Transport of breeder reactor-fire-generated sodium oxide aerosols for building-wake-dominated meteorology

Energy Technology Data Exchange (ETDEWEB)

Fields, D.E.; Cooper, A.C.; Miller, C.W.

1987-02-01

This report describes the methodology used and results obtained in efforts to estimate the sodium aerosol concentrations at air intake ports of a liquid-metal cooled, fast-breeder nuclear reactor. An earlier version of this methodology has been previously discussed (Fields and Miller, 1985). A range of wind speeds from 2 to 10 m/s is assumed, and an effort is made to include building wake effects which, in many cases, dominate the dispersal of aerosols near buildings. For relatively small release rates, on the order of 1 to 10 kg/s, the plume rise is small and estimates of aerosol concentrations are derived using the methodology of Wilson and Britter (1982), which describes releases from surface vents. For release rates on the order of 100 kg/s much higher release velocities are expected, and plume rise is considered. An effective increase in release height is computed using the Split-H methodology with a parameterization suggested by Ramsdell (1983), and the release source strength is transformed to rooftop level. Evaluation of the acute release aerosol concentration is then based on the methodology for releases from a surface release of this transformed source strength. For a horizontal release, a methodology is developed to chart the plume path as a function of release and site meteorology parameters. Results described herein must be regarded as maximum aerosol concentrations, based on models derived from generic wind tunnel studies. More accurate and site-specific results may be obtained through wind tunnel simulations and through simulating emissions from release points other than those assumed here.

Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC Project

Directory of Open Access Journals (Sweden)

C. A. Brock

2011-03-01

Full Text Available We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion.

Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day⁻¹ between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB

Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol

Directory of Open Access Journals (Sweden)

J. G. Slowik

2011-03-01

Full Text Available As part of the BAQS-Met 2007 field campaign, Aerodyne time-of-flight aerosol mass spectrometers (ToF-AMS were deployed at two sites in southwestern Ontario from 17 June to 11 July 2007. One instrument was located at Harrow, ON, a rural, agriculture-dominated area approximately 40 km southeast of the Detroit/Windsor/Windsor urban area and 5 km north of Lake Erie. The second instrument was located at Bear Creek, ON, a rural site approximately 70 km northeast of the Harrow site and 50 km east of Detroit/Windsor. Positive matrix factorization analysis of the combined organic mass spectral dataset yields factors related to secondary organic aerosol (SOA, direct emissions, and a factor tentatively attributed to the reactive uptake of isoprene and/or condensation of its early generation reaction products. This is the first application of PMF to simultaneous AMS measurements at different sites, an approach which allows for self-consistent, direct comparison of the datasets. Case studies are utilized to investigate processing of SOA from (1 fresh emissions from Detroit/Windsor and (2 regional aerosol during periods of inter-site flow. A strong correlation is observed between SOA/excess CO and photochemical age as represented by the NO_x/NO_y ratio for Detroit/Windsor outflow. Although this correlation is not evident for more aged air, measurements at the two sites during inter-site transport nevertheless show evidence of continued atmospheric processing by SOA production. However, the rate of SOA production decreases with airmass age from an initial value of ~10.1 μg m⁻³ ppmv_CO⁻¹ h⁻¹ for the first ~10 h of plume processing to near-zero in an aged airmass (i.e. after several days. The initial SOA production rate is comparable to the observed rate in Mexico City over similar timescales.

Chemical composition, sources and evolution processes of aerosol at an urban site in Yangtze River Delta, China during wintertime

Science.gov (United States)

Zhang, Yunjiang; Tang, Lili; Yu, Hongxia; Wang, Zhuang; Sun, Yele; Qin, Wei; Chen, Wentai; Chen, Changhong; Ding, Aijun; Wu, Jing; Ge, Shun; Chen, Cheng; Zhou, Hong-cang

2015-12-01

To investigate the composition, sources and evolution processes of submicron aerosol during wintertime, a field experiment was conducted during December 1-31, 2013 in urban Nanjing, a megacity in Yangtze River Delta of China. Non-refractory submicron aerosol (NR-PM1) species were measured with an Aerodyne Aerosol Chemical Speciation Monitor. NR-PM1 is dominated by secondary inorganic aerosol (55%) and organic aerosol (OA, 42%) during haze periods. Six OA components were identified by positive matrix factorization of the OA mass spectra. The hydrocarbon-like OA and cooking-related OA represent the local traffic and cooking sources, respectively. A highly oxidized factor related to biomass burning OA accounted for 15% of the total OA mass during haze periods. Three types of oxygenated OA (OOA), i.e., a less-oxidized OOA (LO-OOA), a more-oxidized OOA (MO-OOA), and a low-volatility OOA (LV-OOA), were identified. LO-OOA is likely associated with fresh urban secondary OA. MO-OOA likely represents photochemical products showing a similar diurnal cycle to nitrate with a pronounced noon peak. LV-OOA appears to be a more oxidized factor with a pronounced noon peak. The OA composition is dominated by secondary species, especially during haze events. LO-OOA, MO-OOA and LV-OOA on average account for 11%, (18%), 24% (21%) and 23% (18%) of the total OA mass for the haze (clean) periods respectively. Analysis of meteorological influence suggested that regional transport from the northern and southeastern areas of the city is responsible for large secondary and low-volatility aerosol formation.

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

Science.gov (United States)

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

2007-12-01

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

Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

Science.gov (United States)

Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

2017-06-01

Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

Genetic Dominance & Cellular Processes

Science.gov (United States)

Seager, Robert D.

2014-01-01

In learning genetics, many students misunderstand and misinterpret what "dominance" means. Understanding is easier if students realize that dominance is not a mechanism, but rather a consequence of underlying cellular processes. For example, metabolic pathways are often little affected by changes in enzyme concentration. This means that…

Processing of Unsaturated Organic Acid Aerosols by Ozone

Science.gov (United States)

Aloisio, S.; Donaldson, D. J.; Eliason, T. L.; Cziczo, D.; Vaida, V.

2002-05-01

We present results of in-situ studies of the oxidative "processing" of organic aerosols composed of unsaturated organic compounds. Aerosol samples of 2-octenoic acid and undecylenic acid were exposed to approx. 10 mbar ozone in a room temperature, atmospheric pressure flow tube reactor. In-situ spectroscopic probing of the reaction mixture, as well as GC-MS analysis of the flow tube effluent, shows evidence of efficient oxidation of double bonds in the organic species, with production of gas-phase and aerosol phase ozonolysis products.

Atmospheric aerosol system: An overview

International Nuclear Information System (INIS)

Prospero, J.M.; Charlson, R.J.; Mohnen, V.; Jaenicke, R.; Delany, A.C.; Moyers, J.; Zoller, W.; Rahn, K.

1983-01-01

Aerosols could play a critical role in many processes which impact on our lives either indirectly (e.g., climate) or directly (e.g., health). However, our ability to assess these possible impacts is constrained by our limited knowledge of the physical and chemical properties of aerosols, both anthropogenic and natural. This deficiency is attributable in part to the fact that aerosols are the end product of a vast array of chemical and physical processes. Consequently, the properties of the aerosol can exhibit a great deal of variability in both time and space. Furthermore, most aerosol studies have focused on measurements of a single aerosol characteristic such as composition or size distribution. Such information is generally not useful for the assessment of impacts because the degree of impact may depend on the integral properties of the aerosol, for example, the aerosol composition as a function of particle size. In this overview we discuss recent work on atmospheric aerosols that illustrates the complex nature of the aerosol chemical and physical system, and we suggest strategies for future research. A major conclusion is that man has had a great impact on the global budgets of certain species, especially sulfur and nitrogen, that play a dominant role in the atmospheric aerosol system. These changes could conceivably affect climate. Large-scale impacts are implied because it has recently been demonstrated that natural and pollutant aerosol episodes can be propagated over great distances. However, at present there is no evidence linking anthropogenic activities with a persistent increase in aerosol concentrations on a global scale. A major problem in assessing man's impact on the atmospheric aerosol system and on global budgets is the absence of aerosol measurements in remote marine and continental areas

A simplified model of aerosol removal by natural processes in reactor containments

Energy Technology Data Exchange (ETDEWEB)

Powers, D.A.; Washington, K.E.; Sprung, J.L. [Sandia National Labs., Albuquerque, NM (United States); Burson, S.B. [Nuclear Regulatory Commission, Washington, DC (United States)

1996-07-01

Simplified formulae are developed for estimating the aerosol decontamination that can be achieved by natural processes in the containments of pressurized water reactors and in the drywells of boiling water reactors under severe accident conditions. These simplified formulae were derived by correlation of results of Monte Carlo uncertainty analyses of detailed models of aerosol behavior under accident conditions. Monte Carlo uncertainty analyses of decontamination by natural aerosol processes are reported for 1,000, 2,000, 3,000, and 4,000 MW(th) pressurized water reactors and for 1,500, 2,500, and 3,500 MW(th) boiling water reactors. Uncertainty distributions for the decontamination factors and decontamination coefficients as functions of time were developed in the Monte Carlo analyses by considering uncertainties in aerosol processes, material properties, reactor geometry and severe accident progression. Phenomenological uncertainties examined in this work included uncertainties in aerosol coagulation by gravitational collision, Brownian diffusion, turbulent diffusion and turbulent inertia. Uncertainties in aerosol deposition by gravitational settling, thermophoresis, diffusiophoresis, and turbulent diffusion were examined. Electrostatic charging of aerosol particles in severe accidents is discussed. Such charging could affect both the coagulation and deposition of aerosol particles. Electrostatic effects are not considered in most available models of aerosol behavior during severe accidents and cause uncertainties in predicted natural decontamination processes that could not be taken in to account in this work. Median (50%), 90 and 10% values of the uncertainty distributions for effective decontamination coefficients were correlated with time and reactor thermal power. These correlations constitute a simplified model that can be used to estimate the decontamination by natural aerosol processes at 3 levels of conservatism. Applications of the model are described.

Process for retention of iodine and aerosols during containment venting

International Nuclear Information System (INIS)

Eckardt, B.; Betz, R.; Greger, G.U.; Werner, K.D.

1990-05-01

A process for retention of the majority of aerosols and iodine during containment venting was optimized. For this purpose, sections of a two-stage process comprising a venturi scrubber and a metal-fiber filter demister were tested under containment venting conditions assumed to prevail during a hypothetical core - melt accident and optimized with a view to achieving high decontamination factors and loading capacity while minimizing the size of the process. The loading and retention tests performed in a scrubber operating pressure range between 1 and 10 bar, at temperatures from 50 to 200degC (also boiling pools) and in air and steam atmospheres. Under these unfavorable conditions for aerosol retention, the retention efficiencies were determined at various flow rates with soluble and non-soluble aerosols as well as gaseous iodine. The retention efficiencies for BaSO 4 , uranine and SnO 2 aerosols were determined to be 99.95% to 99.99% for venturi scrubbers with metal-fiber filter demister. The retention efficiency for elemental iodine was determined to be ≥99% including revolatization effects over a 24-hour operating period. The high loading capacity of the venturi scrubber unit was verified after process modifications with various aerosols. The use of full-scale process section together with the best possible simulation of containment venting conditions by the test parameters ensured that the results can be transferred to real venting equipment. The aim of ensuring the retention of the majority of the aerosol-borne activity and of elemental iodine activity and minimizing the process size was clearly achieved and verified by means of this optimized venting equipment under an extremely wide range of hypothetical core-melt accident conditions. (orig.) With 17 refs., 3 tabs., 35 annexes [de

Impacts of Combustion Conditions and Photochemical Processing on the Light Absorption of Biomass Combustion Aerosol.

Science.gov (United States)

Martinsson, J; Eriksson, A C; Nielsen, I Elbæk; Malmborg, V Berg; Ahlberg, E; Andersen, C; Lindgren, R; Nyström, R; Nordin, E Z; Brune, W H; Svenningsson, B; Swietlicki, E; Boman, C; Pagels, J H

2015-12-15

The aim was to identify relationships between combustion conditions, particle characteristics, and optical properties of fresh and photochemically processed emissions from biomass combustion. The combustion conditions included nominal and high burn rate operation and individual combustion phases from a conventional wood stove. Low temperature pyrolysis upon fuel addition resulted in "tar-ball" type particles dominated by organic aerosol with an absorption Ångström exponent (AAE) of 2.5-2.7 and estimated Brown Carbon contributions of 50-70% to absorption at the climate relevant aethalometer-wavelength (520 nm). High temperature combustion during the intermediate (flaming) phase was dominated by soot agglomerates with AAE 1.0-1.2 and 85-100% of absorption at 520 nm attributed to Black Carbon. Intense photochemical processing of high burn rate flaming combustion emissions in an oxidation flow reactor led to strong formation of Secondary Organic Aerosol, with no or weak absorption. PM1 mass emission factors (mg/kg) of fresh emissions were about an order of magnitude higher for low temperature pyrolysis compared to high temperature combustion. However, emission factors describing the absorption cross section emitted per kg of fuel consumed (m(2)/kg) were of similar magnitude at 520 nm for the diverse combustion conditions investigated in this study. These results provide a link between biomass combustion conditions, emitted particle types, and their optical properties in fresh and processed plumes which can be of value for source apportionment and balanced mitigation of biomass combustion emissions from a climate and health perspective.

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

Science.gov (United States)

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

2014-10-07

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

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

Science.gov (United States)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

What Controls the Vertical Distribution of Aerosol? Relationships Between Process Sensitivity in HadGEM3-UKCA and Inter-Model Variation from AeroCom Phase II

Science.gov (United States)

Kipling, Zak; Stier, Philip; Johnson, Colin E.; Mann, Graham W.; Bellouin, Nicolas; Bauer, Susanne E.; Bergman, Tommi; Chin, Mian; Diehl, Thomas; Ghan, Steven J.;

Climatic impacts of anthropogenic aerosols

Energy Technology Data Exchange (ETDEWEB)

Iversen, T. [Oslo Univ. (Norway)

1996-03-01

This paper was read at the workshop ``The Norwegian Climate and Ozone Research Programme`` held on 11-12 March 1996. Anthropogenic production of aerosols is mainly connected with combustion of fossil fuel. Measured by particulate mass, the anthropogenic sulphate production is the dominating source of aerosols in the Northern Hemisphere. Particles emitted in mechanical processes, fly ash etc. are less important because of their shorter atmospheric residence time. Possible climatological effects of anthropogenic aerosols are usually classified in two groups: direct and indirect. Direct effects are alterations of the radiative heating budget due to the aerosol particles in clear air. Indirect effects involve the interaction between particles and cloud processes. A simplified one-layer radiation model gave cooling in the most polluted mid-latitude areas and heating due to soot absorption in the Arctic. This differential trend in heating rates may have significant effects on atmospheric meridional circulations, which is important for the atmosphere as a thermodynamic system. Recently the description of sulphur chemistry in the hemispheric scale dispersion model has been improved and will be used in a model for Mie scattering and absorption

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

Science.gov (United States)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Enhancement of PM2.5 Concentrations by Aerosol-Meteorology Interactions Over China

Science.gov (United States)

Zhang, Xin; Zhang, Qiang; Hong, Chaopeng; Zheng, Yixuan; Geng, Guannan; Tong, Dan; Zhang, Yuxuan; Zhang, Xiaoye

2018-01-01

Aerosol-meteorology interactions can change surface aerosol concentrations via different mechanisms such as altering radiation budget or cloud microphysics. However, few studies investigated the impacts of different mechanisms on temporal and spatial distribution of PM2.5 concentrations over China. Here we used the fully coupled Weather Research and Forecasting model with online chemistry (WRF-Chem) to quantify the enhancement of PM2.5 concentrations by aerosol-meteorology feedback in China in 2014 for different seasons and separate the relative impacts of aerosol radiation interactions (ARIs) and aerosol-cloud interactions (ACIs). We found that ARIs and ACIs could increase population-weighted annual mean PM2.5 concentration over China by 4.0 μg/m3 and 1.6 μg/m3, respectively. We found that ARIs play a dominant role in aerosol-meteorology interactions in winter, while the enhancement of PM2.5 concentration by ARIs and ACIs is comparable in other three seasons. ARIs reduced the wintertime monthly mean wind speed and planetary boundary layer (PBL) height by up to 0.1 m/s and 160 m, respectively, but increased the relative humidity by up to 4%, leading to accumulation of pollutants within PBL. Also, ARIs reduced dry deposition velocity of aerosols by up to 20%, resulting in an increase in PM2.5 lifetime and concentrations. ARIs can increase wintertime monthly mean surface PM2.5 concentration by a maximum of 30 μg/m3 in Sichuan Basin. ACIs can also increase PM2.5 concentration with more significant impacts in wet seasons via reduced wet scavenging and enhanced in-cloud chemistry. Dominant processes in PM2.5 enhancement are also clarified in different seasons. Results show that physical process is more important than chemical processes in winter in ARIs, while chemical process of secondary inorganic aerosols production may be crucial in wet seasons via ACIs.

Simulating gas-aerosol-cirrus interactions: Process-oriented microphysical model and applications

Directory of Open Access Journals (Sweden)

B. Kärcher

2003-01-01

Full Text Available This work describes a process-oriented, microphysical-chemical model to simulate the formation and evolution of aerosols and ice crystals under the conditions prevailing in the upper troposphere and lower stratosphere. The model can be run as a box model or along atmospheric trajectories, and considers mixing, gas phase chemistry of aerosol precursors, binary homogeneous aerosol nucleation, homogeneous and heterogeneous ice nucleation, coagulation, condensation and dissolution, gas retention during particle freezing, gas trapping in growing ice crystals, and reverse processes. Chemical equations are solved iteratively using a second order implicit integration method. Gas-particle interactions and coagulation are treated over various size structures, with fully mass conserving and non-iterative numerical solution schemes. Particle types include quinternary aqueous solutions composed of H2SO4, HNO3, HCl, and HBr with and without insoluble components, insoluble aerosol particles, and spherical or columnar ice crystals deriving from each aerosol type separately. Three case studies are discussed in detail to demonstrate the potential of the model to simulate real atmospheric processes and to highlight current research topics concerning aerosol and cirrus formation near the tropopause. Emphasis is placed on how the formation of cirrus clouds and the scavenging of nitric acid in cirrus depends on small-scale temperature fluctuations and the presence of efficient ice nuclei in the tropopause region, corroborating and partly extending the findings of previous studies.

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

Science.gov (United States)

Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

2008-01-01

Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al ., 2001]." Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 19991. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005

Aerosol processing: a wind of innovation in the field of advanced heterogeneous catalysts.

Science.gov (United States)

Debecker, Damien P; Le Bras, Solène; Boissière, Cédric; Chaumonnot, Alexandra; Sanchez, Clément

2018-04-16

Aerosol processing is long known and implemented industrially to obtain various types of divided materials and nanomaterials. The atomisation of a liquid solution or suspension produces a mist of aerosol droplets which can then be transformed via a diversity of processes including spray-drying, spray pyrolysis, flame spray pyrolysis, thermal decomposition, micronisation, gas atomisation, etc. The attractive technical features of these aerosol processes make them highly interesting for the continuous, large scale, and tailored production of heterogeneous catalysts. Indeed, during aerosol processing, each liquid droplet undergoes well-controlled physical and chemical transformations, allowing for example to dry and aggregate pre-existing solid particles or to synthesise new micro- or nanoparticles from mixtures of molecular or colloidal precursors. In the last two decades, more advanced reactive aerosol processes have emerged as innovative means to synthesise tailored-made nanomaterials with tunable surface properties, textures, compositions, etc. In particular, the "aerosol-assisted sol-gel" process (AASG) has demonstrated tremendous potential for the preparation of high-performance heterogeneous catalysts. The method is mainly based on the low-cost, scalable, and environmentally benign sol-gel chemistry process, often coupled with the evaporation-induced self-assembly (EISA) concept. It allows producing micronic or submicronic, inorganic or hybrid organic-inorganic particles bearing tuneable and calibrated porous structures at different scales. In addition, pre-formed nanoparticles can be easily incorporated or formed in a "one-pot" bottom-up approach within the porous inorganic or hybrid spheres produced by such spray drying method. Thus, multifunctional catalysts with tailored catalytic activities can be prepared in a relatively simple way. This account is an overview of aerosol processed heterogeneous catalysts which demonstrated interesting performance in

Fog and Cloud Induced Aerosol Modification Observed by AERONET

Science.gov (United States)

Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M. A.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Platnick, S. E.; Arnold, G. T.;

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

Science.gov (United States)

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

2012-03-01

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

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.

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

Science.gov (United States)

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

2010-01-01

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

Bounding the heterogeneous gas uptake on aerosols and ground using resistance model

Science.gov (United States)

Su, H.; Li, M.; Cheng, Y.

2017-12-01

Heterogeneous uptake on aerosols and ground are potential important atmospheric sinks for gases. Different schemes have been used to characterize the dry deposition and heterogeneous aerosol gas uptake, although they share similar characteristics. In this work, we propose a unified resistance model to compare the uptake flux on both ground and aerosols, to identify the dominate heterogeneous process within the planetary boundary layer (PBL). The Gamma(eq) is introduced to represent the reactive uptake coefficient on aerosols when these two processes are equally important. It's shown that Gamma(eq) is proportional to the dry deposition velocity, inversely proportional to aerosol surface area concentration. Under typical regional background condition, Gamma(eq) vary from 1x10-5 to 4x10-4 with gas species, land-use type and season, which indicates that aerosol gas uptake should be included in atmospheric models when uptake coefficient higher than 10-5. We address the importance of heterogeneous gas uptake on aerosols over ground especially for ozone uptake on liquid organic aerosols and for marine PBL atmosphere.

Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis

Directory of Open Access Journals (Sweden)

M. Ramonet

2011-08-01

Full Text Available Dual carbon isotope analysis of marine aerosol samples 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 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 terrestrial origin. By contrast, for polluted air advected 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.

Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C 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.; Ramonet, M.; O'Dowd, C. D.

2011-08-01

Dual carbon isotope analysis of marine aerosol samples 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 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 terrestrial origin. By contrast, for polluted air advected 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.

Aerosol processes relevant for the Netherlands

NARCIS (Netherlands)

Brugh, Aan de J.M.J.

