions and vary significantly throughout the burn. Collection strategies must accordingly define ranges in the smoke aerosol concentrations produced. While the highest elemental C concentrations are observed during full-fire conditions, the great majority of smoke aerosol particles are in the form of organic C particles irrespective of fire temperature. The formation of organic C light-scattering particles was a significant process in the burn studied.

Aerosols, clouds and their climatic impacts

Energy Technology Data Exchange (ETDEWEB)

Kulmala, M; Laaksonen, A; Korhonen, P [Helsinki Univ. (Finland). Dept. of Physics

1996-12-31

The increasing atmospheric concentrations of greenhouse gases such as carbon dioxide and methane may drive a significant warming of the earth`s climate. However, a topic of more recent attention is the possibility that increased atmospheric concentrations of aerosol particles might drive a cooling of the planet. There are two distinct cooling mechanisms related to the enhanced concentrations of aerosol particles: the increase in the direct reflection of solar radiation (the direct effect), and the increase in cloud reflectivity caused by greater numbers of cloud condensation nuclei available (the indirect effect). Aerosols and clouds play a major role in the scattering and absorption of radiation in the Earth`s atmosphere. Locally the net effect can vary because of different kinds of surfaces. But according to measurements, the global net effect of clouds (and aerosols) on the atmosphere is net cooling and thus in opposition to the effect of greenhouse gases. The prediction of the future evolution of the climate involves substantial uncertainties. Clouds have a major effect on the radiation balance of the Earth and the prediction of amount and radiative properties of clouds is very difficult. Also the formation mechanisms and residence times of aerosol particles in the atmosphere involve large uncertainties. Thus the most serious difficulties arise in the area of the physics of clouds and aerosols

Aerosols, clouds and their climatic impacts

Energy Technology Data Exchange (ETDEWEB)

Kulmala, M.; Laaksonen, A.; Korhonen, P. [Helsinki Univ. (Finland). Dept. of Physics

1995-12-31

The increasing atmospheric concentrations of greenhouse gases such as carbon dioxide and methane may drive a significant warming of the earth`s climate. However, a topic of more recent attention is the possibility that increased atmospheric concentrations of aerosol particles might drive a cooling of the planet. There are two distinct cooling mechanisms related to the enhanced concentrations of aerosol particles: the increase in the direct reflection of solar radiation (the direct effect), and the increase in cloud reflectivity caused by greater numbers of cloud condensation nuclei available (the indirect effect). Aerosols and clouds play a major role in the scattering and absorption of radiation in the Earth`s atmosphere. Locally the net effect can vary because of different kinds of surfaces. But according to measurements, the global net effect of clouds (and aerosols) on the atmosphere is net cooling and thus in opposition to the effect of greenhouse gases. The prediction of the future evolution of the climate involves substantial uncertainties. Clouds have a major effect on the radiation balance of the Earth and the prediction of amount and radiative properties of clouds is very difficult. Also the formation mechanisms and residence times of aerosol particles in the atmosphere involve large uncertainties. Thus the most serious difficulties arise in the area of the physics of clouds and aerosols

Determination of total carbonates in soil archaeometry using a new pressure method with temperature compensation

Science.gov (United States)