2013-01-01

Particulate matter (or aerosols) are particles suspended in the atmosphere. Aerosols are believed to be the most important pollutant associated with increased human mortality and morbidity. Therefore, it is important to investigate the relationship between sources of aerosols (such as industry)

Design of Nanomaterial Synthesis by Aerosol Processes

Science.gov (United States)

Buesser, Beat; Pratsinis, Sotiris E.

2013-01-01

Aerosol synthesis of materials is a vibrant field of particle technology and chemical reaction engineering. Examples include the manufacture of carbon blacks, fumed SiO2, pigmentary TiO2, ZnO vulcanizing catalysts, filamentary Ni, and optical fibers, materials that impact transportation, construction, pharmaceuticals, energy, and communications. Parallel to this, development of novel, scalable aerosol processes has enabled synthesis of new functional nanomaterials (e.g., catalysts, biomaterials, electroceramics) and devices (e.g., gas sensors). This review provides an access point for engineers to the multiscale design of aerosol reactors for the synthesis of nanomaterials using continuum, mesoscale, molecular dynamics, and quantum mechanics models spanning 10 and 15 orders of magnitude in length and time, respectively. Key design features are the rapid chemistry; the high particle concentrations but low volume fractions; the attainment of a self-preserving particle size distribution by coagulation; the ratio of the characteristic times of coagulation and sintering, which controls the extent of particle aggregation; and the narrowing of the aggregate primary particle size distribution by sintering. PMID:22468598

Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

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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

Cloud Processing of Gases and Aerosols in Air Quality Modeling

Directory of Open Access Journals (Sweden)

Leiming Zhang

2011-10-01

Full Text Available The representations of cloud processing of gases and aerosols in some of the current state-of-the-art regional air quality models in North America and Europe are reviewed. Key processes reviewed include aerosol activation (or nucleation scavenging of aerosols, aqueous-phase chemistry, and wet deposition/removal of atmospheric tracers. It was found that models vary considerably in the parameterizations or algorithms used in representing these processes. As an emerging area of research, the current understanding of the uptake of water soluble organics by cloud droplets and the potential aqueous-phase reaction pathways leading to the atmospheric secondary organic aerosol (SOA formation is also reviewed. Sensitivity tests using the AURAMS model have been conducted in order to assess the impact on modeled regional particulate matter (PM from: (1 the different aerosol activation schemes, (2 the different below-cloud particle scavenging algorithms, and (3 the inclusion of cloud processing of water soluble organics as a potential pathway for the formation of atmospheric SOA. It was found that the modeled droplet number concentrations and ambient PM size distributions were strongly affected by the use of different aerosol activation schemes. The impact on the modeled average ambient PM mass concentration was found to be limited in terms of averaged PM2.5 concentration (~a few percents but more significant in terms of PM1.0 (up to 10 percents. The modeled ambient PM was found to be moderately sensitive to the below-cloud particle scavenging algorithms, with relative differences up to 10% and 20% in terms of PM2.5 and PM10, respectively, when using the two different algorithms for the scavenging coefficient (Λ corresponding to the lower and upper bounds in the parameterization for Λ. The model simulation with the additional cloud uptake and processing of water-soluble organic gases was shown to improve the evaluation statistics for modeled PM2.5 OA

Comparative study on aerosol removal by natural processes in containment in severe accident for AP1000 reactor

International Nuclear Information System (INIS)

Sun, Xiaohui; Cao, Xinrong; Shi, Xingwei; Yan, Jin

2017-01-01

Highlights: • Characteristics of aerosol distribution in containment are obtained. • Aerosol removal by natural processes is comparative studied by two methods. • Traditional rapid assessment method is conservative and can be applied in AP1000 reactor. - Abstract: Focusing on aerosol removal by naturally occurring processes in containment in severe accident for AP1000, integral severe accident code MELCOR and rapid assessment method mentioned in NUREG/CR-6189 are utilized to study aerosol removal by natural processes, respectively. Three typical severe accidents, induced by large break loss of coolant accident (LBLOCA), small break loss of coolant accident (SBLOCA) and steam generator tube rupture (SGTR), respectively, are selected for the study. The results obtained by two methods were further compared in the following several aspects: efficiency of aerosol removal by natural processes, peak time of aerosol suspended in containment atmosphere, peak amount of aerosol suspended in containment atmosphere, time when aerosol removal efficiency by natural processes is up to 99.9%. It was further concluded that results obtained by rapid assessment with shorter calculation process are more conservative. The analysis results provide reference to assessment method selection of severe accident source term for AP1000 nuclear emergency.

Secondary Inorganic Aerosols over an Urban Location in North-Western Himalayan Region: Seasonal Variation in Composition and Formation Process(es)

Science.gov (United States)

Kaushal, D.; Tandon, A.

2017-12-01

Oxidative photo-chemical transformation of precursor gases, mainly of anthropogenic origin, produces secondary aerosols. Secondary inorganic aerosols constitute a significant fraction of total aerosol load over urban locations especially high altitude in wet-temperate climatic set-up. Towns situated in North-Western Himalayan region (NWHR) with sizable population and attractive tourist destinations have been facing ever increasing problem of gaseous and particulate air pollution from exponential increase in vehicular traffic and other anthropogenic emissions. The present study has been planned to investigate the seasonal variations in atmospheric processes responsible for the formation of Secondary Inorganic Aerosols (SIA) and to estimate contribution of SIA to PM­10 load over an Urban location, Dharamshala, in Dhauladhar region of NWHR. Twenty four hourly PM10 aerosol samples were collected, on quartz micro fibre filters in Dharamshala (1350 amsl) on weekly basis for complete one year time-period (February 2015 - January 2016). These samples were analyzed for Water Soluble Inorganic Ions (WSII) using Ion-Chromatographic System. On annual basis, SO42- ions contributed maximum (52%) followed by NO3- (13%) and NH4+ (12%) to WSII. Based upon Principal Component Analysis (PCA), dominant sources contributing to PM10 associated WSII were identified as: Fossil-Fuel and Bio-mass burning, Vehicular (mainly diesel) emissions and gaseous emissions from the microbial degradation of dead bio-mass. Throughout the year, significantly high proportion of SO42- and considerable thermodynamic stability of (NH4)2SO2 at ambient temperatures, made it the major contributor to SIA over NH4NO3 and NH4Cl. On seasonal basis, maximum contribution of SIA to PM10 was observed in monsoon followed by the winter season. Low ambient temperature in winter season favoured formation of NH4NO3 with significant contribution to SIA. It could be concluded that observed variability in the composition and

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

Science.gov (United States)

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

Seawater mesocosm experiments in the Arctic uncover differential transfer of marine bacteria to aerosols.

Science.gov (United States)

Fahlgren, Camilla; Gómez-Consarnau, Laura; Zábori, Julia; Lindh, Markus V; Krejci, Radovan; Mårtensson, E Monica; Nilsson, Douglas; Pinhassi, Jarone

2015-06-01

Biogenic aerosols critically control atmospheric processes. However, although bacteria constitute major portions of living matter in seawater, bacterial aerosolization from oceanic surface layers remains poorly understood. We analysed bacterial diversity in seawater and experimentally generated aerosols from three Kongsfjorden sites, Svalbard. Construction of 16S rRNA gene clone libraries from paired seawater and aerosol samples resulted in 1294 sequences clustering into 149 bacterial and 34 phytoplankton operational taxonomic units (OTUs). Bacterial communities in aerosols differed greatly from corresponding seawater communities in three out of four experiments. Dominant populations of both seawater and aerosols were Flavobacteriia, Alphaproteobacteria and Gammaproteobacteria. Across the entire dataset, most OTUs from seawater could also be found in aerosols; in each experiment, however, several OTUs were either selectively enriched in aerosols or little aerosolized. Notably, a SAR11 clade OTU was consistently abundant in the seawater, but was recorded in significantly lower proportions in aerosols. A strikingly high proportion of colony-forming bacteria were pigmented in aerosols compared with seawater, suggesting that selection during aerosolization contributes to explaining elevated proportions of pigmented bacteria frequently observed in atmospheric samples. Our findings imply that atmospheric processes could be considerably influenced by spatiotemporal variations in the aerosolization efficiency of different marine bacteria. © 2015 Society for Applied Microbiology and John Wiley & Sons Ltd.

Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

Science.gov (United States)

Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

2016-10-01

Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

Secondary organic aerosol formation through cloud processing of aromatic VOCs

Science.gov (United States)

Herckes, P.; Hutchings, J. W.; Ervens, B.

2010-12-01

Field observations have shown substantial concentrations (20-5,500 ng L-1) of aromatic volatile organic compounds (VOC) in cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric laboratory conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction rates decreased with increasing organic carbon content. Kinetic data derived from these experiments were used as input to a multiphase box model in order to evaluate the secondary organic aerosol (SOA) mass formation potential of cloud processing of BTEX. Model results will be presented that quantify the SOA amounts from these aqueous phase pathways. The efficiency of this multiphase SOA source will be compared to SOA yields from the same aromatics as treated in traditional SOA models that are restricted to gas phase oxidation and subsequent condensation on particles.

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.

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.

Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

Science.gov (United States)

Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

2017-12-01

The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

Assessment of Aerosol Distributions from GEOS-5 Using the CALIPSO Feature Mask

Science.gov (United States)

Welton, Ellsworth

2010-01-01

A-train sensors such as MODIS, MISR, and CALIPSO are used to determine aerosol properties, and in the process a means of estimating aerosol type (e.g. smoke vs. dust). Correct classification of aerosol type is important for climate assessment, air quality applications, and for comparisons and analysis with aerosol transport models. The Aerosols-Clouds-Ecosystems (ACE) satellite mission proposed in the NRC Decadal Survey describes a next generation aerosol and cloud suite similar to the current A-train, including a lidar. The future ACE lidar must be able to determine aerosol type effectively in conjunction with modeling activities to achieve ACE objectives. Here we examine the current capabilities of CALIPSO and the NASA Goddard Earth Observing System general circulation model and data assimilation system (GEOS-5), to place future ACE needs in context. The CALIPSO level 2 feature mask includes vertical profiles of aerosol layers classified by type. GEOS-5 provides global 3D aerosol mass for sulfate, sea salt, dust, and black and organic carbon. A GEOS aerosol scene classification algorithm has been developed to provide estimates of aerosol mixtures and extinction profiles along the CALIPSO orbit track. In previous work, initial comparisons between GEOS-5 derived aerosol mixtures and CALIPSO derived aerosol types were presented for July 2007. In general, the results showed that model and lidar derived aerosol types did not agree well in the boundary layer. Agreement was poor over Europe, where CALIPSO indicated the presence of dust and pollution mixtures yet GEOS-5 was dominated by pollution with little dust. Over the ocean in the tropics, the model appeared to contain less sea salt than detected by CALIPSO, yet at high latitudes the situation was reserved. Agreement between CALIPSO and GEOS-5, aerosol types improved above the boundary layer, primarily in dust and smoke dominated regions. At higher altitudes (> 5 km), the model contained aerosol layers not detected

Modelling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

Science.gov (United States)

Karl, M.; Kukkonen, J.; Keuken, M. P.; Lützenkirchen, S.; Pirjola, L.; Hussein, T.

2015-12-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of one hour, i.e. on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using an aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of n-alkanes, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. It was not necessary to model the nucleation of gas-phase vapors, as the computations were started with roadside conditions. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, condensational growth contributed significantly to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes can predict particle number concentrations between roadside and the urban background with an inaccuracy of ∼ 10 %, compared to the fully size-resolved MAFOR model.

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

Science.gov (United States)

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

2018-03-01

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

Real-time, controlled OH-initiated oxidation of biogenic secondary organic aerosol

Directory of Open Access Journals (Sweden)

J. G. Slowik

2012-10-01

Full Text Available The chemical complexity of atmospheric organic aerosol (OA requires novel methods for characterization of its components and description of its atmospheric processing-induced transformations. We present the first field deployment of the Toronto Photooxidation Tube (TPOT, a field-deployable flow reactor for the controlled exposure of ambient aerosol to OH radicals. The system alternates between sampling of (1 (unreacted ambient aerosol, (2 aerosol exposed to UV light and subjected to a ~4 to 10 °C temperature increase, and (3 aerosol that is oxidized by OH (in addition to the aforementioned UV exposure/temperature increase. This allows both characterization of the aging process and classification of aerosol in terms of its volatility and reaction-based properties. Summertime measurements by an aerosol mass spectrometer coupled to the TPOT were performed in the remote forest of western Canada, resulting in aerosol dominated by biogenic secondary organic aerosol. Volatilization/UV exposure resulted in an approximately 10 to 25% decrease in organic mass and resulted in a slight increase in oxygenation. OH oxidation resulted in a further organic mass decrease (additional ~25% and yielded an aerosol with O:C values comparable to those characteristic of low volatility, highly oxygenated OA. Most OH-induced changes occurred within ~3 day-equivalents of atmospheric processing, with further reactions generally proceeding at a greatly reduced rate. Positive matrix factorization (PMF analysis of the TPOT data yielded five factors. One factor is related to primary biomass burning organic aerosol, while the others describe oxygenated organic aerosol (OOA components in terms of reactivity and volatility: (1 volatile and reactive; (2 non-volatile and reactive; (3 non-volatile and reactive early-generation product; (4 non-volatile and non-reactive product. This PMF classification of aerosol components directly in terms of reactivity and volatility is enabled by

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

Science.gov (United States)

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

2015-05-01

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

Aerosol processing for nanomanufacturing

International Nuclear Information System (INIS)

Girshick, Steven L.

2008-01-01

Advances in nanoparticle synthesis are opening new opportunities for a broad variety of technologies that exploit the special properties of matter at the nanoscale. To realize this potential will require the development of new technologies for processing nanoparticles, so as to utilize them in a manufacturing context. Two important classes of such processing technologies include the controlled deposition of nanoparticles onto surfaces, and the application of chemically specific coatings onto individual nanoparticles, so as to either passivate or functionalize their surfaces. This paper provides an overview of three technologies related to these objectives, with an emphasis on aerosol-based methods: first, the deposition of nanoparticles by hypersonic impaction, so as so spray-coat large areas with nanoparticles; second, the use of aerodynamic lenses to produce focused beams of nanoparticles, with beam widths of a few tens of microns, so as to integrate nanoparticle-based structures into microelectromechanical systems; and third, the coating of individual nanoparticles by means of photoinduced chemical vapor deposition (photo-CVD), driven by excimer lamps. We also discuss the combination of these technologies, so that nanoparticle synthesis, together with multiple processing steps, can be accomplished in a single flow stream.

Aerosol and Photo-Oxidant Processes in the Eastern Mediterranean

Czech Academy of Sciences Publication Activity Database

Lazaridis, M.; Spyridaki, A.; Solberg, S.; Smolík, Jiří; Ždímal, Vladimír; Eleftheriadis, K.; Aleksandropoulos, V.; Hov, O.; Georgopoulos, P. G.

2004-01-01

Roč. 4, - (2004), s. 5455-5514 ISSN 1680-7367 Grant - others:ENVK2(XE) 1999-00052 Institutional research plan: CEZ:AV0Z4072921 Keywords : aerosol * mesoscale modeling * photo-oxidant processes Subject RIV: CF - Physical ; Theoretical Chemistry

Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

Directory of Open Access Journals (Sweden)

J. Ofner

2012-07-01

Full Text Available Reactive halogen species (RHS, such as X·, X₂ and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA and organic aerosol derived from biomass-burning (BBOA has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols.

Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS, released from simulated natural halogen sources like salt pans. Subsequently, the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which results in new functional groups (FTIR spectroscopy, changes UV/VIS absorption, chemical composition (ultrahigh resolution mass spectroscopy (ICR-FT/MS, or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

Enhanced Iron Solubility at Low pH in Global Aerosols

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Ellery D. Ingall

2018-05-01

Full Text Available The composition and oxidation state of aerosol iron were examined using synchrotron-based iron near-edge X-ray absorption spectroscopy. By combining synchrotron-based techniques with water leachate analysis, impacts of oxidation state and mineralogy on aerosol iron solubility were assessed for samples taken from multiple locations in the Southern and the Atlantic Oceans; and also from Noida (India, Bermuda, and the Eastern Mediterranean (Crete. These sampling locations capture iron-containing aerosols from different source regions with varying marine, mineral dust, and anthropogenic influences. Across all locations, pH had the dominating influence on aerosol iron solubility. When aerosol samples were approximately neutral pH, iron solubility was on average 3.4%; when samples were below pH 4, the iron solubility increased to 35%. This observed aerosol iron solubility profile is consistent with thermodynamic predictions for the solubility of Fe(III oxides, the major iron containing phase in the aerosol samples. Source regions and transport paths were also important factors affecting iron solubility, as samples originating from or passing over populated regions tended to contain more soluble iron. Although the acidity appears to affect aerosol iron solubility globally, a direct relationship for all samples is confounded by factors such as anthropogenic influence, aerosol buffer capacity, mineralogy and physical processes.

Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

Directory of Open Access Journals (Sweden)

B. Ervens

2010-09-01

Full Text Available This study presents a modeling framework based on laboratory data to describe the kinetics of glyoxal reactions that form secondary organic aerosol (SOA in aqueous aerosol particles. Recent laboratory results on glyoxal reactions are reviewed and a consistent set of empirical reaction rate constants is derived that captures the kinetics of glyoxal hydration and subsequent reversible and irreversible reactions in aqueous inorganic and water-soluble organic aerosol seeds. Products of these processes include (a oligomers, (b nitrogen-containing products, (c photochemical oxidation products with high molecular weight. These additional aqueous phase processes enhance the SOA formation rate in particles and yield two to three orders of magnitude more SOA than predicted based on reaction schemes for dilute aqueous phase (cloud chemistry for the same conditions (liquid water content, particle size.

The application of the new module including detailed chemical processes in a box model demonstrates that both the time scale to reach aqueous phase equilibria and the choice of rate constants of irreversible reactions have a pronounced effect on the predicted atmospheric relevance of SOA formation from glyoxal. During day time, a photochemical (most likely radical-initiated process is the major SOA formation pathway forming ∼5 μg m⁻³ SOA over 12 h (assuming a constant glyoxal mixing ratio of 300 ppt. During night time, reactions of nitrogen-containing compounds (ammonium, amines, amino acids contribute most to the predicted SOA mass; however, the absolute predicted SOA masses are reduced by an order of magnitude as compared to day time production. The contribution of the ammonium reaction significantly increases in moderately acidic or neutral particles (5 < pH < 7.

Glyoxal uptake into ammonium sulfate seed under dark conditions can be represented with a single reaction parameter k_effupt that does not depend

Numerical analysis of the formation process of aerosols in the alveoli

Science.gov (United States)

Haslbeck, Karsten; Seume, Jörg R.

2008-11-01

For a successful diagnosis of lung diseases through an analysis of non-volatile molecules in the exhaled breath, an exact understanding of the aerosol formation process is required. This process is modeled using Computational Fluid Dynamics (CFD). The model shows the interaction of the boundary surface between the streamed airway and the local epithelial liquid layer. A 2-D volume mesh of an alveolus is generated by taking into account the connection of the alveoli with the sacculi alveolares (SA). The Volume of Fluid (VOF) Method is used to model the interface between the gas and the liquid film. The non-Newtonian flow is modeled by the implementation of the Ostwald de Waele model. Surface tension is a function of the surfactant concentration. The VOF-Method allows the distribution of the concentration of the epithelial liquid layer at the surface to be traced in a transient manner. The simulations show the rupturing of the liquid film through the drop formation. Aerosol particles are ejected into the SA and do not collide with the walls. The quantity, the geometrical size as well as the velocity distributions of the generated aerosols are determined. The data presented in the paper provide the boundary conditions for future CFD analysis of the aerosol transport through the airways up to exhalation.

Elemental composition of aerosol particles from two atmospheric monitoring stations in the Amazon Basin

International Nuclear Information System (INIS)

Artaxo, P.; Gerab, F.; Rabello, M.L.C.

1993-01-01

One key region for the study of processes that are changing the composition of the global atmosphere is the Amazon Basin tropical rain forest. The high rate of deforestation and biomass burning is emitting large amounts of gases and fine-mode aerosol particles to the global atmosphere. Two background monitoring stations are operating continuously measuring aerosol composition, at Cuiaba, and Serra do Navio. Fine- and coarse-mode aerosol particles are being collected using stacked filter units. Particle induced X-ray emission (PIXE) was used to measure concentrations of up to 21 elements: Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Se, Br, Rb, Sr, Zr, and Pb. The elemental composition was measured at the new PIXE facility from the University of Sao Paulo, using a dedicated 5SDH tandem Pelletron nuclear accelerator. Absolute principal factor analysis (APFA) has derived absolute elemental source profiles. At the Serra do Navio sampling site a very clean background aerosol is being observed. Biogenic aerosol dominates the fine-mode mass concentration, with the presence of K, P, S, Cl, Zn, Br, and FPM. Three components dominate the aerosol composition: Soil dust particles, the natural biogenic release by the forest, and a marine aerosol component. At the Cuiaba site, during the dry season, a strong component of biomass burning is observed. An aerosol mass concentration up to 120 μg/m 3 was measured. APFA showed three components: Soil dust (Al, Ca, Ti, Mn, Fe), biomass burning (soot, FPM, K, Cl) and natural biogenic particles (K, S, Ca, Mn, Zn). The fine-mode biogenic component of both sites shows remarkable similarities, although the two sampling sites are 3000 km apart. Several essential plant nutrients like P, K, S, Ca, Ni and others are transported in the atmosphere as a result of biomass burning processes. (orig.)

The Role of Aerosols on Precipitation Processes: Cloud Resolving Model Simulations

Science.gov (United States)

Tao, Wei-Kuo; Li, X.; Matsui, T.

2012-01-01

Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, the sub-tropics (Florida) and midlatitudes using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CeN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for these cases. It is shown that since the low (CN case produces fewer droplets, larger sizes develop due to greater condensational and collection growth, leading to a broader size spectrum in comparison to the high CCN case. Sensitivity tests were performed to

Plume dispersion and deposition processes of tracer gas and aerosols in short-distance experiments

International Nuclear Information System (INIS)

Taeschner, M.; Bunnenberg, C.