Barouchas, Pantelis; Koulos, Vasilios; Melfos, Vasilios

2017-04-01

For the determination of total carbonates in soil archaeometry a new technique was applied using a multi-sensor philosophy, which combines simultaneous measurement of pressure and temperature. This technology is innovative and complies with EN ISO 10693:2013, ASTM D4373-02(2007) and Soil Science Society of America standard test methods for calcium carbonate content in soils and sediments. The total carbonates analysis is based on a pressure method that utilizes the FOGII Digital Soil CalcimeterTM, which is a portable apparatus. The total carbonate content determined by treating a 1.000 g (+/- 0.001 g) dried sample specimens with 6N hydrochloric acid (HCL) reagent grade, in an enclosed reaction vessel. Carbon dioxide gas evolved during the reaction between the acid and carbonate fraction of the specimen, was measured by the resulting pressure generated, taking in account the temperature conditions during the reaction. Prior to analysis the procedure was validated with Sand/Soil mixtures from BIPEA proficiency testing program with soils of different origins. For applying this new method in archaeometry a total number of ten samples were used from various rocks which are related with cultural constructions and implements in Greece. They represent a large range of periods since the Neolithic times, and were selected because there was an uncertainty about their accurate mineralogical composition especially regarding the presence of carbonate minerals. The results were compared to the results from ELTRA CS580 inorganic carbon analyzer using an infrared cell. The determination of total carbonates for 10 samples from different ancient sites indicated a very good correlation (R2 >0.97) between the pressure method with temperature compensation and the infrared method. The proposed method is quickly and accurate in archaeometry and can replace easily other techniques for total carbonates testing. The FOGII Digital Soil CalcimeterTM is portable and easily can be carried for

Single-particle characterization of summertime Antarctic aerosols collected at King George Island using quantitative energy-dispersive electron probe X-ray microanalysis and attenuated total reflection Fourier transform-infrared imaging techniques.

Science.gov (United States)

Maskey, Shila; Geng, Hong; Song, Young-Chul; Hwang, Heejin; Yoon, Young-Jun; Ahn, Kang-Ho; Ro, Chul-Un

2011-08-01

Single-particle characterization of Antarctic aerosols was performed to investigate the impact of marine biogenic sulfur species on the chemical compositions of sea-salt aerosols in the polar atmosphere. Quantitative energy-dispersive electron probe X-ray microanalysis was used to characterize 2900 individual particles in 10 sets of aerosol samples collected between March 12 and 16, 2009 at King Sejong Station, a Korean scientific research station located at King George Island in the Antarctic. Two size modes of particles, i.e., PM(2.5-10) and PM(1.0-2.5), were analyzed, and four types of particles were identified, with sulfur-containing sea-salt particles being the most abundant, followed by genuine sea-salt particles without sulfur species, iron-containing particles, and other species including CaCO(3)/CaMg(CO(3))(2), organic carbon, and aluminosilicates. When a sulfur-containing sea-salt particle showed an atomic concentration ratio of sulfur to sodium of >0.083 (seawater ratio), it is regarded as containing nonsea-salt sulfate (nss-SO(4)(2-)) and/or methanesulfonate (CH(3)SO(3)(-)), which was supported by attenuated total reflection Fourier transform-infrared imaging measurements. These internal mixture particles of sea-salt/CH(3)SO(3)(-)/SO(4)(2-) were very frequently encountered. As nitrate-containing particles were not encountered, and the air-masses for all of the samples originated from the Pacific Ocean (based on 5-day backward trajectories), the oxidation of dimethylsulfide (DMS) emitted from phytoplanktons in the ocean is most likely to be responsible for the formation of the mixed sea-salt/CH(3)SO(3)(-)/SO(4)(2-) particles.

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

Chemical compositions, sources and evolution processes of the submicron aerosols in Nanjing, China during wintertime

Science.gov (United States)

Wu, Y.; He, Y.; Ge, X.; Wang, J.; Yu, H.; Chen, M.

2016-12-01

Elevated atmospheric particulate matter pollution is one of the most significant environmental issues in the Yangtze River Delta (YRD), China. Thus it is important to unravel the characteristics, sources and evolution processes of the ambient aerosols in order to improve the air quality. In this study, we report the real-time monitoring results on submicron aerosol particles (PM1) in suburban Nanjing during wintertime of 2015, using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS). This instrument allows the fast measurement of refractory black carbon simultaneously with other aerosol components. Results show that organics was on average the most abundant species of PM1 (25.9%), but other inorganic species, such as nitrate (23.7%) and sulfate (23.3%) also comprised large mass fractions. As the sampling site is heavily influenced by various sources including industrial, traffic and other anthropogenic emissions, etc., six organic aerosol (OA) factors were identified from Positive matrix factorization (PMF) analysis of the SP-AMS OA mass spectra. These factors include three primary OA factors - a hydrocarbon-like OA, an industry-related OA (IOA) and a cooking OA (COA), and three secondary OA factors, i.e., a local OOA (LSOA), a semi-volatile OOA (SV-OOA) and a low-volatility OOA (LV-OOA). Overall, the primary organic aerosol (POA) (HOA, IOA and COA) dominated the total OA mass. Behaviors and evolution processes of these OA factors will be discussed in combining with the other supporting data.