1988-01-01

Data used in this paper were extracted from field experiments carried out in France and Canada to study the pathway of elementary tritium after possible emissions from future fusion reactors and from short-range experiments with nutrient aerosols performed in a German forest in view of a therapy of damaged coniferous trees by foliar nutrition. Comparisons of dispersion parameters evaluated from the tritium field experiments show that in the case of the 30-min release the variations of the wind directions represent the dominant mechanism of lateral plume dispersion under unstable weather conditions. This corresponds with the observation that for the short 2-min emission the plume remains more concentrated during propagation, and the small lateral dispersion parameters typical for stable conditions have to be applied. The investigations on the dispersion of aerosol plumes into a forest boundary layer show that the Gaussian plume model can be modified by a windspeed factor to be valid for predictions on aerosol concentrations and depositions even in a structured topography like a forest

Sensitivity Studies on the Influence of Aerosols on Cloud and Precipitation Development Using WRF Mesoscale Model Simulations

Science.gov (United States)

Thompson, G.; Eidhammer, T.; Rasmussen, R.

2011-12-01

Using the WRF model in simulations of shallow and deep precipitating cloud systems, we investigated the sensitivity to aerosols initiating as cloud condensation and ice nuclei. A global climatological dataset of sulfates, sea salts, and dust was used as input for a control experiment. Sensitivity experiments with significantly more polluted conditions were conducted to analyze the resulting impacts to cloud and precipitation formation. Simulations were performed using the WRF model with explicit treatment of aerosols added to the Thompson et al (2008) bulk microphysics scheme. The modified scheme achieves droplet formation using pre-tabulated CCN activation tables provided by a parcel model. The ice nucleation is parameterized as a function of dust aerosols as well as homogeneous freezing of deliquesced aerosols. The basic processes of aerosol activation and removal by wet scavenging are considered, but aerosol characteristic size or hygroscopicity does not change due to evaporating droplets. In other words, aerosol processing was ignored. Unique aspects of this study include the usage of one to four kilometer grid spacings and the direct parameterization of ice nucleation from aerosols rather than typical temperature and/or supersaturation relationships alone. Initial results from simulations of a deep winter cloud system and its interaction with significant orography show contrasting sensitivities in regions of warm rain versus mixed liquid and ice conditions. The classical view of higher precipitation amounts in relatively clean maritime clouds with fewer but larger droplets is confirmed for regions dominated by the warm-rain process. However, due to complex interactions with the ice phase and snow riming, the simulations revealed the reverse situation in high terrain areas dominated by snow reaching the surface. Results of other cloud systems will be summarized at the conference.

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

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

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.

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

Energy Technology Data Exchange (ETDEWEB)

Zhang, Qi [Univ. of California, Davis, CA (United States)

2017-05-21

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routine measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from this

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

Science.gov (United States)

Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lützenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq

2016-04-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and

Real time measurements of submicrometer aerosols in Seoul, Korea: Sources, characteristics, and processing of organic aerosols during winter time.

Science.gov (United States)

Kim, H.; Zhang, Q.

2016-12-01

Highly time-resolved chemical characterization of non-refractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter when persistent air quality problems associated with elevated PM concentrations were observed. The average NR-PM1 concentration was 27.5 µg m-3 and the average mass was dominated by organics (44%), followed by nitrate (24%) and sulfate (10%). Five distinct sources of organic aerosol (OA) were identified from positive matrix factorization (PMF) analysis of the AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA), cooking represented by a cooking OA factor (COA), wood combustion represented by a biomass burning OA factor (BBOA), and secondary aerosol formation in the atmosphere that is represented by a semi-volatile oxygenated OA factor (SVOOA) and a low volatile oxygenated OA factor (LVOOA). These factors, on average, contributed 16, 20, 23, 15 and 26% to the total OA mass, respectively, with primary organic aerosol (POA = HOA + COA + BBOA) accounting for 59% of the OA mass. On average, both primary emissions and secondary aerosol formation are important factors affecting air quality in Seoul during winter, contributing approximately equal. However, differences in the fraction of PM source and properties were observed between high and low loading PM period. For example, during stagnant period with low wind speed (WS) (0.99 ± 0.7 m/s) and high RH (71%), high PM loadings (43.6 ± 12.4 µg m-3) with enhanced fractions of nitrate (27%) and SVOOA (8%) were observed, indicating a strong influence from locally generated secondary aerosol. On the other hand, when low PM loadings (12.6 ± 7.1 µg m-3), which were commonly associated with high WS (1.8 ± 1.1 m/s) and low RH (50 %), were observed, the fraction of regional sources, such as sulfate (12%) and LVOOA (21

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

Science.gov (United States)

Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic

Dissolution process of atmospheric aerosol particles into cloud droplets; Processus de dissolution des aerosols atmospheriques au sein des gouttes d'eau nuageuses

Energy Technology Data Exchange (ETDEWEB)

Desboeufs, K

2001-01-15

Clouds affect both climate via the role they play in the Earth's radiation balance and tropospheric chemistry since they are efficient reaction media for chemical transformation of soluble species. Cloud droplets are formed in the atmosphere by condensation of water vapour onto aerosol particles, the cloud condensation nuclei (CCN). The water soluble fraction of these CCN governs the cloud micro-physics, which is the paramount factor playing on the radiative properties of clouds. Moreover, this soluble fraction is the source of species imply in the oxidation/reduction reactions in the aqueous phase. Thus, it is of particular importance to understand the process controlling the solubilization of aerosols in the cloud droplets. The main purpose of this work is to investigate experimentally and theoretically the dissolution of particles incorporated in the aqueous phase. From the studies conducted up to now, we have identify several factors playing on the dissolution reaction of aerosols. However, the quantification of the effects of these factors is difficult since the current means of study are not adapted to the complexity of cloud systems. First, this work consisted to perform a experimental system, compound by an open flow reactor, enabling to follow the kinetic of dissolution in conditions representative of cloud. This experimental device is used to a systematic characterisation of the known factors playing on the dissolution, i.e. pH, aerosol nature, aerosol weathering... and also for the identification and the quantification of the effects of other factors: ionic strength, acid nature, clouds processes. These experiments gave quantitative results, which are used to elaborate a simple model of aerosol dissolution in the aqueous phase. This model considers the main factors playing on the dissolution and results in a general mechanism of aerosol dissolution extrapolated to the cloud droplets. (author)

Secondary organic aerosol formation through fog processing of VOCs

Science.gov (United States)

Herckes, P.; Hutchings, J. W.

2010-07-01

Volatile Organic Compounds (VOCs) including benzene, toluene, ethylbenzene and xylenes (BTEX) have been determined in highly concentrated amounts (>1 ug/L) in intercepted clouds in northern Arizona (USA). These VOCs are found in concentrations much higher than predicted by partitioning alone. The reactivity of BTEX in the fog/cloud aqueous phase was investigated through laboratory studies. BTEX species showed fast degradation in the aqueous phase in the presence of peroxides and light. Observed half-lives ranged from three and six hours, substantially shorter than the respective gas phase half-lives (several days). The observed reaction rates were on the order of 1 ppb/min but decreased substantially with increasing concentrations of organic matter (TOC). The products of BTEX oxidation reactions were analyzed using HPLC-UV and LCMS. The first generation of products identified included phenol and cresols which correspond to the hydroxyl-addition reaction to benzene and toluene. Upon investigating of multi-generational products, smaller, less volatile species are predominant although a large variety of products is found. Most reaction products have substantially lower vapor pressure and will remain in the particle phase upon droplet evaporation. The SOA generation potential of cloud and fog processing of BTEX was evaluated using simple calculations and showed that in ideal situations these reactions could add up to 9% of the ambient aerosol mass. In more conservative scenarios, the contribution of the processing of BTEX was around 1% of ambient aerosol concentrations. Overall, cloud processing of VOC has the potential to contribute to the atmospheric aerosol mass. However, the contribution will depend upon many factors such as the irradiation, organic matter content in the droplets and droplet lifetime.

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.

Cloud processing of organic compounds: Secondary organic aerosol and nitrosamine formation

Science.gov (United States)

Hutchings, James W., III

Cloud processing of atmospheric organic compounds has been investigated through field studies, laboratory experiments, and numerical modeling. Observational cloud chemistry studies were performed in northern Arizona and fog studies in central Pennsylvania. At both locations, the cloud and fogs showed low acidity due to neutralization by soil dust components (Arizona) and ammonia (Pennsylvania). The field observations showed substantial concentrations (20-5500 ng•L -1) of volatile organic compounds (VOC) in the cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase with half lives of approximately three hours. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction kinetics decreased with increasing organic carbon content, resulting in half lives of approximately 7 hours. The secondary organic aerosol (SUA) mass formation potential of cloud processing of BTEX was evaluated. SOA mass formation by cloud processing of BTEX, while strongly dependent on the atmospheric conditions, could contribute up to 9% of the ambient atmospheric aerosol mass, although typically ˜1% appears realistic. Field observations also showed the occurrence of N-nitrosodimethylamine (NDMA), a potent carcinogen, in fogs and clouds (100-340 ng•L -1). Laboratory studies were conducted to investigate the formation of NDMA from nitrous acid and dimethylamine in the homogeneous aqueous phase within cloud droplets. While NDMA was produced in the cloud droplets, the low yields (NDMA with partitioning to droplet must be the source of aqueous

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

Directory of Open Access Journals (Sweden)

M. Karl

2016-04-01

Full Text Available This study evaluates the influence of aerosol processes on the particle number (PN concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i the coagulation of particles, (ii the condensation and evaporation of two organic vapors, and (iii dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from −76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of

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

International Nuclear Information System (INIS)

Gillett, Nathan P; Von Salzen, Knut

2013-01-01

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

Numerical simulations of homogeneous freezing processes in the aerosol chamber AIDA

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W. Haag

2003-01-01

Full Text Available The homogeneous freezing of supercooled H2SO4/H2O aerosols in an aerosol chamber is investigated with a microphysical box model using the activity parameterization of the nucleation rate by Koop et al. (2000. The simulations are constrained by measurements of pressure, temperature, total water mixing ratio, and the initial aerosol size distribution, described in a companion paper Möhler et al. (2003. Model results are compared to measurements conducted in the temperature range between 194 and 235 K, with cooling rates in the range between 0.5 and 2.6 K min-1, and at air pressures between 170 and 1000 hPa. The simulations focus on the time history of relative humidity with respect to ice, aerosol size distribution, partitioning of water between gas and particle phase, onset times of freezing, freezing threshold relative humidities, aerosol chemical composition at the onset of freezing, and the number of nucleated ice crystals. The latter four parameters can be inferred from the experiments, the former three aid in interpreting the measurements. Sensitivity studies are carried out to address the relative importance of uncertainties of basic quantities such as temperature, total H2O mixing ratio, aerosol size spectrum, and deposition coefficient of H2O molecules on ice. The ability of the numerical simulations to provide detailed explanations of the observations greatly increases confidence in attempts to model this process under real atmospheric conditions, for instance with regard to the formation of cirrus clouds or polar stratospheric ice clouds, provided that accurate temperature and humidity measurements are available.

An overview of mesoscale aerosol processes, comparisons, and validation studies from DRAGON networks

Science.gov (United States)

Holben, Brent N.; Kim, Jhoon; Sano, Itaru; Mukai, Sonoyo; Eck, Thomas F.; Giles, David M.; Schafer, Joel S.; Sinyuk, Aliaksandr; Slutsker, Ilya; Smirnov, Alexander; Sorokin, Mikhail; Anderson, Bruce E.; Che, Huizheng; Choi, Myungje; Crawford, James H.; Ferrare, Richard A.; Garay, Michael J.; Jeong, Ukkyo; Kim, Mijin; Kim, Woogyung; Knox, Nichola; Li, Zhengqiang; Lim, Hwee S.; Liu, Yang; Maring, Hal; Nakata, Makiko; Pickering, Kenneth E.; Piketh, Stuart; Redemann, Jens; Reid, Jeffrey S.; Salinas, Santo; Seo, Sora; Tan, Fuyi; Tripathi, Sachchida N.; Toon, Owen B.; Xiao, Qingyang

2018-01-01

Over the past 24 years, the AErosol RObotic NETwork (AERONET) program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs) that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

An overview of mesoscale aerosol processes, comparisons, and validation studies from DRAGON networks

Directory of Open Access Journals (Sweden)

B. N. Holben

2018-01-01

Full Text Available Over the past 24 years, the AErosol RObotic NETwork (AERONET program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

Behavioral and social cognitive processes in preschool children's social dominance.

Science.gov (United States)

Pellegrini, Anthony D; Van Ryzin, Mark J; Roseth, Cary; Bohn-Gettler, Catherine; Dupuis, Danielle; Hickey, Meghan; Peshkam, Annie

2011-01-01

This longitudinal, naturalistic study addressed behavioral and social cognitive processes implicated in preschool children's social dominance. In the first objective, we examined the degree to which peer aggression, affiliation, and postaggression reconciliation predicted social dominance across a school year. Consistent with predictions, all three predicted dominance early in the year while only affiliation predicted dominance later in the year, suggesting that aggression, affiliation, and reconciliation were used to establish social dominance where affiliation was used to maintain it. In the second, exploratory, objective we tested the relative importance of social dominance and reconciliation (the Machiavellian and Vygotskian intelligence hypotheses, respectively) in predicting theory of mind/false belief. Results indicated that social dominance accounted for significant variance, beyond that related to reconciliation and affiliation, in predicting theory of mind/false belief status. Results are discussed in terms of specific behavioral and social cognitive processes employed in establishing and maintaining social dominance. © 2011 Wiley-Liss, Inc.

Online Simulations of Global Aerosol Distributions in the NASA GEOS-4 Model and Comparisons to Satellite and Ground-Based Aerosol Optical Depth

Science.gov (United States)

Colarco, Peter; daSilva, Arlindo; Chin, Mian; Diehl, Thomas

2010-01-01

We have implemented a module for tropospheric aerosols (GO CART) online in the NASA Goddard Earth Observing System version 4 model and simulated global aerosol distributions for the period 2000-2006. The new online system offers several advantages over the previous offline version, providing a platform for aerosol data assimilation, aerosol-chemistry-climate interaction studies, and short-range chemical weather forecasting and climate prediction. We introduce as well a methodology for sampling model output consistently with satellite aerosol optical thickness (AOT) retrievals to facilitate model-satellite comparison. Our results are similar to the offline GOCART model and to the models participating in the AeroCom intercomparison. The simulated AOT has similar seasonal and regional variability and magnitude to Aerosol Robotic Network (AERONET), Moderate Resolution Imaging Spectroradiometer, and Multiangle Imaging Spectroradiometer observations. The model AOT and Angstrom parameter are consistently low relative to AERONET in biomass-burning-dominated regions, where emissions appear to be underestimated, consistent with the results of the offline GOCART model. In contrast, the model AOT is biased high in sulfate-dominated regions of North America and Europe. Our model-satellite comparison methodology shows that diurnal variability in aerosol loading is unimportant compared to sampling the model where the satellite has cloud-free observations, particularly in sulfate-dominated regions. Simulated sea salt burden and optical thickness are high by a factor of 2-3 relative to other models, and agreement between model and satellite over-ocean AOT is improved by reducing the model sea salt burden by a factor of 2. The best agreement in both AOT magnitude and variability occurs immediately downwind of the Saharan dust plume.

Improvement of Representation of the Cloud-Aerosol Interaction in Large-Scale Models

Energy Technology Data Exchange (ETDEWEB)

Khain, Alexander [Hebrew Univ. of Jerusalem (Israel); Phillips, Vaughan [Lund Univ. (Sweden); Pinsky, Mark [Hebrew Univ. of Jerusalem (Israel); Lynn, Barry [Hebrew Univ. of Jerusalem (Israel)

2016-12-20

The main achievements reached under the DOE award DE-SC0006788 are described. It is shown that the plan of the Project is completed. Unique results concerning cloud-aerosol interaction are obtained. It is shown that aerosols affect intensity of hurricanes. The effects of small aerosols on formation of ice in anvils of deep convective clouds are discovered, for the first time the mechanisms of drizzle formation are found and described quantitatively. Mechanisms of formation of warm rain are clarified and the dominating role of adiabatic processes and turbulence are stressed. Important results concerning the effects of sea spray on intensity of clouds and tropical cyclones are obtained. A novel methods of calculation of hail formation has been developed and implemented.

Dissolution process of atmospheric aerosol particles into cloud droplets; Processus de dissolution des aerosols atmospheriques au sein des gouttes d'eau nuageuses

Energy Technology Data Exchange (ETDEWEB)

Desboeufs, K.

2001-01-15

Clouds affect both climate via the role they play in the Earth's radiation balance and tropospheric chemistry since they are efficient reaction media for chemical transformation of soluble species. Cloud droplets are formed in the atmosphere by condensation of water vapour onto aerosol particles, the cloud condensation nuclei (CCN). The water soluble fraction of these CCN governs the cloud micro-physics, which is the paramount factor playing on the radiative properties of clouds. Moreover, this soluble fraction is the source of species imply in the oxidation/reduction reactions in the aqueous phase. Thus, it is of particular importance to understand the process controlling the solubilization of aerosols in the cloud droplets. The main purpose of this work is to investigate experimentally and theoretically the dissolution of particles incorporated in the aqueous phase. From the studies conducted up to now, we have identify several factors playing on the dissolution reaction of aerosols. However, the quantification of the effects of these factors is difficult since the current means of study are not adapted to the complexity of cloud systems. First, this work consisted to perform a experimental system, compound by an open flow reactor, enabling to follow the kinetic of dissolution in conditions representative of cloud. This experimental device is used to a systematic characterisation of the known factors playing on the dissolution, i.e. pH, aerosol nature, aerosol weathering... and also for the identification and the quantification of the effects of other factors: ionic strength, acid nature, clouds processes. These experiments gave quantitative results, which are used to elaborate a simple model of aerosol dissolution in the aqueous phase. This model considers the main factors playing on the dissolution and results in a general mechanism of aerosol dissolution extrapolated to the cloud droplets. (author)

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

Science.gov (United States)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

2018-01-01

species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

Science.gov (United States)

Yahya, Khairunnisa; Glotfelty, Timothy; Wang, Kai; Zhang, Yang; Nenes, Athanasios

2017-06-01

Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem) version 3.7.1. The existing Volatility Basis Set (VBS) treatments for organic aerosol (OA) formation in WRF/Chem are improved by considering the following: the secondary OA (SOA) formation from semi-volatile primary organic aerosol (POA), a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010) are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex) campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05) and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07) used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA) compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC) predictions (normalized mean biases from -40.8 % to a range of -34.6 to -27.7 %), with large differences between CB05-CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation parameterization based on the Fountoukis and Nenes

Theoretical studies on aerosol agglomeration processes

Energy Technology Data Exchange (ETDEWEB)

Lehtinen, K.E.J. [VTT Energy, Espoo (Finland). Energy Use

1997-12-31

In this thesis, theoretical modeling of certain aerosol systems has been presented. At first, the aerosol general dynamic equation is introduced, along with a discretization routine for its numerical solution. Of the various possible phenomena affecting aerosol behaviour, this work is mostly focused on aerosol agglomeration. The fundamentals of aerosol agglomeration theory are thus briefly reviewed. The two practical applications of agglomeration studied in this thesis are flue gas cleaning using an electrical agglomerator and nanomaterial synthesis with a free jet reactor. In an electrical agglomerator the aerosol particles are charged and brought into an alternating electric field. The aim is to remove submicron particles from flue gases by collisions with larger particles before conventional gas cleaning devices that have a clear penetration window in the problematic 0.1-1{mu}m size range. A mathematical model was constructed to find out the effects of the different system parameters on the agglomerator`s performance. A crucial part of this task was finding out the collision efficiencies of particles of varying size and charge. The original idea was to use unipolar charging of the particles, and a laboratory scale apparatus was constructed for this purpose. Both theory and experiments clearly show that significant removal of submicron particles can not be achieved by such an arrangement. The theoretical analysis further shows that if the submicron particles and the large collector particles were charged with opposite polarity, significant removal of the submicron particles could be obtained. The second application of agglomeration considered in this thesis is predicting/controlling nanoparticle size in the gas-to-particle aerosol route to material synthesis. In a typical material reactor, a precursor vapor reacts to form molecules of the desired material. In a cooling environment, a particulate phase forms, the dynamics of which are determined by the rates of

Theoretical studies on aerosol agglomeration processes

Energy Technology Data Exchange (ETDEWEB)

Lehtinen, K E.J. [VTT Energy, Espoo (Finland). Energy Use

1998-12-31

In this thesis, theoretical modeling of certain aerosol systems has been presented. At first, the aerosol general dynamic equation is introduced, along with a discretization routine for its numerical solution. Of the various possible phenomena affecting aerosol behaviour, this work is mostly focused on aerosol agglomeration. The fundamentals of aerosol agglomeration theory are thus briefly reviewed. The two practical applications of agglomeration studied in this thesis are flue gas cleaning using an electrical agglomerator and nanomaterial synthesis with a free jet reactor. In an electrical agglomerator the aerosol particles are charged and brought into an alternating electric field. The aim is to remove submicron particles from flue gases by collisions with larger particles before conventional gas cleaning devices that have a clear penetration window in the problematic 0.1-1{mu}m size range. A mathematical model was constructed to find out the effects of the different system parameters on the agglomerator`s performance. A crucial part of this task was finding out the collision efficiencies of particles of varying size and charge. The original idea was to use unipolar charging of the particles, and a laboratory scale apparatus was constructed for this purpose. Both theory and experiments clearly show that significant removal of submicron particles can not be achieved by such an arrangement. The theoretical analysis further shows that if the submicron particles and the large collector particles were charged with opposite polarity, significant removal of the submicron particles could be obtained. The second application of agglomeration considered in this thesis is predicting/controlling nanoparticle size in the gas-to-particle aerosol route to material synthesis. In a typical material reactor, a precursor vapor reacts to form molecules of the desired material. In a cooling environment, a particulate phase forms, the dynamics of which are determined by the rates of

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

Directory of Open Access Journals (Sweden)

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

The Pasadena Aerosol Characterization Observatory (PACO: chemical and physical analysis of the Western Los Angeles basin aerosol

Directory of Open Access Journals (Sweden)

S. P. Hersey

2011-08-01

in accumulation mode aerosol, while afternoon SOA production coincides with the appearance of a distinct fine mode dominated by organics. Particulate NH₄NO₃ and (NH₄₂SO₄ appear to be NH₃-limited in regimes I and II, but a significant excess of particulate NH₄⁺ in the hot, dry regime III suggests less SO₄²⁻ and the presence of either organic amines or NH₄⁺-associated organic acids. C-ToF-AMS data were analyzed by Positive Matrix Factorization (PMF, which resolved three factors, corresponding to a hydrocarbon-like OA (HOA, semivolatile OOA (SV-OOA, and low-volatility OOA (LV-OOA. HOA appears to be a periodic plume source, while SV-OOA exhibits a strong diurnal pattern correlating with ozone. Peaks in SV-OOA concentration correspond to peaks in DMA number concentration and the appearance of a fine organic mode. LV-OOA appears to be an aged accumulation mode constituent that may be associated with aqueous-phase processing, correlating strongly with sulfate and representing the dominant background organic component. Periods characterized by high SV-OOA and LV-OOA were analyzed by filter analysis, revealing a complex mixture of species during periods dominated by SV-OOA and LV-OOA, with LV-OOA periods characterized by shorter-chain dicarboxylic acids (higher O:C ratio, as well as appreciable amounts of nitrate- and sulfate-substituted organics. Phthalic acid was ubiquitous in filter samples, suggesting that PAH photochemistry may be an important SOA pathway in Los Angeles. Aerosol composition was related to water uptake characteristics, and it is concluded that hygroscopicity is largely controlled by organic mass fraction (OMF. The hygroscopicity parameter κ averaged 0.31 ± 0.08, approaching 0.5 at low OMF and 0.1 at high OMF, with increasing OMF suppressing hygroscopic growth and increasing critical dry diameter for CCN activation

Regional Climate Effects of Aerosols Over South Asia: a Synthesis of Hybrid-Synergistic Analysis

Science.gov (United States)

Subba, T.; Gogoi, M. M.; Pathak, B.; Bhuyan, P. K.

2017-12-01

The south-Asian region faces formidable challenges in the accurate estimation of the aerosol-climate forcing due to the increasing demographic pressure and the rapid socio-economic growth which intensify the anthropogenic emissions causing degradation of regional air quality and climate. In this context, the present study employs a hybrid-method synergizing the aerosol data from ground-based measurements, satellite retrievals and radiative transfer simulations over the south-Asian region. The ground based aerosol and solar radiation data (2010-2015) are considered for nine selected locations of India as well as the adjoining Bay of Bengal representing distinct aerosol environment. The land use land cover (LULC) data from Indian remote sensing satellite (IRS-P6) is used to understand the association of aerosol environment with the change in the land surface pattern.The results indicate that the northern part, pre-dominantly the Indo-Gangetic plains (IGP) experiences the highest aerosol optical depth throughout the year. While the presence of dust plays a significant role in modifying the radiation balance over the west Asian region, extending to IGP; the highest Fire Radiative Power is observed over Eastern India ( 30 MW), the hotspot of biomass burning sources, followed by Central, South/West and Northern India. Considering the distinct source processes, incoming ground reaching fluxes are simulated using radiative transfer model, which showed a good correlation with the measured values (R2 0.97) with the mean bias errors between -40 to +7 Wm-2 (an overestimation of 2-4%). Estimated aerosol direct radiative forcing efficiency (DRFE) is highest over the eastern IGP due to heavy loading of long range transported aerosols from the arid region in the west, followed by the Himalayan foothills and west-Asian regions which are mostly dominated by agro-industrial and dust activities. However, a pristine high altitude location in the Western Ghats showed lower DRFE compared

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V M; Hillamo, R; Maekinen, M; Virkkula, A; Maekelae, T; Pakkanen, T [Helsinki Univ. (Finland). Dept. of Physics

1997-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

1996-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

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

Science.gov (United States)

Qureshi, Asif; MacLeod, Matthew; Hungerbühler, Konrad

2009-10-01

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

The fluorescence properties of aerosol larger than 0.8 μm in an urban and a PBA-dominated location

Science.gov (United States)

Gabey, A. M.; Stanley, W. R.; Gallagher, M. W.; Kaye, P. H.

2011-01-01

Dual-wavelength Ultraviolet light-induced fluorescence (UV-LIF) measurements were performed on ambient environmental aerosol in Manchester, UK (urban city centre, winter) and Borneo, Malaysia (remote, tropical), which are taken to represent environments with negligible and significant primary biological aerosol (PBA) influences, respectively. Single-particle fluorescence intensity and optical equivalent diameter were measured with a Wide Issue Bioaerosol Sensor, version 3 (WIBS3) in the diameter range 0.8 μm≤DP≤20 μm for 2-3 weeks and filters were analysed using energy dispersive X-ray (EDX) spectroscopy, which revealed mostly non-PBA dominated particle sizes larger than 1 μm in Manchester. The WIBS3 features three fluorescence channels: Fluorescence excited at 280 nm is recorded at 310-400 nm and 400-600 nm and fluorescence excited at 370 nm is detected at 400-600 nm. In Manchester the primary size mode of fluorescent and non-fluorescent material was at 1.2 μm. In Borneo non-fluorescent material peaked at 1.2 μm and fluorescent at 3-4 μm. The fluorescence intensity at 400-600 nm generally increased with DP at both sites, as did the 310-400 nm intensity in Borneo. In Manchester the 310-400 m fluorescence decreased at DP>4 μm, suggesting this channel offers additional discrimination between fluorescent particle types. Finally, the ratio of fluorescence intensity in two pairs of channels was investigated as a function of particle diameter and this varied significantly between the two environments, demonstrating that the fluorescent aerosol in each can in principle be distinguished using a combination of fluorescence and elastic scattering measurements.

Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

Science.gov (United States)

Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

2015-02-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

Aerosol light absorption and its measurement: A review

International Nuclear Information System (INIS)

Moosmueller, H.; Chakrabarty, R.K.; Arnott, W.P.

2009-01-01

Light absorption by aerosols contributes to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer. Besides the direct radiative effect, the heating can evaporate clouds and change the atmospheric dynamics. Aerosol light absorption in the atmosphere is dominated by black carbon (BC) with additional, significant contributions from the still poorly understood brown carbon and from mineral dust. Sources of these absorbing aerosols include biomass burning and other combustion processes and dust entrainment. For particles much smaller than the wavelength of incident light, absorption is proportional to the particle volume and mass. Absorption can be calculated with Mie theory for spherical particles and with more complicated numerical methods for other particle shapes. The quantitative measurement of aerosol light absorption is still a challenge. Simple, commonly used filter measurements are prone to measurement artifacts due to particle concentration and modification of particle and filter morphology upon particle deposition, optical interaction of deposited particles and filter medium, and poor angular integration of light scattered by deposited particles. In situ methods measure particle absorption with the particles in their natural suspended state and therefore are not prone to effects related to particle deposition and concentration on filters. Photoacoustic and refractive index-based measurements rely on the heating of particles during light absorption, which, for power-modulated light sources, causes an acoustic signal and modulation of the refractive index in the air surrounding the particles that can be quantified with a microphone and an interferometer, respectively. These methods may suffer from some interference due to light-induced particle evaporation. Laser-induced incandescence also monitors particle heating upon absorption, but heats absorbing particles to much higher temperatures to quantify BC mass

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

Science.gov (United States)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

organic aerosol (OOA) factors: a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). The MO-OOA dominated during the pre-monsoon period, whereas LO-OOA dominated during monsoon. The sensitivity of air mass transport during pre-monsoon with synoptic process was also evaluated with a 3-D chemical transport model.

An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten

Directory of Open Access Journals (Sweden)

P. Tunved

2004-01-01

Full Text Available Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E. Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing different stages of the aerosol lifecycle. The atmospheric aerosol size distributions were interpreted as belonging to fresh, intermediate and aged types of size distribution. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-Lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features that are likely to be related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability of the aerosol size distribution. Processing by clouds and precipitation is shown to be especially crucial in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions indicating signs of recent new particle formation (~30% of the observed size distributions represent the first stage in the lifecycle. Aging of the aerosol size distribution may follow two branches: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area in environments similar to the one studied.

Characterisation of radioactivity carrying aerosol in a mineral sand processing plant

International Nuclear Information System (INIS)

Jeffries, C.; Morawska, L.

1998-01-01

The techniques used to separate heavy mineral sand into mineral products produce a large amount of airborne particulate. Some of these particles are radioactive which is due to the thorium and, to a lesser extent, the uranium content of mineral sands. This study has investigated both the radioactive and respirable particle components (<10 μm) of the aerosol in a dry sand processing plant in Brisbane, Australia. A number of different measurement techniques have been used to characterise the aerosol in the plant. The mass, number and activity distributions have been determined by an eight stage cascade impactor and an Aerodynamic Particle Sizer (APS) with both instruments measuring 0.4 to 10 μm. Measurements of radon progeny concentrations and the extent of radon progeny attachment to micrometer sized particles has been investigated, as well as the extent of airborne thorium and uranium. The preliminary results from two sites are presented and comments are made on the relationship between total and radioactive aerosol

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

Directory of Open Access Journals (Sweden)

J. Wang

2016-07-01

, 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 bivariate polar plots show that the SV-OOA was formed locally, and the variations of hydrogen-to-carbon (H ∕ C and oxygen-to-carbon (O ∕ C ratios in the Van Krevelen space further suggests an evolution pathway of SV-OOA to LV-OOA. Our findings regarding springtime aerosol chemistry in Nanjing may have important implications for the air quality remediation in the densely populated regions.

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

Science.gov (United States)

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

2014-05-01

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

Aerosol optical properties and precipitable water vapor column in the atmosphere of Norway.

Science.gov (United States)

Muyimbwa, Dennis; Frette, Øyvind; Stamnes, Jakob J; Ssenyonga, Taddeo; Chen, Yi-Chun; Hamre, Børge

2015-02-20

Between February 2012 and April 2014, we measured and analyzed direct solar radiances at a ground-based station in Bergen, Norway. We discovered that the spectral aerosol optical thickness (AOT) and precipitable water vapor column (PWVC) retrieved from these measurements have a seasonal variation with highest values in summer and lowest values in winter. The highest value of the monthly median AOT at 440 nm of about 0.16 was measured in July and the lowest of about 0.04 was measured in December. The highest value of the monthly median PWVC of about 2.0 cm was measured in July and the lowest of about 0.4 cm was measured in December. We derived Ångström exponents that were used to deduce aerosol particle size distributions. We found that coarse-mode aerosol particles dominated most of the time during the measurement period, but fine-mode aerosol particles dominated during the winter seasons. The derived Ångström exponent values suggested that aerosols containing sea salt could have been dominating at this station during the measurement period.

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

Science.gov (United States)

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

2016-12-01

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

Origins of atmospheric aerosols. Basic concepts on aerosol main physical properties; L`aerosol atmospherique: ses origines quelques notions sur les principales proprietes physiques des aerosols

Energy Technology Data Exchange (ETDEWEB)

Renoux, A. [Paris-12 Univ., 94 - Creteil (France). Laboratoire de Physique des aerosols et de transferts des contaminations

1996-12-31

Natural and anthropogenic sources of atmospheric aerosols are reviewed and indications of their concentrations and granulometry are given. Calculation of the lifetime of an atmospheric aerosol of a certain size is presented and the various modes of aerosol granulometry and their relations with photochemical and physico-chemical processes in the atmosphere are discussed. The main physical, electrical and optical properties of aerosols are also presented: diffusion coefficient, dynamic mobility and relaxation time, Stokes number, limit rate of fall, electrical mobility, optical diffraction

Elucidating dominant pathways of the nano-particle self-assembly process.

Science.gov (United States)

Zeng, Xiangze; Li, Bin; Qiao, Qin; Zhu, Lizhe; Lu, Zhong-Yuan; Huang, Xuhui

2016-09-14

Self-assembly processes play a key role in the fabrication of functional nano-structures with widespread application in drug delivery and micro-reactors. In addition to the thermodynamics, the kinetics of the self-assembled nano-structures also play an important role in determining the formed structures. However, as the self-assembly process is often highly heterogeneous, systematic elucidation of the dominant kinetic pathways of self-assembly is challenging. Here, based on mass flow, we developed a new method for the construction of kinetic network models and applied it to identify the dominant kinetic pathways for the self-assembly of star-like block copolymers. We found that the dominant pathways are controlled by two competing kinetic parameters: the encounter time Te, characterizing the frequency of collision and the transition time Tt for the aggregate morphology change from rod to sphere. Interestingly, two distinct self-assembly mechanisms, diffusion of an individual copolymer into the aggregate core and membrane closure, both appear at different stages (with different values of Tt) of a single self-assembly process. In particular, the diffusion mechanism dominates the middle-sized semi-vesicle formation stage (with large Tt), while the membrane closure mechanism dominates the large-sized vesicle formation stage (with small Tt). Through the rational design of the hydrophibicity of the copolymer, we successfully tuned the transition time Tt and altered the dominant self-assembly pathways.

Rapid Measurements of Aerosol Size Distribution and Hygroscopic Growth via Image Processing with a Fast Integrated Mobility Spectrometer (FIMS)

Science.gov (United States)

Wang, Y.; Pinterich, T.; Spielman, S. R.; Hering, S. V.; Wang, J.

2017-12-01

Aerosol size distribution and hygroscopicity are among key parameters in determining the impact of atmospheric aerosols on global radiation and climate change. In situ submicron aerosol size distribution measurements commonly involve a scanning mobility particle sizer (SMPS). The SMPS scanning time is in the scale of minutes, which is often too slow to capture the variation of aerosol size distribution, such as for aerosols formed via nucleation processes or measurements onboard research aircraft. To solve this problem, a Fast Integrated Mobility Spectrometer (FIMS) based on image processing was developed for rapid measurements of aerosol size distributions from 10 to 500 nm. The FIMS consists of a parallel plate classifier, a condenser, and a CCD detector array. Inside the classifier an electric field separates charged aerosols based on electrical mobilities. Upon exiting the classifier, the aerosols pass through a three stage growth channel (Pinterich et al. 2017; Spielman et al. 2017), where aerosols as small as 7 nm are enlarged to above 1 μm through water or heptanol condensation. Finally, the grown aerosols are illuminated by a laser sheet and imaged onto a CCD array. The images provide both aerosol concentration and position, which directly relate to the aerosol size distribution. By this simultaneous measurement of aerosols with different sizes, the FIMS provides aerosol size spectra nearly 100 times faster than the SMPS. Recent deployment onboard research aircraft demonstrated that the FIMS is capable of measuring aerosol size distributions in 1s (Figure), thereby offering a great advantage in applications requiring high time resolution (Wang et al. 2016). In addition, the coupling of the FIMS with other conventional aerosol instruments provides orders of magnitude more rapid characterization of aerosol optical and microphysical properties. For example, the combination of a differential mobility analyzer, a relative humidity control unit, and a FIMS was

A terrestrial ecosystem model (SOLVEG) coupled with atmospheric gas and aerosol exchange processes

International Nuclear Information System (INIS)

Katata, Genki; Ota, Masakazu

2017-01-01

In order to predict the impact of atmospheric pollutants (gases and aerosols) to the terrestrial ecosystem, new schemes for calculating the processes of dry deposition of gases and aerosols, and water and carbon cycles in terrestrial ecosystems were implemented in the one-dimensional atmosphere-SOiL-VEGetation model, SOLVEG. We made performance tests at various vegetation areas to validate the newly developed schemes. In this report, the detail in each modeled process is described with an instruction how to use the modified SOLVEG. The framework of 'terrestrial ecosystem model' was developed for investigation of a change in water, energy, and carbon cycles associated with global warming and air pollution and its impact on terrestrial ecosystems. (author)

Uncertainty from the choice of microphysics scheme in convection-permitting models significantly exceeds aerosol effects

Directory of Open Access Journals (Sweden)

B. White

2017-10-01

Full Text Available This study investigates the hydrometeor development and response to cloud droplet number concentration (CDNC perturbations in convection-permitting model configurations. We present results from a real-data simulation of deep convection in the Congo basin, an idealised supercell case, and a warm-rain large-eddy simulation (LES. In each case we compare two frequently used double-moment bulk microphysics schemes and investigate the response to CDNC perturbations. We find that the variability among the two schemes, including the response to aerosol, differs widely between these cases. In all cases, differences in the simulated cloud morphology and precipitation are found to be significantly greater between the microphysics schemes than due to CDNC perturbations within each scheme. Further, we show that the response of the hydrometeors to CDNC perturbations differs strongly not only between microphysics schemes, but the inter-scheme variability also differs between cases of convection. Sensitivity tests show that the representation of autoconversion is the dominant factor that drives differences in rain production between the microphysics schemes in the idealised precipitating shallow cumulus case and in a subregion of the Congo basin simulations dominated by liquid-phase processes. In this region, rain mass is also shown to be relatively insensitive to the radiative effects of an overlying layer of ice-phase cloud. The conversion of cloud ice to snow is the process responsible for differences in cold cloud bias between the schemes in the Congo. In the idealised supercell case, thermodynamic impacts on the storm system using different microphysics parameterisations can equal those due to aerosol effects. These results highlight the large uncertainty in cloud and precipitation responses to aerosol in convection-permitting simulations and have important implications not only for process studies of aerosol–convection interaction, but also for

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

Aerosol Size and Chemical Composition in the Canadian High Arctic

Science.gov (United States)

Chang, R. Y. W.; Hayes, P. L.; Leaitch, W. R.; Croft, B.; O'Neill, N. T.; Fogal, P.; Drummond, J. R.; Sloan, J. J.

2015-12-01

Arctic aerosol have a strong annual cycle, with winter months dominated by long range transport from lower latitudes resulting in high mass loadings. Conversely, local emissions are more prominent in the summer months because of the decreased influence of transported aerosol, allowing us to regularly observe both transported and local aerosol. This study will present observations of aerosol chemical composition and particle number size distribution collected at the Polar Environment Artic Research Laboratory and the Alert Global Atmospheric Watch Observatory at Eureka (80N, 86W) and Alert (82N, 62W), Nunavut, respectively. Summer time observations of the number size distribution reveal a persistent mode of particles centered between 30-50 nm, with occasional bursts of smaller particles. The non-refractory aerosol chemical composition, measured by the Canadian Network for the Detection of Atmospheric Change quadrupole aerosol mass spectrometer, is primarily organic, with contributions from both aged and fresher organic aerosol. Factor analysis will be conducted to better understand these sources. The site at Eureka is more susceptible to long range transport since it is at the top of a mountain ridge (610 m above sea level) and will be compared to the site at Alert on an elevated plain (200 m above sea level). This will allow us to determine the relative contributions from processes and sources at the sites at different elevations. Comparisons with aerosol optical depth and GEOS-Chem model output will also be presented to put these surface measurements into context with the overlying and regional atmosphere. Results from this study contribute to our knowledge of aerosol in the high Arctic.

Modeling of the Wegener-Bergeron-Findeisen process-implications for aerosol indirect effects

International Nuclear Information System (INIS)

Storelvmo, T; Lohmann, U; Kristjansson, J E; Iversen, T; Kirkevaag, A; Seland, O

2008-01-01

A new parameterization of the Wegener-Bergeron-Findeisen (WBF) process has been developed, and implemented in the general circulation model CAM-Oslo. The new parameterization scheme has important implications for the process of phase transition in mixed-phase clouds. The new treatment of the WBF process replaces a previous formulation, in which the onset of the WBF effect depended on a threshold value of the mixing ratio of cloud ice. As no observational guidance for such a threshold value exists, the previous treatment added uncertainty to estimates of aerosol effects on mixed-phase clouds. The new scheme takes subgrid variability into account when simulating the WBF process, allowing for smoother phase transitions in mixed-phase clouds compared to the previous approach. The new parameterization yields a model state which gives reasonable agreement with observed quantities, allowing for calculations of aerosol effects on mixed-phase clouds involving a reduced number of tunable parameters. Furthermore, we find a significant sensitivity to perturbations in ice nuclei concentrations with the new parameterization, which leads to a reversal of the traditional cloud lifetime effect.

Optical properties of the urban aerosol and their relation to chemical composition

International Nuclear Information System (INIS)

Leaderer, B.P.; Stolwijk, J.A.J.

1980-01-01

Light extinction and resulting visibility degradation in an unsaturated precipitation-free atmosphere are determined by light absorption and scattering and are caused by a complex mix of natural components and anthropogenic pollutants. The paper reviews correlation studies relating light scattering and light extinction (visibility) to concentrations of sulfate mass, nitrate mass, the remainder of the mass, and in some cases organic aerosol mass, while accounting for variations in relative humidity. It is found that sulfate aerosol mass is the dominant chemical aerosol species affecting light scattering and extinction. The dominant effect of sulfate mass on light scattering and extinction, even when sulfates account for a relatively small fraction of the total mass, results from the fact that sulfates are secondary aerosols and are mostly found in the 0.1-1.0 micron size range

Chemical, physical, and optical evolution of biomass burning aerosols: a case study

Science.gov (United States)

Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

2011-02-01

In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

Effects of stratospheric aerosol surface processes on the LLNL two-dimensional zonally averaged model

International Nuclear Information System (INIS)

Connell, P.S.; Kinnison, D.E.; Wuebbles, D.J.; Burley, J.D.; Johnston, H.S.