Particulate carbon in the atmosphere

International Nuclear Information System (INIS)

Surakka, J.

1992-01-01

Carbonaceous aerosols are emitted to the atmosphere in combustion processes. Carbon particles are very small and have a long residence time in the air. Black Carbon, a type of carbon aerosol, is a good label when transport of combustion emissions in the atmosphere is studied. It is also useful tool in air quality studies. Carbon particles absorb light 6.5 to 8 times stronger than any other particulate matter in the air. Their effect on decreasing visibility is about 50 %. Weather disturbances are also caused by carbon emissions e.g. in Kuwait. Carbon particles have big absorption surface and capacity to catalyze different heterogenous reactions in air. Due to their special chemical and physical properties particulate carbon is a significant air pollution specie, especially in urban air. Average particulate carbon concentration of 5.7 μg/m 2 have been measured in winter months in Helsinki

Development and first application of an Aerosol Collection Module (ACM) for quasi online compound specific aerosol measurements

Science.gov (United States)

Hohaus, Thorsten; Kiendler-Scharr, Astrid; Trimborn, Dagmar; Jayne, John; Wahner, Andreas; Worsnop, Doug

2010-05-01

Atmospheric aerosols influence climate and human health on regional and global scales (IPCC, 2007). In many environments organics are a major fraction of the aerosol influencing its properties. Due to the huge variety of organic compounds present in atmospheric aerosol current measurement techniques are far from providing a full speciation of organic aerosol (Hallquist et al., 2009). The development of new techniques for compound specific measurements with high time resolution is a timely issue in organic aerosol research. Here we present first laboratory characterisations of an aerosol collection module (ACM) which was developed to allow for the sampling and transfer of atmospheric PM1 aerosol. The system consists of an aerodynamic lens system focussing particles on a beam. This beam is directed to a 3.4 mm in diameter surface which is cooled to -30 °C with liquid nitrogen. After collection the aerosol sample can be evaporated from the surface by heating it to up to 270 °C. The sample is transferred through a 60cm long line with a carrier gas. In order to test the ACM for linearity and sensitivity we combined it with a GC-MS system. The tests were performed with octadecane aerosol. The octadecane mass as measured with the ACM-GC-MS was compared versus the mass as calculated from SMPS derived total volume. The data correlate well (R2 0.99, slope of linear fit 1.1) indicating 100 % collection efficiency. From 150 °C to 270 °C no effect of desorption temperature on transfer efficiency could be observed. The ACM-GC-MS system was proven to be linear over the mass range 2-100 ng and has a detection limit of ~ 2 ng. First experiments applying the ACM-GC-MS system were conducted at the Jülich Aerosol Chamber. Secondary organic aerosol (SOA) was formed from ozonolysis of 600 ppbv of b-pinene. The major oxidation product nopinone was detected in the aerosol and could be shown to decrease from 2 % of the total aerosol to 0.5 % of the aerosol over the 48 hours of

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.

Particle-Resolved Modeling of Aerosol Mixing State in an Evolving Ship Plume

Science.gov (United States)