1992-01-01

We have investigated the effects of incorporating representations of heterogeneous chemical processes associated with stratospheric sulfuric acid aerosol into the LLNL two-dimensional, zonally averaged, model of the troposphere and stratosphere. Using distributions of aerosol surface area and volume density derived from SAGE 11 satellite observations, we were primarily interested in changes in partitioning within the Cl- and N- families in the lower stratosphere, compared to a model including only gas phase photochemical reactions

Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

Science.gov (United States)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

Coupling aerosol-cloud-radiative processes in the WRF-Chem model: Investigating the radiative impact of elevated point sources

Directory of Open Access Journals (Sweden)

E. G. Chapman

2009-02-01

Full Text Available The local and regional influence of elevated point sources on summertime aerosol forcing and cloud-aerosol interactions in northeastern North America was investigated using the WRF-Chem community model. The direct effects of aerosols on incoming solar radiation were simulated using existing modules to relate aerosol sizes and chemical composition to aerosol optical properties. Indirect effects were simulated by adding a prognostic treatment of cloud droplet number and adding modules that activate aerosol particles to form cloud droplets, simulate aqueous-phase chemistry, and tie a two-moment treatment of cloud water (cloud water mass and cloud droplet number to precipitation and an existing radiation scheme. Fully interactive feedbacks thus were created within the modified model, with aerosols affecting cloud droplet number and cloud radiative properties, and clouds altering aerosol size and composition via aqueous processes, wet scavenging, and gas-phase-related photolytic processes. Comparisons of a baseline simulation with observations show that the model captured the general temporal cycle of aerosol optical depths (AODs and produced clouds of comparable thickness to observations at approximately the proper times and places. The model overpredicted SO₂ mixing ratios and PM_2.5 mass, but reproduced the range of observed SO₂ to sulfate aerosol ratios, suggesting that atmospheric oxidation processes leading to aerosol sulfate formation are captured in the model. The baseline simulation was compared to a sensitivity simulation in which all emissions at model levels above the surface layer were set to zero, thus removing stack emissions. Instantaneous, site-specific differences for aerosol and cloud related properties between the two simulations could be quite large, as removing above-surface emission sources influenced when and where clouds formed within the modeling domain. When summed spatially over the finest

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

Directory of Open Access Journals (Sweden)

J. Xu

2018-01-01

high-resolution mass spectra of OA identified two oxygenated organic aerosol (OOA factors: a less oxidized OOA (LO-OOA and a more oxidized OOA (MO-OOA. The MO-OOA dominated during the pre-monsoon period, whereas LO-OOA dominated during monsoon. The sensitivity of air mass transport during pre-monsoon with synoptic process was also evaluated with a 3-D chemical transport model.

Aerosol effects in radiation transfer

International Nuclear Information System (INIS)

Binenko, V.I.; Harshvardhan, H.

1993-01-01

The radiative properties and effects of aerosols are assessed for the following aerosol sources: relatively clean background aerosol, dust storms and dust outbreaks, anthropogenic pollution, and polluted cloud layers. Studies show it is the submicron aerosol fraction that plays a dominant radiative role in the atmosphere. The radiative effect of the aerosol depends not only on its loading but also on the underlying surface albedo and on solar zenith angle. It is only with highly reflecting surfaces such as Arctic ice that aerosols have a warming effect. Radiometric, microphysical, mineral composition, and refractive index measurements are presented for dust and in particular for the Saharan aerosol layer (SAL). Short-wave radiative heating of the atmosphere is caused by the SAL and is due mainly to absorption. However, the SAL does not contribute significantly to the long-wave thermal radiation budget. Field program studies of the radiative effects of aerosols are described. Anthropogenic aerosols deplete the incoming solar radiation. A case field study for a regional Ukrainian center is discussed. The urban aerosol causes a cooling of metropolitan centers, compared with outlying areas, during the day, which is followed by a warming trend at night. In another study, an increase in turbidity by a factor of 3 due to increased industrialization for Mexico City is noted, together with a drop in atmospheric transmission by 10% over a 50-year period. Numerous studies are cited that demonstrate that anthropogenic aerosols affect both the microphysical and radiative properties of clouds, which in turn affect regional climate. Particles acting as cloud nuclei are considered to have the greatest indirect effect on cloud absorptivity of short-wave radiation. Satellite observations show that low-level stratus clouds contaminated by ship exhaust at sea lead to an increase in cloud albedo

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

Science.gov (United States)

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

2017-12-01

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

Modeling the feedback between aerosol and boundary layer processes: a case study in Beijing, China.

Science.gov (United States)

Miao, Yucong; Liu, Shuhua; Zheng, Yijia; Wang, Shu

2016-02-01

Rapid development has led to frequent haze in Beijing. With mountains and sea surrounding Beijing, the pollution is found to be influenced by the mountain-plain breeze and sea-land breeze in complex ways. Meanwhile, the presence of aerosols may affect the surface energy balance and impact these boundary layer (BL) processes. The effects of BL processes on aerosol pollution and the feedback between aerosol and BL processes are not yet clearly understood. Thus, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to investigate the possible effects and feedbacks during a haze episode on 23 September 2011. Influenced by the onshore prevailing wind, sea-breeze, and upslope breeze, about 45% of surface particulate matter (PM)2.5 in Beijing are found to be contributed by its neighbor cities through regional transport. In the afternoon, the development of upslope breeze suppresses the growth of BL in Beijing by imposing a relatively low thermal stable layer above the BL, which exacerbates the pollution. Two kinds of feedback during the daytime are revealed as follows: (1) as the aerosols absorb and scatter the solar radiation, the surface net radiation and sensible heat flux are decreased, while BL temperature is increased, resulting in a more stable and shallower BL, which leads to a higher surface PM2.5 concentration in the morning and (2) in the afternoon, as the presence of aerosols increases the BL temperature over plains, the upslope breeze is weakened, and the boundary layer height (BLH) over Beijing is heightened, resulting in the decrease of the surface PM2.5 concentration there.

Quantifying enhancement in aerosol radiative forcing during ‘extreme aerosol days’ in summer at Delhi National Capital Region, India

Energy Technology Data Exchange (ETDEWEB)

Kumar, Sumant [School of Environmental Sciences, Jawaharlal Nehru University, New Delhi 110067 (India); Dey, Sagnik [Centre for Atmospheric Sciences, IIT Delhi, New Delhi 110016 (India); Srivastava, Arun [School of Environmental Sciences, Jawaharlal Nehru University, New Delhi 110067 (India)

2016-04-15

Changes in aerosol characteristics (spectral aerosol optical depth, AOD and composition) are examined during the transition from ‘relatively clean’ to ‘extreme’ aerosol days in the summer of 2012 at Delhi National Capital Region (NCR), India. AOD smaller than 0.54 (i.e. 12-year mean AOD − 1σ) represents ‘relatively clean’ days in Delhi during the summer. ‘Extreme’ days are defined by the condition when AOD{sub 0.5} exceeds 12-year mean AOD + 1 standard deviation (σ). Mean (± 1σ) AOD increases to 1.2 ± 0.12 along with a decrease of Angstrom Exponent from 0.54 ± 0.09 to 0.22 ± 0.12 during the ‘extreme’ days. Aerosol composition is inferred by fixing the number concentrations of various individual species through iterative tweaking when simulated (following Mie theory) AOD spectrum matches with the measured one. Contribution of coarse mode dust to aerosol mass increased from 76.8% (relatively clean) to 96.8% (extreme events), while the corresponding contributions to AOD{sub 0.5} increased from 35.0% to 70.8%. Spectrally increasing single scattering albedo (SSA) and CALIPSO aerosol sub-type information support the dominant presence of dust during the ‘extreme’ aerosol days. Aerosol direct radiative forcing (ADRF) at the top-of-the-atmosphere increases from 21.2 W m{sup −2} (relatively clean) to 56.6 W m{sup −2} (extreme), while the corresponding change in surface ADRF is from − 99.5 W m{sup −2} to − 153.5 W m{sup −2}. Coarse mode dust contributes 60.3% of the observed surface ADRF during the ‘extreme’ days. On the contrary, 0.4% mass fraction of black carbon (BC) translates into 13.1% contribution to AOD{sub 0.5} and 33.5% to surface ADRF during the ‘extreme’ days. The atmospheric heating rate increased by 75.1% from 1.7 K/day to 2.96 K/day during the ‘extreme’ days. - Graphical abstract: Deviation (in %) of aerosol properties from ‘relatively clean’ days to ‘extreme’ aerosol days. - Highlights: �

Ergodic averages via dominating processes

DEFF Research Database (Denmark)

Møller, Jesper; Mengersen, Kerrie

2006-01-01

We show how the mean of a monotone function (defined on a state space equipped with a partial ordering) can be estimated, using ergodic averages calculated from upper and lower dominating processes of a stationary irreducible Markov chain. In particular, we do not need to simulate the stationary...... Markov chain and we eliminate the problem of whether an appropriate burn-in is determined or not. Moreover, when a central limit theorem applies, we show how confidence intervals for the mean can be estimated by bounding the asymptotic variance of the ergodic average based on the equilibrium chain....

Sources of anions in aerosols in northeast Greenland during late winter

DEFF Research Database (Denmark)

Lauridsen, Marlene Fenger; Sørensen, Lise Lotte; Kristensen, Kasper

2013-01-01

−4 is by far the dominating anion accounting for 50–85% of the analyzed mass. The analysis suggests that Cl− and NO−3 in coarser particles (> 1.5 μm) originate from local/regional sources. Under conditions where the air mass is transported over sea ice at high wind speeds, very coarse particles (> 18 μm...... ), respectively. The aerosols in late winter/early spring, after polar sunrise, are found to be a mixture of long-range transported and regional to local originating aerosols. Fine particles, smaller than 1 μm, containing SO2−4 , Cl− and NO− 3 , are hypothesized to originate from long-range transport, where SO2......The knowledge of climate effects of atmospheric aerosols is associated with large uncertainty, and a better understanding of their physical and chemical properties is needed, especially in the Arctic environment. The objective of the present study is to improve our understanding of the processes...

Organic condensation - a vital link connecting aerosol formation to climate forcing

Science.gov (United States)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-01-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Clarifying the dominant sources and mechanisms of cirrus cloud formation.

Science.gov (United States)

Cziczo, Daniel J; Froyd, Karl D; Hoose, Corinna; Jensen, Eric J; Diao, Minghui; Zondlo, Mark A; Smith, Jessica B; Twohy, Cynthia H; Murphy, Daniel M

2013-06-14

Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated. Our results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent. Further, composition analysis combined with relative humidity measurements suggests that heterogeneous freezing was the dominant formation mechanism of these clouds.

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

Directory of Open Access Journals (Sweden)

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.

Interaction of Microphysical Aerosol Processes with Hydrodynamics Mixing

KAUST Repository

Alshaarawi, Amjad

2015-12-15

This work is concerned with the interaction between condensing aerosol dynamics and hydrodynamic mixing within ow configurations in which aerosol particles form (nucleate) from a supersaturated vapor and supersaturation is induced by the mixing of two streams (a saturated stream and a cold one). Two canonical hydrodynamic configurations are proposed for the investigation. The First is the steady one-dimensional opposed-ow configuration. The setup consists of the two (saturated and cold) streams owing from opposite nozzles. A mixing layer is established across a stagnation plane in the center where nucleation and other aerosol dynamics are triggered. The second is homogeneous isotropic turbulence in a three-dimensional periodic domain. Patches of a hot saturated gas mix with patches of a cold one. A mixing layer forms across the growing interface where the aerosol dynamics of interest occur. In both configurations, a unique analogy is observed. The results reveal a complex response to variations in the mixing rates. Depending on the mixing rate, the response of the number density falls into one of two regimes. For fast mixing rates, the maximum reached number density of the condensing droplets increases with the hydrodynamic time. We refer to this as the nucleation regime. On the contrary, for low mixing rates, the maximum reached number density decreases with the hydrodynamic time. We refer to this as the consumption regime. It is shown that vapor scavenging by the aerosol phase is key to explaining the transition between these two regimes.

Identification of aerosol types over an urban site based on air-mass trajectory classification

Science.gov (United States)

Pawar, G. V.; Devara, P. C. S.; Aher, G. R.

2015-10-01

Columnar aerosol properties retrieved from MICROTOPS II Sun Photometer measurements during 2010-2013 over Pune (18°32‧N; 73°49‧E, 559 m amsl), a tropical urban station in India, are analyzed to identify aerosol types in the atmospheric column. Identification/classification is carried out on the basis of dominant airflow patterns, and the method of discrimination of aerosol types on the basis of relation between aerosol optical depth (AOD500 nm) and Ångström exponent (AE, α). Five potential advection pathways viz., NW/N, SW/S, N, SE/E and L have been identified over the observing site by employing the NOAA-HYSPLIT air mass back trajectory analysis. Based on AE against AOD500 nm scatter plot and advection pathways followed five major aerosol types viz., continental average (CA), marine continental average (MCA), urban/industrial and biomass burning (UB), desert dust (DD) and indeterminate or mixed type (MT) have been identified. In winter, sector SE/E, a representative of air masses traversed over Bay of Bengal and Eastern continental Indian region has relatively small AOD (τpλ = 0.43 ± 0.13) and high AE (α = 1.19 ± 0.15). These values imply the presence of accumulation/sub-micron size anthropogenic aerosols. During pre-monsoon, aerosols from the NW/N sector have high AOD (τpλ = 0.61 ± 0.21), and low AE (α = 0.54 ± 0.14) indicating an increase in the loading of coarse-mode particles over Pune. Dominance of UB type in winter season for all the years (i.e. 2010-2013) may be attributed to both local/transported aerosols. During pre-monsoon seasons, MT is the dominant aerosol type followed by UB and DD, while the background aerosols are insignificant.

Identification of secondary aerosol precursors emitted by an aircraft turbofan

Science.gov (United States)

Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

2018-05-01

Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Climate Impacts From a Removal of Anthropogenic Aerosol Emissions

Science.gov (United States)

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

2018-01-01

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

Evolution of Asian aerosols during transpacific transport in INTEX-B

Energy Technology Data Exchange (ETDEWEB)

Dunlea, E. J.; DeCarlo, Peter; Aiken, Allison; Kimmel, Joel; Peltier, R. E.; Weber, R. J.; Tomlinson, Jason M.; Collins, Donald R.; Shinozuka, Yohei; McNaughton, C. S.; Howell, S. G.; Clarke, A. D.; Emmons, L.; Apel, Eric; Pfister, G. G.; van Donkelaar, A.; Martin, R. V.; Millet, D. B.; Heald, C. L.; Jimenez, J. L.

2009-10-01

Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B 5 (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to 10 be a robust tracer for air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). 15 Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, 20 the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of SOA mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary 25 organic aerosol formation in the free troposphere.

Detection of a gas flaring signature in the AERONET optical properties of aerosols at a tropical station in West Africa

Science.gov (United States)

Fawole, Olusegun G.; Cai, Xiaoming; Levine, James G.; Pinker, Rachel T.; MacKenzie, A. R.

2016-12-01

The West African region, with its peculiar climate and atmospheric dynamics, is a prominent source of aerosols. Reliable and long-term in situ measurements of aerosol properties are not readily available across the region. In this study, Version 2 Level 1.5 Aerosol Robotic Network (AERONET) data were used to study the absorption and size distribution properties of aerosols from dominant sources identified by trajectory analysis. The trajectory analysis was used to define four sources of aerosols over a 10 year period. Sorting the AERONET aerosol retrievals by these putative sources, the hypothesis that there exists an optically distinct gas flaring signal was tested. Dominance of each source cluster varies with season: desert-dust (DD) and biomass burning (BB) aerosols are dominant in months prior to the West African Monsoon (WAM); urban (UB) and gas flaring (GF) aerosol are dominant during the WAM months. BB aerosol, with single scattering albedo (SSA) at 675 nm value of 0.86 ± 0.03 and GF aerosol with SSA (675 nm) value of 0.9 ± 0.07, is the most absorbing of the aerosol categories. The range of Absorption Angstr&öm Exponent (AAE) for DD, BB, UB and GF classes are 1.99 ± 0.35, 1.45 ± 0.26, 1.21 ± 0.38 and 0.98 ± 0.25, respectively, indicating different aerosol composition for each source. The AAE (440-870 nm) and Angstr&öm Exponent (AE) (440-870 nm) relationships further show the spread and overlap of the variation of these optical and microphysical properties, presumably due in part to similarity in the sources of aerosols and in part, due to mixing of air parcels from different sources en route to the measurement site.

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.

On the Scattering Properties of Urban and Maritime Aerosols and its ...

African Journals Online (AJOL)

The scattering properties of aerosols play a dominant role in radiative energy transfer and consequently influencing the visibility and turbidity in the atmosphere. In the present attempt, calculations for scattered intensity have been made in case of urban and maritime aerosols in the varying conditions of relative humidity.

Does temperature nudging overwhelm aerosol radiative ...

Science.gov (United States)

For over two decades, data assimilation (popularly known as nudging) methods have been used for improving regional weather and climate simulations by reducing model biases in meteorological parameters and processes. Similar practice is also popular in many regional integrated meteorology-air quality models that include aerosol direct and indirect effects. However in such multi-modeling systems, temperature changes due to nudging can compete with temperature changes induced by radiatively active & hygroscopic short-lived tracers leading to interesting dilemmas: From weather and climate prediction’s (retrospective or future) point of view when nudging is continuously applied, is there any real added benefit of using such complex and computationally expensive regional integrated modeling systems? What are the relative sizes of these two competing forces? To address these intriguing questions, we convert temperature changes due to nudging into radiative fluxes (referred to as the pseudo radiative forcing, PRF) at the surface and troposphere, and compare the net PRF with the reported aerosol radiative forcing. Results indicate that the PRF at surface dominates PRF at top of the atmosphere (i.e., the net). Also, the net PRF is about 2-4 times larger than estimated aerosol radiative forcing at regional scales while it is significantly larger at local scales. These results also show large surface forcing errors at many polluted urban sites. Thus, operational c

Characterization of biogenic secondary organic aerosols using statistical methods; Charakterisierung Biogener Sekundaerer Organischer Aerosole mit Statistischen Methoden

Energy Technology Data Exchange (ETDEWEB)

Spindler, Christian

2010-07-01

Atmospheric aerosols have important influence on the radiation balance of the Earth, on visibility and human health. Secondary organic aerosol is formed from gas-to-particle conversion of oxidized volatile organic compounds. A dominant fraction of the gases originates from plant emissions, making biogenic secondary organic aerosol (BSOA) an especially important constituent of the atmosphere. Knowing the chemical composition of BSOA particles is crucial for a thorough understanding of aerosol processes in the environment. In this work, the chemical composition of BSOA particles was measured with aerosol mass spectrometry and analyzed with statistical methods. The experimental part of the work comprises process studies of the formation and aging of biogenic aerosols in simulation chambers. Using a plant chamber, real tree emissions were used to produce particles in a way close to conditions in forest environments. In the outdoor chamber SAPHIR, OH-radicals were produced from the photooxidation of ozone under illumination with natural sunlight. Here, BSOA was produced from defined mixtures of mono- and sesquiterpenes that represent boreal forest emissions. A third kind of experiments was performed in the indoor chamber AIDA. Here, particles were produced from ozonolysis of single monoterpenes and aged by condensing OH-oxidation products. Two aerosol mass spectrometers (AMS) were used to measure the chemical composition of the particles. One of the instruments is equipped with a quadrupole mass spectrometer providing unit mass resolution. The second instrument contains a time-of-flight mass spectrometer and provides mass resolution sufficient to distinguish different fragments with the same nominal mass. Aerosol mass spectra obtained with these instruments are strongly fragmented due to electron impact ionization of the evaporated molecules. In addition, typical BSOA mass spectra are very similar to each other. In order to get a more detailed knowledge about the mass

Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

Directory of Open Access Journals (Sweden)

Abhijit Chatterjee

Full Text Available BACKGROUND: There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. METHODOLOGY/PRINCIPAL FINDINGS: An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl, latitude 27 degrees 01'N and longitude 88 degrees 15'E, a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3 and 19.6+/-11.1 microg m(-3 respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4NO(3 in fine mode aerosol during winter and as NaNO(3 in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2 during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4(2- in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. CONCLUSIONS/SIGNIFICANCE: The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over

Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

Science.gov (United States)

Chatterjee, Abhijit; Adak, Anandamay; Singh, Ajay K; Srivastava, Manoj K; Ghosh, Sanjay K; Tiwari, Suresh; Devara, Panuganti C S; Raha, Sibaji

2010-06-16

There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl), latitude 27 degrees 01'N and longitude 88 degrees 15'E), a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3) and 19.6+/-11.1 microg m(-3) respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4)NO(3) in fine mode aerosol during winter and as NaNO(3) in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2) during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4)(2-) in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over northeastern Himalayas, and should be useful to policy makers in making control

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

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

2014-12-01

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

Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

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L. Hildebrandt

2011-12-01

Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O₃, NO_x and NO_y concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

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

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Strada, Susanna; Unger, Nadine

2016-04-01

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

Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

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K. Yahya

2017-06-01

Full Text Available Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem version 3.7.1. The existing Volatility Basis Set (VBS treatments for organic aerosol (OA formation in WRF/Chem are improved by considering the following: the secondary OA (SOA formation from semi-volatile primary organic aerosol (POA, a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010 are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05 and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07 used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC predictions (normalized mean biases from −40.8 % to a range of −34.6 to −27.7 %, with large differences between CB05–CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation

Sources of carbonaceous aerosol in the Amazon basin

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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

Ground-based aerosol characterization during the South American Biomass Burning Analysis (SAMBBA field experiment

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J. Brito

2014-11-01

aerosol processing (O : C ≅ 0.25 to O : C ≅ 0.6, no remarkable change is observed in the H : C ratio (~1.35. Such a result contrasts strongly with previous observations of chemical ageing of both urban and Amazonian biogenic aerosols. At higher levels of processing (O : C > 0.6, the H : C ratio changes with a H : C / O : C slope of −0.5, possibly due to the development of a combination of BB (H : C / O : C slope = 0 and biogenic (H : C /O :C slope =−1 organic aerosol (OA. An analysis of the ΔOA /ΔCO mass ratios yields very little enhancement in the OA loading with atmospheric processing, consistent with previous observations. These results indicate that negligible secondary organic aerosol (SOA formation occurs throughout the observed BB plume processing, or that SOA formation is almost entirely balanced by OA volatilization. Positive matrix factorization (PMF of the organic aerosol spectra resulted in three factors: fresh BBOA, aged BBOA, and low-volatility oxygenated organic aerosol (LV-OOA. Analysis of the diurnal patterns and correlation with external markers indicates that during the first part of the campaign, OA concentrations are impacted by local fire plumes with some chemical processing occurring in the near-surface layer. During the second part of the campaign, long-range transport of BB plumes above the surface layer, as well as potential SOAs formed aloft, dominates OA concentrations at our ground-based sampling site. This manuscript describes the first ground-based deployment of the aerosol mass spectrometry at a site heavily impacted by biomass burning in the Amazon region, allowing a deeper understanding of aerosol life cycle in this important ecosystem.

Modelling aerosol behavior in reactor cooling systems

International Nuclear Information System (INIS)

McDonald, B.H.

1990-01-01

This paper presents an overview of some of the areas of concern in using computer codes to model fission-product aerosol behavior in the reactor cooling system (RCS) of a water-cooled nuclear reactor during a loss-of-coolant accident. The basic physical processes that require modelling include: fission product release and aerosol formation in the reactor core, aerosol transport and deposition in the reactor core and throughout the rest of the RCS, and the interaction between aerosol transport processes and the thermalhydraulics. In addition to these basic physical processes, chemical reactions can have a large influence on the nature of the aerosol and its behavior in the RCS. The focus is on the physics and the implications of numerical methods used in the computer codes to model aerosol behavior in the RCS

Fission product vapour - aerosol interactions in the containment: simulant fuel studies

International Nuclear Information System (INIS)

Beard, A.M.; Benson, C.G.; Bowsher, B.R.

1988-12-01

Experiments have been conducted in the Falcon facility to study the interaction of fission product vapours released from simulant fuel samples with control rod aerosols. The aerosols generated from both the control rod and fuel sample were chemically distinct and had different deposition characteristics. Extensive interaction was observed between the fission product vapours and the control rod aerosol. The two dominant mechanisms were condensation of the vapours onto the aerosol, and chemical reactions between the two components; sorption phenomena were believed to be only of secondary importance. The interaction of fission product vapours and reactor materials aerosols could have a major impact on the transport characteristics of the radioactive emission from a degrading core. (author)

Substantial convection and precipitation enhancements by ultrafine aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; Giangrande, Scott E.; Li, Zhanqing; Machado, Luiz A. T.; Martin, Scot T.; Yang, Yan; Wang, Jian; Artaxo, Paulo; Barbosa, Henrique M. J.; Braga, Ramon C.; Comstock, Jennifer M.; Feng, Zhe; Gao, Wenhua; Gomes, Helber B.; Mei, Fan; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; de Souza, Rodrigo A. F.

2018-01-25

Aerosol-cloud interaction remains the largest uncertainty in climate projections. Ultrafine aerosol particles (UAP; size <50nm) are considered too small to serve as cloud condensation nuclei conventionally. However, this study provides observational evidence to accompany insights from numerical simulations to support that deep convective clouds (DCCs) over Amazon have strong capability of nucleating UAP from an urban source and forming greater numbers of droplets, because fast drop coalescence in these DCCs reduces drop surface area available for condensation, leading to high vapor supersaturation. The additional droplets subsequently decrease supersaturation and release more condensational latent heating, a dominant contributor to convection intensification, whereas enhanced latent heat from ice-related processes plays a secondary role. Therefore, the addition of anthropogenic UAP may play a much greater role in modulating clouds than previously believed over the Amazon region and possibly in other relatively pristine regions such as maritime and forest locations.

Analysis of aerosol absorption properties and transport over North Africa and the Middle East using AERONET data

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A. Farahat

2016-11-01

Full Text Available In this paper particle categorization and absorption properties were discussed to understand transport mechanisms at different geographic locations and possible radiative impacts on climate. The long-term Aerosol Robotic Network (AERONET data set (1999–2015 is used to estimate aerosol optical depth (AOD, single scattering albedo (SSA, and the absorption Ångström exponent (αabs at eight locations in North Africa and the Middle East. Average variation in SSA is calculated at four wavelengths (440, 675, 870, and 1020 nm, and the relationship between aerosol absorption and physical properties is used to infer dominant aerosol types at different locations. It was found that seasonality and geographic location play a major role in identifying dominant aerosol types at each location. Analyzing aerosol characteristics among different sites using AERONET Version 2, Level 2.0 data retrievals and the Hybrid Single Particle Lagrangian Integrated Trajectory model (HYSPLIT backward trajectories shows possible aerosol particle transport among different locations indicating the importance of understanding transport mechanisms in identifying aerosol sources.

Constraining Aerosol-Cloud-Precipitation Interactions of Orographic Mixed-Phase Clouds with Trajectory Budgets

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Glassmeier, F.; Lohmann, U.

2016-12-01

Orographic precipitation is prone to strong aerosol-cloud-precipitation interactions because the time for precipitation development is limited to the ascending section of mountain flow. At the same time, cloud microphysical development is constraint by the strong dynamical forcing of the orography. In this contribution, we discuss how changes in the amount and composition of droplet- and ice-forming aerosols influence precipitation in idealized simulations of stratiform orographic mixed-phase clouds. We find that aerosol perturbations trigger compensating responses of different precipitation formation pathways. The effect of aerosols is thus buffered. We explain this buffering by the requirement to fulfill aerosol-independent dynamical constraints. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with a bell-shaped mountain. The model is coupled to a 2-moment warm and cold cloud microphysics scheme. Activation and freezing rates are parameterized based on prescribed aerosol fields that are varied in number, size and composition. Our analysis is based on the budget of droplet water along trajectories of cloud parcels. The budget equates condensation as source term with precipitation formation from autoconversion, accretion, riming and the Wegener-Bergeron-Findeisen process as sink terms. Condensation, and consequently precipitation formation, is determined by dynamics and largely independent of the aerosol conditions. An aerosol-induced change in the number of droplets or crystals perturbs the droplet budget by affecting precipitation formation processes. We observe that this perturbation triggers adjustments in liquid and ice water content that re-equilibrate the budget. As an example, an increase in crystal number triggers a stronger glaciation of the cloud and redistributes precipitation formation from collision-coalescence to riming and from riming to vapor deposition. We theoretically confirm the dominant effect of water

Cloud Processing of Secondary Organic Aerosol from Isoprene and Methacrolein Photooxidation.

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Giorio, Chiara; Monod, Anne; Brégonzio-Rozier, Lola; DeWitt, Helen Langley; Cazaunau, Mathieu; Temime-Roussel, Brice; Gratien, Aline; Michoud, Vincent; Pangui, Edouard; Ravier, Sylvain; Zielinski, Arthur T; Tapparo, Andrea; Vermeylen, Reinhilde; Claeys, Magda; Voisin, Didier; Kalberer, Markus; Doussin, Jean-François

2017-10-12

Aerosol-cloud interaction contributes to the largest uncertainties in the estimation and interpretation of the Earth's changing energy budget. The present study explores experimentally the impacts of water condensation-evaporation events, mimicking processes occurring in atmospheric clouds, on the molecular composition of secondary organic aerosol (SOA) from the photooxidation of methacrolein. A range of on- and off-line mass spectrometry techniques were used to obtain a detailed chemical characterization of SOA formed in control experiments in dry conditions, in triphasic experiments simulating gas-particle-cloud droplet interactions (starting from dry conditions and from 60% relative humidity (RH)), and in bulk aqueous-phase experiments. We observed that cloud events trigger fast SOA formation accompanied by evaporative losses. These evaporative losses decreased SOA concentration in the simulation chamber by 25-32% upon RH increase, while aqueous SOA was found to be metastable and slowly evaporated after cloud dissipation. In the simulation chamber, SOA composition measured with a high-resolution time-of-flight aerosol mass spectrometer, did not change during cloud events compared with high RH conditions (RH > 80%). In all experiments, off-line mass spectrometry techniques emphasize the critical role of 2-methylglyceric acid as a major product of isoprene chemistry, as an important contributor to the total SOA mass (15-20%) and as a key building block of oligomers found in the particulate phase. Interestingly, the comparison between the series of oligomers obtained from experiments performed under different conditions show a markedly different reactivity. In particular, long reaction times at high RH seem to create the conditions for aqueous-phase processing to occur in a more efficient manner than during two relatively short cloud events.

Identification of secondary aerosol precursors emitted by an aircraft turbofan

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D. Kılıç

2018-05-01

Full Text Available Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS for nonrefractory particulate matter (NR-PM1 were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5–7 %, more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

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

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J. N. Smith

2011-02-01

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

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.

Improvement of aerosol optical depth retrieval from MODIS spectral reflectance over the global ocean using new aerosol models archived from AERONET inversion data and tri-axial ellipsoidal dust database

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J. Lee

2012-08-01

Full Text Available New over-ocean aerosol models are developed by integrating the inversion data from the Aerosol Robotic Network (AERONET sun/sky radiometers with a database for the optical properties of tri-axial ellipsoid particles. The new aerosol models allow more accurate retrieval of aerosol optical depth (AOD from the Moderate Resolution Imaging Spectroradiometer (MODIS in the case of high AOD (AOD > 0.3. The aerosol models are categorized by using the fine-mode fraction (FMF at 550 nm and the single-scattering albedo (SSA at 440 nm from the AERONET inversion data to include a variety of aerosol types found around the globe. For each aerosol model, the changes in the aerosol optical properties (AOPs as functions of AOD are considered to better represent aerosol characteristics. Comparisons of AODs between AERONET and MODIS for the period from 2003 to 2010 show that the use of the new aerosol models enhances the AOD accuracy with a Pearson coefficient of 0.93 and a regression slope of 0.99 compared to 0.92 and 0.85 calculated using the MODIS Collection 5 data. Moreover, the percentage of data within an expected error of ± (0.03 + 0.05 × AOD is increased from 62% to 64% for overall data and from 39% to 5% for AOD > 0.3. Errors in the retrieved AOD are further characterized with respect to the Ångström exponent (AE, scattering angle (Θ, SSA, and air mass factor (AMF. Due to more realistic AOPs assumptions, the new algorithm generally reduces systematic errors in the retrieved AODs compared with the current operational algorithm. In particular, the underestimation of fine-dominated AOD and the scattering angle dependence of dust-dominated AOD are significantly mitigated as results of the new algorithm's improved treatment of aerosol size distribution and dust particle nonsphericity.

Improvement of Aerosol Optical Depth Retrieval from MODIS Spectral Reflectance over the Global Ocean Using New Aerosol Models Archived from AERONET Inversion Data and Tri-axial Ellipsoidal Dust Database

Science.gov (United States)

Lee, J.; Kim, J.; Yang, P.; Hsu, N. C.

2012-01-01

New over-ocean aerosol models are developed by integrating the inversion data from the Aerosol Robotic Network (AERONET) sun/sky radiometers with a database for the optical properties of tri-axial ellipsoid particles. The new aerosol models allow more accurate retrieval of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) in the case of high AOD (AOD greater than 0.3). The aerosol models are categorized by using the fine-mode fraction (FMF) at 550 nm and the singlescattering albedo (SSA) at 440 nm from the AERONET inversion data to include a variety of aerosol types found around the globe. For each aerosol model, the changes in the aerosol optical properties (AOPs) as functions of AOD are considered to better represent aerosol characteristics. Comparisons of AODs between AERONET and MODIS for the period from 2003 to 2010 show that the use of the new aerosol models enhances the AOD accuracy with a Pearson coefficient of 0.93 and a regression slope of 0.99 compared to 0.92 and 0.85 calculated using the MODIS Collection 5 data. Moreover, the percentage of data within an expected error of +/-(0.03 + 0.05xAOD) is increased from 62 percent to 64 percent for overall data and from 39 percent to 51 percent for AOD greater than 0.3. Errors in the retrieved AOD are further characterized with respect to the Angstrom exponent (AE), scattering angle, SSA, and air mass factor (AMF). Due to more realistic AOPs assumptions, the new algorithm generally reduces systematic errors in the retrieved AODs compared with the current operational algorithm. In particular, the underestimation of fine-dominated AOD and the scattering angle dependence of dust-dominated AOD are significantly mitigated as results of the new algorithm's improved treatment of aerosol size distribution and dust particle nonsphericity.

Project Overview: Cumulus Humilis Aerosol Processing Study (CHAPS): Proposed Summer 2007 ASP Field Campaign

Energy Technology Data Exchange (ETDEWEB)

Berkowitz, Carl M.; Berg, Larry K.; Ogren, J. A.; Hostetler, Chris A.; Ferrare, Richard

2006-05-18

This white paper presents the scientific motivation and preliminary logistical plans for a proposed ASP field campaign to be carried out in the summer of 2007. The primary objective of this campaign is to use the DOE Gulfstream-1 aircraft to make measurements characterizing the chemical, physical and optical properties of aerosols below, within and above large fields of fair weather cumulus and to use the NASA Langley Research Center’s High Spectral Resolution Lidar (HSRL) to make independent measurements of aerosol backscatter and extinction profiles in the vicinity of these fields. Separate from the science questions to be addressed by these observations will be information to add in the development of a parameterized cumulus scheme capable of including multiple cloud fields within a regional or global scale model. We will also be able to compare and contrast the cloud and aerosol properties within and outside the Oklahoma City plume to study aerosol processes within individual clouds. Preliminary discussions with the Cloud and Land Surface Interaction Campaign (CLASIC) science team have identified overlap between the science questions posed for the CLASIC Intensive Operation Period (IOP) and the proposed ASP campaign, suggesting collaboration would benefit both teams.

Towards simplification of hydrologic modeling: identification of dominant processes

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S. L. Markstrom

2016-11-01

Full Text Available parameter hydrologic model, has been applied to the conterminous US (CONUS. Parameter sensitivity analysis was used to identify: (1 the sensitive input parameters and (2 particular model output variables that could be associated with the dominant hydrologic process(es. Sensitivity values of 35 PRMS calibration parameters were computed using the Fourier amplitude sensitivity test procedure on 110 000 independent hydrologically based spatial modeling units covering the CONUS and then summarized to process (snowmelt, surface runoff, infiltration, soil moisture, evapotranspiration, interflow, baseflow, and runoff and model performance statistic (mean, coefficient of variation, and autoregressive lag 1. Identified parameters and processes provide insight into model performance at the location of each unit and allow the modeler to identify the most dominant process on the basis of which processes are associated with the most sensitive parameters. The results of this study indicate that: (1 the choice of performance statistic and output variables has a strong influence on parameter sensitivity, (2 the apparent model complexity to the modeler can be reduced by focusing on those processes that are associated with sensitive parameters and disregarding those that are not, (3 different processes require different numbers of parameters for simulation, and (4 some sensitive parameters influence only one hydrologic process, while others may influence many.

Towards simplification of hydrologic modeling: Identification of dominant processes

Science.gov (United States)

Markstrom, Steven; Hay, Lauren E.; Clark, Martyn P.

2016-01-01

The Precipitation–Runoff Modeling System (PRMS), a distributed-parameter hydrologic model, has been applied to the conterminous US (CONUS). Parameter sensitivity analysis was used to identify: (1) the sensitive input parameters and (2) particular model output variables that could be associated with the dominant hydrologic process(es). Sensitivity values of 35 PRMS calibration parameters were computed using the Fourier amplitude sensitivity test procedure on 110 000 independent hydrologically based spatial modeling units covering the CONUS and then summarized to process (snowmelt, surface runoff, infiltration, soil moisture, evapotranspiration, interflow, baseflow, and runoff) and model performance statistic (mean, coefficient of variation, and autoregressive lag 1). Identified parameters and processes provide insight into model performance at the location of each unit and allow the modeler to identify the most dominant process on the basis of which processes are associated with the most sensitive parameters. The results of this study indicate that: (1) the choice of performance statistic and output variables has a strong influence on parameter sensitivity, (2) the apparent model complexity to the modeler can be reduced by focusing on those processes that are associated with sensitive parameters and disregarding those that are not, (3) different processes require different numbers of parameters for simulation, and (4) some sensitive parameters influence only one hydrologic process, while others may influence many

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

Science.gov (United States)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

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

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S. Strada

2016-04-01

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

Aerosol composition and its sources at the King Sejong Station, Antarctic peninsula

Science.gov (United States)

Mishra, Vinit K.; Kim, Ki-Hyun; Hong, Sungmin; Lee, Khanghyun

The annual cycles of major metals and ions in suspended particulate matters (SPM) have been investigated at a costal site of the Antarctic Peninsula in order to elucidate temporal variations as well as major source processes responsible for their formation. The measurements had been performed from January 2000 to December 2001 at the Korean Antarctic research station, 'King Sejong' (62°13' S, 58°47' W). The observed time series of important aerosol components showed clear seasonal variation patterns, while the mean elemental concentrations (e.g., 1875 (Al), 10.3 (Ba), 0.3 (Bi), 1.3 (Cd), 1.7 pg m -3 (Co)) were generally compatible with those reported previously. The presence of high EF values with respect to both mean crustal and seawater composition (such as Bi, Cd, Cr, Cu, Ni, V, and Zn), however, suggests a possibly important role of anthropogenic processes in this remote site. In contrast, the concentrations of ionic species were not clearly distinguishable from those of other Antarctic sites; but the consideration of ionic mass balance between cations and anions pointed out the uniqueness of their source/sink processes in the study area. The major source processes of those aerosol components were also investigated using a series of statistical analyses. The overall results of our study indicated the dominance of several processes (or sources) such as sea-salt emission, secondary aerosol formation, and anthropogenic pollution from both local and distant sources.

Insight into Chemistry on Cloud/Aerosol Water Surfaces.

Science.gov (United States)

Zhong, Jie; Kumar, Manoj; Francisco, Joseph S; Zeng, Xiao Cheng

2018-05-15

, whereas on a water surface, the HNO 3 -mediated stepwise hydration of anti-CH 3 CHOO is dominantly observed. The high surface/volume ratio of interfacial water molecules at the aerosol water surface can significantly lower the energy barriers for the proton transfer reactions in the atmosphere. Such catalysis by the aerosol water surface is shown to cause the barrier-less formation of ammonium bisulfate from hydrated NH 3 and SO 3 molecules rather than from the reaction of H 2 SO 4 with NH 3 . Finally, an aerosol water droplet is a polar solvent, which would favorably interact with high polarity substrates. This can accelerate interconversion of different conformers (e.g., anti and syn) of atmospheric species, such as glyoxal, depending on their polarity. The results discussed here enable an improved understanding of atmospheric processes on the aerosol water surface.

Antarctic aerosols - A review

Science.gov (United States)

Shaw, Glenn E.

1988-02-01

Tropospheric aerosols with the diameter range of half a micron reside in the atmosphere for tens of days and teleconnect Antarctica with other regions by transport that reaches planetary scales of distances; thus, the aerosol on the Antarctic ice represents 'memory modules' of events that took place at regions separated from Antarctica by tens of thousands of kilometers. In terms of aerosol mass, the aerosol species include insoluble crustal products (less than 5 percent), transported sea-salt residues (highly variable but averaging about 10 percent), Ni-rich meteoric material, and anomalously enriched material with an unknown origin. Most (70-90 percent by mass) of the aerosol over the Antarctic ice shield, however, is the 'natural acid sulfate aerosol', apparently deriving from biological processes taking place in the surrounding oceans.

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2007-09-30

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Tropospheric Aerosols

Science.gov (United States)

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

2003-12-01

�m, PM10=1.1 μg m-3; estimated coefficient of light scattering by particulate matter, σep, at 570 nm=12 Mm-1). (b) High aerosol concentration (PM2.5=43.9 μg m-3; PM10=83.4 μg m-3; estimated σep at 570 nm=245 Mm-1) (reproduced by permission of National Park Service, 2002). Although comprising only a small fraction of the mass of Earth's atmosphere, aerosol particles are highly important constituents of the atmosphere. Special interest has focused on aerosols in the troposphere, the lowest part of the atmosphere, extending from the land or ocean surface typically to ˜8 km at high latitudes, ˜12 km in mid-latitudes, and ˜16 km at low latitudes. That interest arises in large part because of the importance of aerosol particles in geophysical processes, human health impairment through inhalation, environmental effects through deposition, visibility degradation, and influences on atmospheric radiation and climate.Anthropogenic aerosols are thought to exert a substantial influence on Earth's climate, and the need to quantify this influence has sparked much of the current interest in and research on tropospheric aerosols. The principal mechanisms by which aerosols influence the Earth radiation budget are scattering and absorbing solar radiation (the so-called "direct effects") and modifying clouds and precipitation, thereby affecting both radiation and hydrology (the so-called "indirect effects"). Light scattering by aerosols increases the brightness of the planet, producing a cooling influence. Light-absorbing aerosols such as black carbon exert a warming influence. Aerosols increase the reflectivity of clouds, another cooling influence. These radiative influences are quantified as forcings, where a forcing is a perturbation to the energy balance of the atmosphere-Earth system, expressed in units of watts per square meter, W m-2. A warming influence is denoted a positive forcing, and a cooling influence, negative. The radiative direct and indirect forcings by

Aerosol physical and optical properties in the Eastern Mediterranean Basin, Crete, from Aerosol Robotic Network data

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A. Fotiadi

2006-01-01

Full Text Available In this study, we investigate the aerosol optical properties, namely aerosol extinction optical thickness (AOT, Angström parameter and size distribution over the Eastern Mediterranean Basin, using spectral measurements from the recently established FORTH (Foundation for Research and Technology-Hellas AERONET station in Crete, for the two-year period 2003–2004. The location of the FORTH-AERONET station offers a unique opportunity to monitor aerosols from different sources. Maximum values of AOT are found primarily in spring, which together with small values of the Angström parameter indicate dust transported from African deserts, whereas the minimum values of AOT occur in winter. In autumn, large AOT values observed at near-infrared wavelengths arise also from dust transport. In summer, large AOT values at ultraviolet (340 nm and visible wavelengths (500 nm, together with large values of the Angström parameter, are associated with transport of fine aerosols of urban/industrial and biomass burning origin. The Angström parameter values vary on a daily basis within the range 0.05–2.20, and on a monthly basis within the range 0.68–1.9. This behaviour, together with broad frequency distributions and back-trajectory analyses, indicates a great variety of aerosol types over the study region including dust, urban-industrial and biomass-burning pollution, and maritime, as well as mixed aerosol types. Large temporal variability is observed in AOT, Angström parameter, aerosol content and size. The fine and coarse aerosol modes persist throughout the year, with the coarse mode dominant except in summer. The highest values of AOT are related primarily to southeasterly winds, associated with coarse aerosols, and to a less extent to northwesterly winds associated with fine aerosols. The results of this study show that the FORTH AERONET station in Crete is well suited for studying the transport and mixing of different types of aerosols from a variety

[Microphysics of atmospheric aerosols during winter haze/fog events in Nanjing].