Riemer, N. S.; Tian, J.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

2011-12-01

The aerosol mixing state is important since it impacts the particles' optical and CCN properties and thereby their climate impact. It evolves continuously during the particles' residence time in the atmosphere as a result of coagulation with other particles and condensation of secondary aerosol species. This evolution is challenging to represent in traditional aerosol models since they require the representation of a multi-dimensional particle distribution. While modal or sectional aerosol representations cannot practically resolve the aerosol mixing state for more than a few species, particle-resolved models store the composition of many individual aerosol particles directly. They thus sample the high-dimensional composition state space very efficiently and so can deal with tens of species, fully resolving the mixing state. Here we use the capabilities of the particle-resolved model PartMC-MOSAIC to simulate the evolution of particulate matter emitted from marine diesel engines and compare the results to aircraft measurements made in the English Channel in 2007 as part of the European campaign QUANTIFY. The model was initialized with values of gas concentrations and particle size distributions and compositions representing fresh ship emissions. These values were obtained from a test rig study in the European project HERCULES in 2006 using a serial four-stroke marine diesel engine operating on high-sulfur heavy fuel oil. The freshly emitted particles consisted of sulfate, black carbon, organic carbon and ash. We then tracked the particle population for several hours as it evolved undergoing coagulation, dilution with the background air, and chemical transformations in the aerosol and gas phase. This simulation was used to compute the evolution of CCN properties and optical properties of the plume on a per-particle basis. We compared our results to size-resolved data of aged ship plumes from the QUANTIFY Study in 2007 and showed that the model was able to reproduce

Brown Carbon and Black Carbon in the Smoky Atmosphere during Boreal Forest Fires

Science.gov (United States)

Gorchakov, G. I.; Karpov, A. V.; Pankratova, N. V.; Semoutnikova, E. G.; Vasiliev, A. V.; Gorchakova, I. A.

2017-12-01

We have investigated the variability of smoke aerosol absorbing ability with variations in the content of brown carbon (BrC) and black carbon (BC). Using monitoring data on radiative characteristics of smoke aerosol at AERONET stations and the spatial distribution of aerosol optical depth (AOD) obtained by the MODIS spectrometer ( Terra satellite), we have detected large-scale smokes during boreal forest fires in Russia and Canada (1995-2012). The spatial distribution (50°-70° N, 95°-125° W) and temporal variability (at AERONET station Fort McMurray) of AOD during the smoking of a part of Canada in July 2012 have been analyzed. AOD probability distributions for July 14-18, 2012, and an estimate of aerosol radiative forcing of smoke aerosol at the upper boundary of the atmosphere have been obtained. We have proposed a technique for the diagnostics of BrC and BC in smoke aerosol particles from the spectral dependence of the imaginary part of the refractive index. At a wavelength of 440 nm, the contributions of BrC and BC to the smokeaerosol absorbing abitity can be comparable in magnitude. In many cases, the absorption spectra of smoke aerosol can be adequately approximated by either power or exponential functions. The presence of BrC in smoke-aerosol particles highly extends the variety of observed absorption spectra in a smoky atmosphere and spectral dependences of single scattering albedo. In the spectral range of 440-1020 nm, the radiative characteristics of smoke aerosol are largely contributed by its fine mode.

Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

Science.gov (United States)

Lohmann, U.; Hoose, C.

2009-11-01

Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

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.;

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.

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

Science.gov (United States)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

Continuous flame aerosol synthesis of carbon-coated nano-LiFePO4 for Li-ion batteries

Science.gov (United States)

Waser, Oliver; Büchel, Robert; Hintennach, Andreas; Novák, Petr; Pratsinis, Sotiris E.

2013-01-01

Core-shell, nanosized LiFePO4-carbon particles were made in one step by scalable flame aerosol technology at 7 g/h. Core LiFePO4 particles were made in an enclosed flame spray pyrolysis (FSP) unit and were coated in-situ downstream by auto thermal carbonization (pyrolysis) of swirl-fed C2H2 in an O2-controlled atmosphere. The formation of acetylene carbon black (ACB) shell was investigated as a function of the process fuel-oxidant equivalence ratio (EQR). The core-shell morphology was obtained at slightly fuel-rich conditions (1.0 < EQR < 1.07) whereas segregated ACB and LiFePO4 particles were formed at fuel-lean conditions (0.8 < EQR < 1). Post-annealing of core-shell particles in reducing environment (5 vol% H2 in argon) at 700 °C for up to 4 hours established phase pure, monocrystalline LiFePO4 with a crystal size of 65 nm and 30 wt% ACB content. Uncoated LiFePO4 or segregated LiFePO4-ACB grew to 250 nm at these conditions. Annealing at 800 °C induced carbothermal reduction of LiFePO4 to Fe2P by ACB shell consumption that resulted in cavities between carbon shell and core LiFePO4 and even slight LiFePO4 crystal growth but better electrochemical performance. The present carbon-coated LiFePO4 showed superior cycle stability and higher rate capability than the benchmark, commercially available LiFePO4. PMID:23407817

Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

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B. Croft

2010-02-01

Full Text Available A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90% scavenged by cloud nucleation processes for all aerosol species, except for dust (50%. The aerosol number scavenged is primarily (>90% attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20–30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds

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

AEROSOL VARIABILITY OBSERVED WITH RPAS

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B. Altstädter

2013-08-01

Full Text Available To observe the origin, vertical and horizontal distribution and variability of aerosol particles, and especially ultrafine particles recently formed, we plan to employ the remotely piloted aircraft system (RPAS Carolo-P360 "ALADINA" of TU Braunschweig. The goal of the presented project is to investigate the vertical and horizontal distribution, transport and small-scale variability of aerosol particles in the atmospheric boundary layer using RPAS. Two additional RPAS of type MASC of Tübingen University equipped with turbulence instrumentation add the opportunity to study the interaction of the aerosol concentration with turbulent transport and exchange processes of the surface and the atmosphere. The combination of different flight patterns of the three RPAS allows new insights in atmospheric boundary layer processes. Currently, the different aerosol sensors are miniaturized at the Leibniz Institute for Tropospheric Research, Leipzig and together with the TU Braunschweig adapted to fit into the RPAS. Moreover, an additional meteorological payload for measuring temperature, humidity and turbulence properties is constructed by Tübingen University. Two condensation particle counters determine the total aerosol number with a different lower detection threshold in order to investigate the horizontal and vertical aerosol variability and new particle formation (aerosol particles of some nm diameter. Further the aerosol size distribution in the range from about 0.300 to ~5 μm is given by an optical particle counter.

Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: a study on freshly formed and aged biogenic SOA

Science.gov (United States)

Gkatzelis, Georgios I.; Tillmann, Ralf; Hohaus, Thorsten; Müller, Markus; Eichler, Philipp; Xu, Kang-Ming; Schlag, Patrick; Schmitt, Sebastian H.; Wegener, Robert; Kaminski, Martin; Holzinger, Rupert; Wisthaler, Armin; Kiendler-Scharr, Astrid

2018-03-01

An intercomparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic secondary organic aerosol (BSOA) formation and aging at the atmosphere simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction chamber). Three different aerosol sampling techniques - the aerosol collection module (ACM), the chemical analysis of aerosol online (CHARON) and the collection thermal-desorption unit (TD) were connected to proton transfer reaction time-of-flight mass spectrometers (PTR-ToF-MSs) to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS). The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene-limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine). The SOA was subsequently aged by photo-oxidation, except for limonene SOA, which was aged by NO3 oxidation. Despite significant differences in the aerosol collection and desorption methods of the PTR-based techniques, the determined chemical composition, i.e. the same major contributing signals, was found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD provided additional information on the volatility of individual compounds and showed relatively good agreement. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied within 80 ± 10, 51 ± 5 and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen-to-carbon ratios (O : C) obtained by AMS showed that all PTR-based techniques observed lower O : C ratios, indicating a loss of molecular oxygen either during aerosol sampling or detection. The differences in total

Radiocarbon variability of fatty acids in semi-urban aerosol samples

International Nuclear Information System (INIS)

Matsumoto, Kohei; Uchida, Masao; Kawamura, Kimitaka; Shibata, Yasuyuki; Morita, Masatoshi