Science.gov (United States)

Yang, Jun; Niu, Zhong-qing; Shi, Chun-e; Liu, Duan-yang; Li, Zi-hua

2010-07-01

Intensive field observations of fog/haze events, including simultaneous measurements of aerosol particle and fog droplet size distributions, were conducted in Nanjing in November, 2007. Four weather conditions (fog, mist, wet haze and haze) were distinguished based on visibility and liquid water content firstly. Then, the microphysical characteristics of coarse and fine particles in each condition were investigated. The results showed the dominant sequence of the four weather conditions was hazemist-->wet haze-->fog-->, wet haze-->misthaze. The lasting time of pre-fog wet haze was longer than that of post-fog wet haze. The number, surface area and volume concentration of coarse particles with diameter larger than 2.0 micron in fog were much higher than those in the other three conditions, and the smallest concentrations were observed in haze. The size distributions of surface area and volume concentration exhibited multi-peak in fog droplets, while it showed single peak for coarse particles in haze, mist and wet haze. For the fine particles with diameter larger than 0.010 microm, the spectral shapes of surface area concentration are similar in fog (mist) and wet haze (haze) condition. The dominant size ranges of fine particle number concentration were in 0.04-0.13 microm and 0.02-0.14 microm for fog and wet haze, separately. The same dominant size ranges located in 0.02-0.06 microm for both mist and haze. During the transition processes from haze, mist and wet haze to fog, the concentration of smaller particles (less than 0.060-0.090 microm) reduced and vice versa for the corresponding larger particles. Temporal variation of aerosol number concentration correlated well with the root mean diameters negatively during the observation period. The number concentration of aerosol was the lowest and the mean diameter was the largest in fog periods.

Summer/winter variability of the surfactants in aerosols from Grenoble, France

Science.gov (United States)

Baduel, Christine; Nozière, Barbara; Jaffrezo, Jean-Luc

2012-02-01

Many atmospheric aerosols seem to contain strong organic surfactants likely to enhance their cloud-forming properties. Yet, few techniques allow for the identification and characterization of these compounds. Recently, we introduced a double extraction method to isolate the surfactant fraction of atmospheric aerosol samples, and evidenced their very low surface tension (≤30 mN m -1). In this work, this analytical procedure was further optimized. In addition to an optimized extraction and a reduction of the analytical time, the improved method led to a high reproducibility in the surface tension curves obtained (shapes and minimal values), illustrated by the low uncertainties on the values, ±10% or less. The improved method was applied to PM 10 aerosols from the urban area of Grenoble, France collected from June 2009 to January 2010. Significant variability was observed between the samples. The minimum surface tension obtained from the summer samples was systematically lower (30 mN m -1) than that of the winter samples (35-45 mN m -1). Sharp transitions in the curves together with the very low surface tensions suggested that the dominating surfactants in the summer samples were biosurfactants, which would be consistent with the high biogenic activity in that season. One group of samples from the winter also displayed sharp transitions, which, together with the slightly higher surface tension, suggested the presence of weaker, possibly man-made, surfactants. A second group of curves from the winter did not display any clear transition but were similar to those of macromolecular surfactants such as polysaccharides or humic substances from wood burning. These surfactants are thus likely to originate from wood burning, the dominating source for aerosols in Grenoble in winter. These observations thus confirm the presence of surfactants from combustion processes in urban aerosols reported by other groups and illustrates the ability of our method to distinguish between

Lab-scale development of a high temperature aerosol particle sampling probe system for field measurements in thermochemical conversion of biomass

Energy Technology Data Exchange (ETDEWEB)

Lindskog, M.; Malik, A.; Pagels, J.; Sanati, M. [Lund Univ., Lund (Sweden). Div. of Ergonomics and Aerosol Technology

2010-07-01

Thermochemical conversion of biomass requires both combustion in an oxygen rich environment and gasification in an oxygen deficient environment. Therefore, the mass concentration of fly ash from combustion processes is dominated by inorganic compounds, and the particulate matter obtained from gasification is dominated by carbonaceous compounds. The fine fly ash particles can initiate corrosion and fouling and also increases emissions of fine particulates to the atmosphere. This study involved the design of a laboratory scale setup consisting of a high temperature sampling probe and an aerosol generation system to study the formation of fine particle from biomass gasification processes. An aerosol model system using potassium chloride (KCl) as the ash compound and Di Octyl Sebacate oil (DOS) as the volatile organic part was used to test the high temperature sampling probe. Tests conducted at 200 degrees C showed good reproducibility of the aerosol generator. The tests also demonstrated suitable dilution ratios which enabled the denuder to absorb all of the gaseous organic compounds in the set up, thus enabling measurement of only the particle phase. Condensable organic concentrations of 1-68 mg/m{sup 3} were easily handled by the high temperature sampling probe system, indicating that the denuder worked well. Additional tests will be performed using an Aerosol Mass Spectrometer (AMST) to verify that the denuder can capture all of the gaseous organic compounds also when condensed onto agglomerated soot particles. 6 refs., 1 tab., 9 figs.

Classification of aerosol properties derived from AERONET direct sun data

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G. P. Gobbi

2007-01-01

Full Text Available Aerosol spectral measurements by sunphotometers can be characterized by three independent pieces of information: 1 the optical thickness (AOT, a measure of the column aerosol concentration, 2 the optical thickness average spectral dependence, given by the Angstrom exponent (α, and 3 the spectral curvature of α (δα. We propose a simple graphical method to visually convert (α, δα to the contribution of fine aerosol to the AOT and the size of the fine aerosols. This information can be used to track mixtures of pollution aerosol with dust, to distinguish aerosol growth from cloud contamination and to observe aerosol humidification. The graphical method is applied to the analysis of yearly records at 8 sites in 3 continents, characterized by different levels of pollution, biomass burning and mineral dust concentrations. Results depict the dominance of fine mode aerosols in driving the AOT at polluted sites. In stable meteorological conditions, we see an increase in the size of the fine aerosol as the pollution stagnates and increases in optical thickness. Coexistence of coarse and fine particles is evidenced at the polluted sites downwind of arid regions.

Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

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L. Deguillaume

2008-07-01

Full Text Available This paper discusses the influence of primary biological aerosols (PBA on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

Impact of varying lidar measurement and data processing techniques in evaluating cirrus cloud and aerosol direct radiative effects

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S. Lolli

2018-03-01

Full Text Available In the past 2 decades, ground-based lidar networks have drastically increased in scope and relevance, thanks primarily to the advent of lidar observations from space and their need for validation. Lidar observations of aerosol and cloud geometrical, optical and microphysical atmospheric properties are subsequently used to evaluate their direct radiative effects on climate. However, the retrievals are strongly dependent on the lidar instrument measurement technique and subsequent data processing methodologies. In this paper, we evaluate the discrepancies between the use of Raman and elastic lidar measurement techniques and corresponding data processing methods for two aerosol layers in the free troposphere and for two cirrus clouds with different optical depths. Results show that the different lidar techniques are responsible for discrepancies in the model-derived direct radiative effects for biomass burning (0.05 W m−2 at surface and 0.007 W m−2 at top of the atmosphere and dust aerosol layers (0.7 W m−2 at surface and 0.85 W m−2 at top of the atmosphere. Data processing is further responsible for discrepancies in both thin (0.55 W m−2 at surface and 2.7 W m−2 at top of the atmosphere and opaque (7.7 W m−2 at surface and 11.8 W m−2 at top of the atmosphere cirrus clouds. Direct radiative effect discrepancies can be attributed to the larger variability of the lidar ratio for aerosols (20–150 sr than for clouds (20–35 sr. For this reason, the influence of the applied lidar technique plays a more fundamental role in aerosol monitoring because the lidar ratio must be retrieved with relatively high accuracy. In contrast, for cirrus clouds, with the lidar ratio being much less variable, the data processing is critical because smoothing it modifies the aerosol and cloud vertically resolved extinction profile that is used as input to compute direct radiative effect calculations.

Impact of varying lidar measurement and data processing techniques in evaluating cirrus cloud and aerosol direct radiative effects

Science.gov (United States)

Lolli, Simone; Madonna, Fabio; Rosoldi, Marco; Campbell, James R.; Welton, Ellsworth J.; Lewis, Jasper R.; Gu, Yu; Pappalardo, Gelsomina

2018-03-01

In the past 2 decades, ground-based lidar networks have drastically increased in scope and relevance, thanks primarily to the advent of lidar observations from space and their need for validation. Lidar observations of aerosol and cloud geometrical, optical and microphysical atmospheric properties are subsequently used to evaluate their direct radiative effects on climate. However, the retrievals are strongly dependent on the lidar instrument measurement technique and subsequent data processing methodologies. In this paper, we evaluate the discrepancies between the use of Raman and elastic lidar measurement techniques and corresponding data processing methods for two aerosol layers in the free troposphere and for two cirrus clouds with different optical depths. Results show that the different lidar techniques are responsible for discrepancies in the model-derived direct radiative effects for biomass burning (0.05 W m-2 at surface and 0.007 W m-2 at top of the atmosphere) and dust aerosol layers (0.7 W m-2 at surface and 0.85 W m-2 at top of the atmosphere). Data processing is further responsible for discrepancies in both thin (0.55 W m-2 at surface and 2.7 W m-2 at top of the atmosphere) and opaque (7.7 W m-2 at surface and 11.8 W m-2 at top of the atmosphere) cirrus clouds. Direct radiative effect discrepancies can be attributed to the larger variability of the lidar ratio for aerosols (20-150 sr) than for clouds (20-35 sr). For this reason, the influence of the applied lidar technique plays a more fundamental role in aerosol monitoring because the lidar ratio must be retrieved with relatively high accuracy. In contrast, for cirrus clouds, with the lidar ratio being much less variable, the data processing is critical because smoothing it modifies the aerosol and cloud vertically resolved extinction profile that is used as input to compute direct radiative effect calculations.

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

Science.gov (United States)

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

Climatology of Aerosol Optical Properties in Southern Africa

Science.gov (United States)

Queface, Antonio J.; Piketh, Stuart J.; Eck, Thomas F.; Tsay, Si-Chee

2011-01-01

A thorough regionally dependent understanding of optical properties of aerosols and their spatial and temporal distribution is required before we can accurately evaluate aerosol effects in the climate system. Long term measurements of aerosol optical depth, Angstrom exponent and retrieved single scattering albedo and size distribution, were analyzed and compiled into an aerosol optical properties climatology for southern Africa. Monitoring of aerosol parameters have been made by the AERONET program since the middle of the last decade in southern Africa. This valuable information provided an opportunity for understanding how aerosols of different types influence the regional radiation budget. Two long term sites, Mongu in Zambia and Skukuza in South Africa formed the core sources of data in this study. Results show that seasonal variation of aerosol optical thicknesses at 500 nm in southern Africa are characterized by low seasonal multi-month mean values (0.11 to 0.17) from December to May, medium values (0.20 to 0.27) between June and August, and high to very high values (0.30 to 0.46) during September to November. The spatial distribution of aerosol loadings shows that the north has high magnitudes than the south in the biomass burning season and the opposite in none biomass burning season. From the present aerosol data, no long term discernable trends are observable in aerosol concentrations in this region. This study also reveals that biomass burning aerosols contribute the bulk of the aerosol loading in August-October. Therefore if biomass burning could be controlled, southern Africa will experience a significant reduction in total atmospheric aerosol loading. In addition to that, aerosol volume size distribution is characterized by low concentrations in the non biomass burning period and well balanced particle size contributions of both coarse and fine modes. In contrast high concentrations are characteristic of biomass burning period, combined with

Global direct radiative forcing by process-parameterized aerosol optical properties

Science.gov (United States)

KirkevâG, Alf; Iversen, Trond

2002-10-01

A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

Nuclear aerosol behavior during reactor accidents

International Nuclear Information System (INIS)

Williams, M.M.R.

1990-01-01

Some early reactor accidents are recalled together with their associated environmental consequences. One such consequence is the generation of radioactive aerosol. We described the various physical processes that such an aerosol cloud undergoes within the secondary containment building. These physical processes are then brought together quantitatively in a balance equation for the aerosol size spectrum as a function of position and time. Methods for solving this equation are discussed and illustrated by the method of moments based upon log-normal and modified gamma distributions. Current problems are outlined and directions for future work into aerosol behavior are suggested. (author)

Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

Energy Technology Data Exchange (ETDEWEB)

Turner, David, D.; Ferrare, Richard, A.

2011-07-06

The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

AEROSOL VARIABILITY OBSERVED WITH RPAS

Directory of Open Access Journals (Sweden)

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.

Photochemical organonitrate formation in wet aerosols

Science.gov (United States)

Lim, Yong Bin; Kim, Hwajin; Kim, Jin Young; Turpin, Barbara J.

2016-10-01

Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal- and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NOx and O3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids) were formed in both ammonium sulfate (AS) aerosols and sulfuric acid (SA) aerosols. However, the major products were organonitrogens (CHNO), organosulfates (CHOS), and organonitrogen sulfates (CHNOS). These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH), two main products for both AS and SA aerosols were organonitrates, which appeared at m / z- 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NOx and OH during the irradiation.

Light extinction by aerosols during summer air pollution

Science.gov (United States)

Kaufman, Y. J.; Fraser, R. S.

1983-01-01

In order to utilize satellite measurements of optical thickness over land for estimating aerosol properties during air pollution episodes, the optical thickness was measured from the surface and investigated. Aerosol optical thicknesses have been derived from solar transmission measurements in eight spectral bands within the band lambda 440-870 nm during the summers of 1980 and 1981 near Washington, DC. The optical thicknesses for the eight bands are strongly correlated. It was found that first eigenvalue of the covariance matrix of all observations accounts for 99 percent of the trace of the matrix. Since the measured aerosol optical thickness was closely proportional to the wavelength raised to a power, the aerosol size distribution derived from it is proportional to the diameter (d) raised to a power for the range of diameters between 0.1 to 1.0 micron. This power is insensitive to the total optical thickness. Changes in the aerosol optical thickness depend on several aerosol parameters, but it is difficult to identify the dominant one. The effects of relative humidity and accumulation mode concentration on the optical thickness are analyzed theoretically, and compared with the measurements.

Estimating the maritime component of aerosol optical depth and its dependency on surface wind speed using satellite data

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Y. Lehahn

2010-07-01

Full Text Available Six years (2003–2008 of satellite measurements of aerosol parameters from the Moderate Resolution Imaging Spectroradiometer (MODIS and surface wind speeds from Quick Scatterometer (QuikSCAT, the Advanced Microwave Scanning Radiometer (AMSR-E, and the Special Sensor Microwave Imager (SSM/I, are used to provide a comprehensive perspective on the link between surface wind speed and marine aerosol optical depth over tropical and subtropical oceanic regions. A systematic comparison between the satellite derived fields in these regions allows to: (i separate the relative contribution of wind-induced marine aerosol to the aerosol optical depth; (ii extract an empirical linear equation linking coarse marine aerosol optical depth and wind intensity; and (iii identify a time scale for correlating marine aerosol optical depth and surface wind speed. The contribution of wind induced marine aerosol to aerosol optical depth is found to be dominated by the coarse mode elements. When wind intensity exceeds 4 m/s, coarse marine aerosol optical depth is linearly correlated with the surface wind speed, with a remarkably consistent slope of 0.009±0.002 s/m. A detailed time scale analysis shows that the linear correlation between the fields is well kept within a 12 h time frame, while sharply decreasing when the time lag between measurements is longer. The background aerosol optical depth, associated with aerosols that are not produced in-situ through wind driven processes, can be used for estimating the contributions of terrestrial and biogenic marine aerosol to over-ocean satellite retrievals of aerosol optical depth.

Overview and preliminary results of the Surface Ocean Aerosol Production (SOAP campaign

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C. S. Law

2017-11-01

, contaminant markers and a common aerosol inlet facilitated multi-sensor measurement of uncontaminated air. Aerosol characterization identified variable Aitken mode and consistent submicron-sized accumulation and coarse modes. Submicron aerosol mass was dominated by secondary particles containing ammonium sulfate/bisulfate under light winds, with an increase in sea salt under higher wind speeds. MBL measurements and chamber experiments identified a significant organic component in primary and secondary aerosols. Comparison of SOAP aerosol number and size distributions reveals an underprediction in GLOMAP (GLObal Model of Aerosol Processes-mode aerosol number in clean marine air masses, suggesting a missing marine aerosol source in the model. The SOAP data will be further examined for evidence of nucleation events and also to identify relationships between MBL composition and surface ocean biogeochemistry that may provide potential proxies for aerosol precursors and production.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

Science.gov (United States)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Dunne, Eimear M.; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S.; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A.; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty J.; Richards, Nigel A. D.; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S.

2016-10-01

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m-2 (27%) to -0.60 W m-2. Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation.

Science.gov (United States)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Dunne, Eimear M; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty J; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S

2016-10-25

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Dominant rate process of silicon surface etching by hydrogen chloride gas

International Nuclear Information System (INIS)

Habuka, Hitoshi; Suzuki, Takahiro; Yamamoto, Sunao; Nakamura, Akio; Takeuchi, Takashi; Aihara, Masahiko

2005-01-01

Silicon surface etching and its dominant rate process are studied using hydrogen chloride gas in a wide concentration range of 1-100% in ambient hydrogen at atmospheric pressure in a temperature range of 1023-1423 K, linked with the numerical calculation accounting for the transport phenomena and the surface chemical reaction in the entire reactor. The etch rate, the gaseous products and the surface morphology are experimentally evaluated. The dominant rate equation accounting for the first-order successive reactions at silicon surface by hydrogen chloride gas is shown to be valid. The activation energy of the dominant surface process is evaluated to be 1.5 x 10 5 J mol - 1 . The silicon deposition by the gaseous by-product, trichlorosilane, is shown to have a negligible influence on the silicon etch rate

Aerosol climatology over the Mexico City basin: Characterization of optical properties

Science.gov (United States)

Carabali, Giovanni; Estévez, Héctor Raúl; Valdés-Barrón, Mauro; Bonifaz-Alfonzo, Roberto; Riveros-Rosas, David; Velasco-Herrera, Víctor Manuel; Vázquez-Gálvez, Felipe Adrián

2017-09-01

Climatology of Aerosol Optical Depth (AOD), Single Scattering Albedo (SSA), and aerosol particle-size distribution were analyzed using a 15-year (1999-2014) dataset from AErosol RObotic NETwork (AERONET) observations over the Mexico City (MC) basin. The atmosphere over this site is dominated by two main aerosol types, represented by urban/industrial pollution and biomass-burning particles. Due to the specific meteorological conditions within the basin, seasons are usually classified into three as follows: Dry Winter (DW) (November-February); Dry Spring (DS) (March-April), and the RAiny season (RA) (May-October), which are mentioned throughout this article. Using a CIMEL sun photometer, we conducted continuous observations over the MC urban area from January 1999 to December 2014. Aerosol Optical Depth (AOD), Ångström exponent (α440-870), Single Scattering Albedo (SSA), and aerosol particle-size distribution were derived from the observational data. The overall mean AOD500 during the 1999-2014 period was 0.34 ± 0.07. The monthly mean AOD reached a maximal value of 0.49 in May and a minimal value of 0.27 in February and March. The average α440-870 value for the period studied was 1.50 ± 0.16. The monthly average of α440-870 reached a minimal value of 1.32 in August and a maximal value of 1.61 in May. Average SSA at 440 nm was 0.89 throughout the observation period, indicating that aerosols over Mexico City are composed mainly of absorptive particles. Concentrations of fine- and coarse-mode aerosols over MC were highest in DS season compared with other seasons, especially for particles with radii measuring between 0.1 and 0.2 μm. Results from the Spectral De-convolution Algorithm (SDA) show that fine-mode aerosols dominated AOD variability in MC. In the final part of this article, we present a classification of aerosols in MC by using the graphical method proposed by Gobbi et al. (2007), which is based on the combined analysis of α and its spectral curvature

Cluster analysis of the impact of air back-trajectories on aerosol optical properties at Hornsund, Spitsbergen

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A. Rozwadowska

2010-02-01

Full Text Available In this paper, spectra of aerosol optical thickness from the AERONET (AErosol RObotic NETwork station at Hornsund in the southern part of Spitsbergen were employed to study the impact of air mass history on aerosol optical thickness for wavelength λ=500 nm – AOT(500 – and the Ångström exponent. Backward trajectories computed, using the NOAA HYSPLIT model, were used to trace air history. It was found that in spring, the changes in AOT values over the Hornsund station were strongly influenced by air mass trajectories 8 days or longer in duration, arriving both in the free troposphere and at an altitude of 1 km above sea level. Nevertheless, free tropospheric advection was dominant. AOT variability in summer was best explained by the local direction and speed of advection (1-day trajectories and was dominated by the effectiveness of cleansing processes. During the ASTAR 2007 campaign, the aerosols near Hornsund displayed low AOT values ranging from 0.06 to 0.09, which is lower than the mean AOT(500 for spring seasons from 2005 to 2007 (0.110±0.007; mean ± standard deviation of mean. 9 April 2007 with AOT(500=0.147 was exceptional. The back-trajectories belonged to clusters with low and average cluster mean AOT. Apart from the maximum AOT of 9 April 2007, the observed AOT values were close to or lower than the means for the clusters to which they belonged.

Left hemispheric dominance of vestibular processing indicates lateralization of cortical functions in rats.

Science.gov (United States)

Best, Christoph; Lange, Elena; Buchholz, Hans-Georg; Schreckenberger, Mathias; Reuss, Stefan; Dieterich, Marianne

2014-11-01

Lateralization of cortical functions such as speech dominance, handedness and processing of vestibular information are present not only in humans but also in ontogenetic older species, e.g. rats. In human functional imaging studies, the processing of vestibular information was found to be correlated with the hemispherical dominance as determined by the handedness. It is located mainly within the right hemisphere in right handers and within the left hemisphere in left handers. Since dominance of vestibular processing is unknown in animals, our aim was to study the lateralization of cortical processing in a functional imaging study applying small-animal positron emission tomography (microPET) and galvanic vestibular stimulation in an in vivo rat model. The cortical and subcortical network processing vestibular information could be demonstrated and correlated with data from other animal studies. By calculating a lateralization index as well as flipped region of interest analyses, we found that the vestibular processing in rats follows a strong left hemispheric dominance independent from the "handedness" of the animals. These findings support the idea of an early hemispheric specialization of vestibular cortical functions in ontogenetic older species.