2004-01-01

We analyzed radiocarbon and the stable carbon isotope ratio for individual monocarboxylic (fatty) acids in an aerosol sample (QFF 2138) and compared the results with data of the aerosol sample taken in another year. The fatty acid concentration distribution of aerosol sample QFF 2138 showed a bimodal pattern with maxima at C 16 and C 26 . Stable carbon isotope ratios of the fatty acids ranged from -30.8 per mille to -23.0 per mille which indicates the animal and/or marine algae origins for C 16 -C 19 fatty acids and mainly terrestrial C 3 plant origins for C >20 fatty acids. Δ 14 C values for fatty acids ranged from -89.7 per mille to +83.5 per mille. Compared with QFF1969, we found that the Δ 14 C values of fatty acids exhibited a wide diversity and Δ 14 C values for each fatty acid in QFF 2138 were largely different from those of QFF 1969

Laboratory Measurements of Mass Specific Absorption Spectra for Suites of Black Carbon-like, Biomass Burning and Mineral Dust Aerosols

Science.gov (United States)

Radney, J.; Zangmeister, C.

2017-12-01

Light-absorbing atmospheric aerosols can be grouped into three categories: black carbon (BC), brown carbon (BrC) or mineral dust (MD). In many cases, the absorption of these species is best quantified using a mass-specific absorption cross section (MAC) since the particles are in the Rayleigh regime (BC) or optically thin (BrC and MD); notably, MAC values are both traceable to the SI and transferrable between photoacoustic spectroscopy and filter-based absorption measurements. Here, we present laboratory measurements of MAC for all three light-absorbing aerosol classes. Particles were size- and mass-selected using a differential mobility analyzer and aerosol particle mass analyzer, respectively, with absorption coefficients (αabs) and number concentrations (N) being measured by a broadband photoacoustic spectrometer and condensation particle counter, respectively. This suite of instrumentation allows for direct quantification of MAC from the measured parameters (MAC = αabs/Nmp). Further, the measurements contained > 8 data points spanning λ = 405 nm to 840 nm allowing for spectral curvatures (i.e. the Absorption Angstrom Exponent or AAE) to be fit from many data points versus the more common 2-point interpolations. For the carbonaceous, BC-like aerosols - five samples generated from flames, spark discharge soot (i.e. fullerene soot), graphene, reduced graphene oxide (rGO), and fullerene (C60) - we found: 1) measured MAC ranged between 2.4 m2 g-1 and 8.6 m2 g-1 at λ = 550 nm, 2) most AAEs ranged between 0.5 and 1.3; C60 AAE was 7.5 ± 0.9 and 3) MAC spectra were dependent on fuel type and formation conditions. For BrC particles generated from smoldering combustion of 3 hardwood (Oak, Hickory and Mesquite) and 3 softwood species (Western redcedar, Blue spruce and Baldcypress), we found: 1) median MAC values ranged from 1.4 x 10-2 m2 g-1 to 7.9 x 10-2 m2 g-1 at λ = 550 nm, 2) AAE values ranged between 3.5 and 6.2, and 3) Oak, Western redcedar and Blue spruce

Hygroscopic growth of water soluble organic carbon isolated from atmospheric aerosol collected at US national parks and Storm Peak Laboratory

Science.gov (United States)

Taylor, Nathan F.; Collins, Don R.; Lowenthal, Douglas H.; McCubbin, Ian B.; Gannet Hallar, A.; Samburova, Vera; Zielinska, Barbara; Kumar, Naresh; Mazzoleni, Lynn R.

2017-02-01

Due to the atmospheric abundance and chemical complexity of water soluble organic carbon (WSOC), its contribution to the hydration behavior of atmospheric aerosol is both significant and difficult to assess. For the present study, the hygroscopicity and CCN activity of isolated atmospheric WSOC particulate matter was measured without the compounding effects of common, soluble inorganic aerosol constituents. WSOC was extracted with high purity water from daily high-volume PM2.5 filter samples and separated from water soluble inorganic constituents using solid-phase extraction. The WSOC filter extracts were concentrated and combined to provide sufficient mass for continuous generation of the WSOC-only aerosol over the combined measurement time of the tandem differential mobility analyzer and coupled scanning mobility particle sizer-CCN counter used for the analysis. Aerosol samples were taken at Great Smoky Mountains National Park during the summer of 2006 and fall-winter of 2007-2008; Mount Rainier National Park during the summer of 2009; Storm Peak Laboratory (SPL) near Steamboat Springs, Colorado, during the summer of 2010; and Acadia National Park during the summer of 2011. Across all sampling locations and seasons, the hygroscopic growth of WSOC samples at 90 % RH, expressed in terms of the hygroscopicity parameter, κ, ranged from 0.05 to 0.15. Comparisons between the hygroscopicity of WSOC and that of samples containing all soluble materials extracted from the filters implied a significant modification of the hydration behavior of inorganic components, including decreased hysteresis separating efflorescence and deliquescence and enhanced water uptake between 30 and 70 % RH.

Spatial distribution of aerosol black carbon over India during pre-monsoon season

Science.gov (United States)

Beegum, S. Naseema; Moorthy, K. Krishna; Babu, S. Suresh; Satheesh, S. K.; Vinoj, V.; Badarinath, K. V. S.; Safai, P. D.; Devara, P. C. S.; Singh, Sacchidanand; Vinod; Dumka, U. C.; Pant, P.

Aerosol black carbon (BC) mass concentrations ([BC]), measured continuously during a mutli-platform field experiment, Integrated Campaign for Aerosols gases and Radiation Budget (ICARB, March-May 2006), from a network of eight observatories spread over geographically distinct environments of India, (which included five mainland stations, one highland station, and two island stations (one each in Arabian Sea and Bay of Bengal)) are examined for their spatio-temporal characteristics. During the period of study, [BC] showed large variations across the country, with values ranging from 27 μg m -3 over industrial/urban locations to as low as 0.065 μg m -3 over the Arabian Sea. For all mainland stations, [BC] remained high compared to highland as well as island stations. Among the island stations, Port Blair (PBR) had higher concentration of BC, compared to Minicoy (MCY), implying more absorbing nature of Bay of Bengal aerosols than Arabian Sea. The highland station Nainital (NTL), in the central Himalayas, showed low values of [BC], comparable or even lower than that of the island station PBR, indicating the prevalence of cleaner environment over there. An examination of the changes in the mean temporal features, as the season advances from winter (December-February) to pre-monsoon (March-May), revealed that: (a) Diurnal variations were pronounced over all the mainland stations, with an afternoon low and a nighttime high; (b) At the islands, the diurnal variations, though resembled those over the mainlands, were less pronounced; and (c) In contrast to this, highland station showed an opposite pattern with an afternoon high and a late night or early morning low. The diurnal variations at all stations are mainly caused by the dynamics of local Atmospheric Boundary Layer (ABL). At the entire mainland as well as island stations (except HYD and DEL), [BC] showed a decreasing trend from January to May. This is attributed to the increased convective mixing and to the

Constraining Absorption of Organic Aerosol from Biomass Burning with Observations

Science.gov (United States)

Feng, Y.; Liu, X.

2014-12-01

Biomass burning emissions contribute to a large fraction of global organic aerosol (OA) emissions. In most models, radiative forcing of black carbon (BC) and OA from biomass burning offsets each other to give a small or close to zero total forcing, i.e., an estimate of 0 (-0.2 to +0.2) W m-2 by IPCC-AR5. Recent observational and modeling studies have shown the absorbing part of OA, referred to as "brown" carbon (BrC), to be a significant source of direct absorption of solar radiation thus positive forcing, in particular over regions dominated by biomass burning and biofuel emissions. Here we implement optical treatment for the BrC absorption in the CESM1/CAM5 model, and compare the calculated aerosol spectral absorption with ground-based AERONET and DOE/ARM observations. In this version of CAM5, biomass burning and biofuel OA are treated separately from fossil fuel OA with different imaginary refractive index. Because the absorption of BrC is highly variable and uncertain depending on source, aging, and mixing state, sensitivity studies of BrC refractive index parameterized by fuel type and ratio of BC to OA mass will be examined and the resulting uncertainty in the estimated forcing will be discussed. Preliminary results suggest the simulated wavelength dependence of aerosol absorption, as measured by the absorption Ångström exponent (AAE), increases from 0.9 for non-absorbing OA to 1.2 (or 1.0) for strongly (or moderately) absorbing BrC. The AAE calculated for the strongly absorbing BrC agrees with AERONET spectral observations at 440-870 nm over most regions but overpredicts for the open biomass burning-dominated South America and southern Africa, in which inclusion of moderately absorbing BrC exhibits better agreement.

Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

DEFF Research Database (Denmark)

Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.

2017-01-01

-NOx conditions, with OH scavengers and in the absence of seed particles. The excess of ozone and long residence time in the flow chamber ensured that virtually all α-pinene had reacted. Product SOA was collected on two sequential quartz filters. The filters were analysed offline by heating them stepwise from 100...... it is difficult to apply because neither the isotopic composition of aerosol precursors nor the fractionation of aerosol forming processes is well characterised. In this paper, SOA formation from ozonolysis of α-pinene - an important precursor and perhaps the best-known model system used in laboratory studies...... - was investigated using position-dependent and average determinations of 13C in α-pinene and advanced analysis of reaction products using thermal-desorption proton-transfer-reaction mass spectrometry (PTR-MS). The total carbon (TC) isotopic composition δ13C of the initial α-pinene was measured, and the δ13C...

Aerosol characterization in smoke plumes from a wetlands fire

International Nuclear Information System (INIS)

Woods, D.C.; Cofer, W.R. III; Levine, J.S.; Chuan, R.L.

1991-01-01

In this chapter, the authors present results from airborne measurements of aerosol mass loading, size distribution, and elemental composition obtained in a smoke plume from the burning of vegetation at a Florida wildlife refuge. These are important parameters in assessing the impact of biomass burning on the atmosphere. The results show that there was a high concentration of carbon-containing aerosols and salt crystals in the 0.1 μm to 0.2 μm size range, giving rise to a relatively strong fine particle size mode, during the hot flaming phase of the burning, compared to that during the smoldering phase, when a higher concentration of coarse particles were produced. They also found that the composition and morphology of the aerosols differed with size. They used the aerosol mass concentration along with CO 2 concentrations to calculate ratios or aerosol and CO 2 , which we found to be higher for the smoldering phase than for the flaming phase of combustion

Strong impacts on aerosol indirect effects from historical oxidant changes

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I. H. H. Karset

2018-06-01

Full Text Available Uncertainties in effective radiative forcings through aerosol–cloud interactions (ERFaci, also called aerosol indirect effects contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from −1.32 to −1.07 W m−2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3. The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

Investigation of size-fractionated urban aerosol and trace gases in Budapest by nuclear-related and other analytical techniques

International Nuclear Information System (INIS)

Salma, I.; Maenhaut, W.; Zemplen-Papp, E.; Bobvos, J.

1998-01-01

An air pollution study was conducted at two urban residential sites in Budapest (one representing the downtown, the other representing a wooded suburb) from 9 April till 17 May 1996. Size-fractionated aerosol samples were simultaneously collected on a daily basis, and meteorological conditions were recorded at both sampling sites. Stacked filter units (SFUs) with an upper size inlet cut-off were used as sampling device separating the urban aerosol into a coarse (about 10-2 μm equivalent aerodynamic diameter, EAD) and a fine ( 2 , SO 2 , CO and the total mass of the suspended particulate matter were measured every half hour at one of the sampling sites by commercial equipment. The SFU filters were analyzed by gravimetry for the total particle mass, by a light reflectance technique for black carbon, by particle-induced X-ray emission analysis and instrumental neutron activation analysis for elemental composition (in combination for up to 40-45 elements). The analytical results were used for characterizing the levels and the multi-elemental composition of the urban aerosol at both sampling sites and for both size fractions, for investigating the atmospheric concentrations and diurnal variation of some criteria pollutants, and for comparing the time-trends of aerosols and trace gases. Identification of the major source types of the aerosol fractions and trace gases, and assessment of the relative contribution from these sources are to be accomplished by multivariate receptor modeling. The present paper reports on the status of the air pollution study, and gives a discussion of the results