Influence of anthropogenic aerosol on solar radiation in Europe

Energy Technology Data Exchange (ETDEWEB)

Ten Brink, H M

1993-12-01

Backscatter of solar radiation by aerosol and the cooling thus induced, is the single largest uncertainty factor in assessing the climate effect of the greenhouse gases. The dominant reason for the uncertainty in the aerosol effect is its local nature. Therefore it is only via localized efforts that estimates can be improved. It is the aim of the present study to better assess the amount of solar radiation intercepted by aerosol, especially that of aerosol of anthropogenic origin in Europe. The assessment is realized along three interconnected approaches. First, empirical factors stemming from measurements in the US and used in the present estimates of the reflection of solar radiation by anthropogenic aerosol are checked for their validity in the European domain. Secondly, historical data on solar flux in Europe are related to the historic trend in aerosol loading. Finally, a sophisticated aerosol and cloud (radiation) module is developed for incorporation in a climate model. The radiation module uses aerosol characteristics as measured in the field and is validated via solar radiation measurements. The concerted investigation started in January 1993. The data obtained in the first phase of the study formed the basis for the definite detailed approach and will therefore be reported in this text. 1 fig., 9 refs.

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.

Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

Science.gov (United States)

Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.

2013-01-01

An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

Aerosol Production from Charbroiled and Wet-Fried Meats

Science.gov (United States)

Niedziela, R. F.; Blanc, L. E.

2012-12-01

Previous work in our laboratory focused on the chemical and optical characterization of aerosols produced during the dry-frying of different meat samples. This method yielded a complex ensemble of particles composed of water and long-chain fatty acids with the latter dominated by oleic, stearic, and palmitic acids. The present study examines how wet-frying and charbroiling cooking methods affect the physical and chemical properties of their derived aerosols. Samples of ground beef, salmon, chicken, and pork were subject to both cooking methods in the laboratory, with their respective aerosols swept into a laminar flow cell where they were optically analyzed in the mid-infrared and collected through a gas chromatography probe for chemical characterization. This presentation will compare and contrast the nature of the aerosols generated in each cooking method, particularly those produced during charbroiling which exposes the samples, and their drippings, to significantly higher temperatures. Characterization of such cooking-related aerosols is important because of the potential impact of these particles on air quality, particularly in urban areas.

Realization of nuclear track filters and their applications to the study of environmental aerosol samples

International Nuclear Information System (INIS)

Guo Shilun

1993-01-01

Detailed study of the behaviours of radon decay products requires the knowledge of environmental aerosols. A combination of devices and instruments have been tested to be superior in study of aerosol characteristics. Nuclear track filters and cascade track filter impactor are basic devices, which bring the functions of α -spectrometer, scanning electron microscope and electron microprobe into full play. This paper describes how to use these devices and instruments to collect aerosols, to determine aerosol radioactivity, size distribution and elemental compositions and to determine the concentration of aerosols in air as a function of aerosol sizes, which are important parameters in dominating the interactions between aerosol and radon decay products. (author). 15 refs, 7 figs

Examination of the potential impacts of dust and pollution aerosol acting as cloud nucleating aerosol on water resources in the Colorado River Basin

Science.gov (United States)

Jha, Vandana

In this study we examine the cumulative effect of dust acting as cloud nucleating aerosol (cloud condensation nuclei (CCN), giant cloud condensation nuclei (GCCN), and ice nuclei (IN)) along with anthropogenic aerosol pollution acting primarily as CCN, over the entire Colorado Rocky Mountains from the months of October to April in the year 2004-2005; the snow year. This ˜6.5 months analysis provides a range of snowfall totals and variability in dust and anthropogenic aerosol pollution. The specific objectives of this research is to quantify the impacts of both dust and pollution aerosols on wintertime precipitation in the Colorado Mountains using the Regional Atmospheric Modeling System (RAMS). In general, dust enhances precipitation primarily by acting as IN, while aerosol pollution reduces water resources in the CRB via the so-called "spill-over" effect, by enhancing cloud droplet concentrations and reducing riming rates. Dust is more episodic and aerosol pollution is more pervasive throughout the winter season. Combined response to dust and aerosol pollution is a net reduction of water resources in the CRB. The question is by how much are those water resources affected? Our best estimate is that total winter-season precipitation loss for for the CRB the 2004-2005 winter season due to the combined influence of aerosol pollution and dust is 5,380,00 acre-feet of water. Sensitivity studies for different cases have also been run for the specific cases in 2004-2005 winter season to analyze the impact of changing dust and aerosol ratios on precipitation in the Colorado River Basin. The dust is varied from 3 to 10 times in the experiments and the response is found to be non monotonic and depends on various environmental factors. The sensitivity studies show that adding dust in a wet system increases precipitation when IN affects are dominant. For a relatively dry system high concentrations of dust can result in over-seeding the clouds and reductions in precipitation

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.

PIXE investigation of aerosol composition over the Zambian Copperbelt

Science.gov (United States)

Meter, S. L.; Formenti, P.; Piketh, S. J.; Annegarn, H. J.; Kneen, M. A.

1999-04-01

Atmospheric sulphate aerosol concentrations are of interest in climate change studies because of their negative climate forcing potential. Quantification of their forcing strength requires the compilation of global sulphur emission inventories to determine the magnitude of regional sources. We report on measurements of the ambient aerosol concentrations in proximity to a copper refinery in the central African Copperbelt, along the border of Zambia and the Democratic Republic of the Congo. This region is historically regarded as one of the largest African sources of sulphate aerosols. Sulphate is produced by oxidation in the atmosphere of SO 2 emitted during the pyrometallurgical processing of Cu-Co sulphide ores. Since the last quantification of sulphur emissions (late 1960s), there has been large-scale reduction in copper production and more frequent use of the leaching technique with negligible sulphur emissions. Samples were collected over four weeks, November-December 1996, at Kitwe, Zambia. A low volume two-stage time-resolving aerosol sampler (streaker) was used. Coarse and fine mode aerosols were separated at >2.5 and >10 μmad. Hourly elemental concentrations were determined by 3.2 MeV PIXE, and routinely yielded Si, S, K, Ca, Ti, Mn, Fe, Cu and Zn, above detection limits. Si, K, Ca and Fe (major crustal components) dominated the coarse elemental mass. In the fine stage, S and Si accounted for up to 80% of the measured mass, and S alone up to 60%. Time series analysis allowed the division of sulphur and crustal elements (Si, K, Ca, Fe) between (i) background concentrations representative of synoptic scale air masses; and (ii) contributions from local sources, i.e., copper smelter and re-suspended soil dust. Short duration episodes of S concentrations, up to 26 μg/m 3, were found simultaneously with enhanced Cu, Fe and Zn. Contributions from individual pyrometallurgic processes and the cobalt slag dump could be distinguished from the elemental signatures

PIXE investigation of aerosol composition over the Zambian Copperbelt

International Nuclear Information System (INIS)

Meter, S.L.; Formenti, P.; Piketh, S.J.; Annegarn, H.J.; Kneen, M.A.

1999-01-01

Atmospheric sulphate aerosol concentrations are of interest in climate change studies because of their negative climate forcing potential. Quantification of their forcing strength requires the compilation of global sulphur emission inventories to determine the magnitude of regional sources. We report on measurements of the ambient aerosol concentrations in proximity to a copper refinery in the central African Copperbelt, along the border of Zambia and the Democratic Republic of the Congo. This region is historically regarded as one of the largest African sources of sulphate aerosols. Sulphate is produced by oxidation in the atmosphere of SO 2 emitted during the pyrometallurgical processing of Cu-Co sulphide ores. Since the last quantification of sulphur emissions (late 1960s), there has been large-scale reduction in copper production and more frequent use of the leaching technique with negligible sulphur emissions. Samples were collected over four weeks, November-December 1996, at Kitwe, Zambia. A low volume two-stage time-resolving aerosol sampler (streaker) was used. Coarse and fine mode aerosols were separated at >2.5 and >10 μmad. Hourly elemental concentrations were determined by 3.2 MeV PIXE, and routinely yielded Si, S, K, Ca, Ti, Mn, Fe, Cu and Zn, above detection limits. Si, K, Ca and Fe (major crustal components) dominated the coarse elemental mass. In the fine stage, S and Si accounted for up to 80% of the measured mass, and S alone up to 60%. Time series analysis allowed the division of sulphur and crustal elements (Si, K, Ca, Fe) between (i) background concentrations representative of synoptic scale air masses; and (ii) contributions from local sources, i.e., copper smelter and re-suspended soil dust. Short duration episodes of S concentrations, up to 26 μg/m 3 , were found simultaneously with enhanced Cu, Fe and Zn. Contributions from individual pyrometallurgic processes and the cobalt slag dump could be distinguished from the elemental signatures

Changes in aerosol properties during spring-summer period in the Arctic troposphere

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A.-C. Engvall

2008-02-01

Full Text Available The change in aerosol properties during the transition from the more polluted spring to the clean summer in the Arctic troposphere was studied. A six-year data set of observations from Ny-Ålesund on Svalbard, covering the months April through June, serve as the basis for the characterisation of this time period. In addition four-day-back trajectories were used to describe air mass histories. The observed transition in aerosol properties from an accumulation-mode dominated distribution to an Aitken-mode dominated distribution is discussed with respect to long-range transport and influences from natural and anthropogenic sources of aerosols and pertinent trace gases. Our study shows that the air-mass transport is an important factor modulating the physical and chemical properties observed. However, the air-mass transport cannot alone explain the annually repeated systematic and rather rapid change in aerosol properties, occurring within a limited time window of approximately 10 days. With a simplified phenomenological model, which delivers the nucleation potential for new-particle formation, we suggest that the rapid shift in aerosol microphysical properties between the Arctic spring and summer is mainly driven by the incoming solar radiation in concert with transport of precursor gases and changes in condensational sink.

Characteristics and direct radiative effect of mid-latitude continental aerosols: the ARM case

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M. G. Iziomon

2003-01-01

Full Text Available A multi-year field measurement analysis of the characteristics and direct radiative effect of aerosols at the Southern Great Plains (SGP central facility of the Atmospheric Radiation Measurement (ARM Program is presented. Inter-annual mean and standard deviation of submicrometer scattering fraction (at 550 nm and Ångström exponent å (450 nm, 700 nm at the mid-latitude continental site are indicative of the scattering dominance of fine mode aerosol particles, being 0.84±0.03 and 2.25±0.09, respectively. We attribute the diurnal variation of submicron aerosol concentration to coagulation, photochemistry and the evolution of the boundary layer. Precipitation does not seem to play a role in the observed afternoon maximum in aerosol concentration. Submicron aerosol mass at the site peaks in the summer (12.1±6.7mg m-3, with the summer value being twice that in the winter. Of the chemically analyzed ionic components (which exclude carbonaceous aerosols, SO4= and NH4+ constitute the dominant species at the SGP seasonally, contributing 23-30% and 9-12% of the submicron aerosol mass, respectively. Although a minor species, there is a notable rise in NO3- mass fraction in winter. We contrast the optical properties of dust and smoke haze. The single scattering albedo w0 shows the most remarkable distinction between the two aerosol constituents. We also present aircraft measurements of vertical profiles of aerosol optical properties at the site. Annually, the lowest 1.2 km contributes 70% to the column total light scattering coefficient. Column-averaged and surface annual mean values of hemispheric backscatter fraction (at 550 nm, w0 (at 550 nm and å (450 nm, 700 nm agree to within 5% in 2001. Aerosols produce a net cooling (most pronounced in the spring at the ARM site

Cloud albedo changes in response to anthropogenic sulfate and non-sulfate aerosol forcings in CMIP5 models

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L. Frey

2017-07-01

Full Text Available The effects of different aerosol types on cloud albedo are analysed using the linear relation between total albedo and cloud fraction found on a monthly mean scale in regions of subtropical marine stratocumulus clouds and the influence of simulated aerosol variations on this relation. Model experiments from the Coupled Model Intercomparison Project phase 5 (CMIP5 are used to separately study the responses to increases in sulfate, non-sulfate and all anthropogenic aerosols. A cloud brightening on the month-to-month scale due to variability in the background aerosol is found to dominate even in the cases where anthropogenic aerosols are added. The aerosol composition is of importance for this cloud brightening, that is thereby region dependent. There is indication that absorbing aerosols to some extent counteract the cloud brightening but scene darkening with increasing aerosol burden is generally not supported, even in regions where absorbing aerosols dominate. Month-to-month cloud albedo variability also confirms the importance of liquid water content for cloud albedo. Regional, monthly mean cloud albedo is found to increase with the addition of anthropogenic aerosols and more so with sulfate than non-sulfate. Changes in cloud albedo between experiments are related to changes in cloud water content as well as droplet size distribution changes, so that models with large increases in liquid water path and/or cloud droplet number show large cloud albedo increases with increasing aerosol. However, no clear relation between model sensitivities to aerosol variations on the month-to-month scale and changes in cloud albedo due to changed aerosol burden is found.

Aerosol science: theory and practice

International Nuclear Information System (INIS)

Williams, M.M.R.; Loyalka, S.K.

1991-01-01

The purpose of this book is twofold. First, it is intended to give a thorough treatment of the fundamentals of aerosol behavior with rigorous proofs and detailed derivations of the basic equations and removal mechanisms. Second, it is intended to provide practical examples with special attention to radioactive particles and their distribution in size following a radioactive release arising from an accident with a nuclear system. We start with a brief introduction to the applications of aerosol science and the characteristics of aerosols in Chapter 1. In Chapter 2, we devote considerable attention to single and two particle motion with respect to both translation and rotation. Chapter 3 contains extensive discussion of the aerosol general dynamical equation and the dependences of aerosol distributions on size, shape, space, composition, radioactivity, and charge. Important particle rate processes of coagulation, condensation, and deposition/resuspension are discussed in the chapters 4, 6 and 7, respectively. In Chapter 5, we provide a thorough treatment of the analytical and numerical methods used in solving the various forms of the aerosol dynamical equation. We discuss the importance and applications of aerosol science to nuclear technology and, in particular, the nuclear source term in Chapter 8. Our focus in this chapter is on discussions of nuclear accidents that can potentially release large amount of radioactivity to environment. We also discuss the progress that has been made in understanding the natural and engineered aerosol processes that limit or affect such releases. (author)

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

Review of recent research on the climatic effect of aerosols

International Nuclear Information System (INIS)

Charlock, T.P.; Kondratyev, K.; Prokofyev, M.

1993-01-01

A review of relatively recent research on the climatic effects of aerosols is presented. Most of the inferences of the climatic effects of aerosols have been obtained through assuming a certain aerosol model in conjunction with a particular climate model. The following radiative effects of aerosols are identified: The planetary albedo is generally increased due to the backscatter of solar radiation by aerosols, with the exception of aerosols situated above a highly reflecting surface. Solar radiation absorption by some aerosols can offset the cooling due to aerosol backscatter. Although aerosol effects dominate for short-wave radiation, absorption and emission of terrestrial radiation by aerosols produces a warming effect. Various climate models are used to assess the impact of aerosols on climate. A two-stream approximation to the radiation transfer equation is adequate for optically thin layers where single scattering is applicable. Improved models to include aerosol terrestrial radiation effects, important feedback mechanisms, and the prediction of globally and seasonally averaged surface and atmospheric temperatures are provided by the so-called radiative-convective models (RCM's). The basic structure of the RCM's, which is regarded as adequate for many aerosol climate applications, is described. The general circulation model (GCM) is also described briefly. A full-scale GCM incorporating realistic aerosol inputs is yet to be formulated to include regional variability of the aerosol. Moreover, detailed computer modeling associated with GCM climate models can often confuse the basic physics. Because volcanic aerosols injected into the stratosphere have long residence times, they provide a good case study of the climate response to a change in the atmospheric aerosol. The chapter gives a critique of modeling work done to establish climatic effects of stratospheric aerosols

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

The fifth Finnish national aerosol symposium

International Nuclear Information System (INIS)

Mikkanen, P.; Haemeri, K.; Kauppinen, E.

1993-01-01

The Fifth Finnish Aerosol Symposium was held June 1-3, 1993. Symposium is jointly organized by FAAR, Aerosol Technology Group of Technical Research Centre of Finland and Helsinki University, Department of Physics. Aerosols, the suspensions of solid and liquid particles and gases, are receiving increasing importance in many areas of science and technology. These include industrial hygiene, ambient and indoor air pollution, pollution control technologies, cloud physics, nuclear safety engineering, combustion science and engineering, clean manufacturing technologies and material processing. The importance of aerosol issues during the development of advanced fuel conversion and material processing technologies can be realized when looking at the numerous papers presented on these topics at the Symposium

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.

Right Hemispheric Dominance in Processing of Unconscious Negative Emotion

Science.gov (United States)

Sato, Wataru; Aoki, Satoshi

2006-01-01

Right hemispheric dominance in unconscious emotional processing has been suggested, but remains controversial. This issue was investigated using the subliminal affective priming paradigm combined with unilateral visual presentation in 40 normal subjects. In either left or right visual fields, angry facial expressions, happy facial expressions, or…

Aerosol optical properties in the southeastern United States in summer – Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

Directory of Open Access Journals (Sweden)

C. A. Brock

2016-04-01

Full Text Available Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US. Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015. We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH. For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates

Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

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R. Wagner

2012-09-01

Full Text Available The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA, levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re

The intercomparison of aerosol codes

International Nuclear Information System (INIS)

Dunbar, I.H.; Fermandjian, J.; Gauvain, J.

1988-01-01

The behavior of aerosols in a reactor containment vessel following a severe accident could be an important determinant of the accident source term to the environment. Various processes result in the deposition of the aerosol onto surfaces within the containment, from where they are much less likely to be released. Some of these processes are very sensitive to particle size, so it is important to model the aerosol growth processes: agglomeration and condensation. A number of computer codes have been written to model growth and deposition processes. They have been tested against each other in a series of code comparison exercises. These exercises have investigated sensitivities to physical and numerical assumptions and have also proved a useful means of quality control for the codes. Various exercises in which code predictions are compared with experimental results are now under way

Aerosol transport over the Gangetic basin during ISRO-GBP land campaign-II

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M. Aloysius

2008-03-01

Full Text Available MODIS (Moderate Resolution Imaging Spectroradiometer Level-3 aerosol optical depth (AOD data and NCEP (National Centre for Environmental Prediction reanalysis winds were incorporated into an aerosol flux continuity equation, for a quantitative assessment of the sources of aerosol generation over the Ganga basin in the winter month of December 2004. Preliminary analysis on the aerosol distribution and wind fields showed wind convergence to be an important factor which, supported by the regional topography, confines aerosols in a long band over the Indo Gangetic plain (IGP stretching from the west of the Thar desert into the Head-Bay-of-Bengal. The prevailing winds of the season carry the aerosols from Head-Bay-of-Bengal along the east coast as far as the southern tip of the peninsular India. A detailed examination of MODIS data revealed significant day-to-day variations in aerosol loading in localised pockets over the central and eastern parts of the Indo Gangetic plain during the second half of December, with AOD values even exceeding unity. Aerosols over the Ganga basin were dominated by fine particles (geometric mean radius ~0.05–0.1μm while those over the central and western India were dominated by large particles (geometric mean radius ~0.3–0.7μ. Before introducing it into the flux equation, the MODIS derived AOD was validated through a comparison with the ground-based measurements collected at Kharagpur and Kanpur; two stations located over the Ganga basin. The strength of the aerosol generation computed using the flux equation indicated the existence of aerosol sources whose locations almost coincided with the concentration of thermal power plants. The quantitative agreement between the source strength and the power plant concentration, with a correlation coefficient 0.85, pointed to thermal power plants as substantial contributors to the high aerosol loading over the Ganga Basin in winter. The layout of aerosol sources also nearly

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

Science.gov (United States)

Logan, Timothy S.

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

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

Science.gov (United States)

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

2014-01-01

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

ARTIST: An International Project Investigating Aerosol Retention in a Ruptured Steam Generator

International Nuclear Information System (INIS)

Guentay, S.; Dehbi, A.; Suckow, D.; Birchley, J.

2002-01-01

Steam generator tube ruptures (SGTR) with a concurrent stuck open safety relief valve are counted among the risk dominant accident sequences because of the potential for radioactive products to bypass the containment. Owing to the absence of relevant empirical data and the complexity of the geometry and controlling processes, the aerosol removal in the steam generator (SG) tubes and in the secondary side is not well understood. Therefore, little or no credit is usually taken for aerosol retention due to natural processes in the various components of a SG. To help reduce the uncertainties associated with fission product release following an SGTR sequence, the Paul Scherrer Institut has initiated an international experimental project to be performed in the ARTIST (AeRosol Trapping In a Steam generaTor) facility in the time period from 2002 to 2007. The ARTIST test section is a scaled model of a real SG, and is comprised of a 264-tube bundle with a maximum height of 3.8 m, as well as one full-size droplet separator and one full-size steam dryer. The ARTIST facility is capable of producing soluble and insoluble aerosols and entrain them at sonic gas flow rates (up to 0.25 kg/s, thus matching comparable values predicted by the codes. In addition, aerosols can be generated at prototypical concentrations (up to 5 g/m 3 ) and sizes (0.2-5 mm AMMD). State of the art instrumentation is used (Low-pressure impactors, photometers, on-line particle sizer, online droplet sizer, etc.). The ARTIST project will simulate the flow and retention of aerosol-borne fission products in the SG, and provide a unique database to support safety assessments and analytical models. The project is foreseen in seven phases: 1) Aerosol retention in the tube under dry secondary side conditions, 2) Aerosol retention in the near field close to break under dry conditions, 3) Aerosol retention in the bundle far field under dry conditions, 4) Aerosol retention in the separator and dryer under dry

Influence of Atmospheric Processes on the Solubility and Composition of Iron in Saharan Dust.

Science.gov (United States)

Longo, Amelia F; Feng, Yan; Lai, Barry; Landing, William M; Shelley, Rachel U; Nenes, Athanasios; Mihalopoulos, Nikolaos; Violaki, Kalliopi; Ingall, Ellery D

2016-07-05

Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation state became more reduced, and aerosol acidity increased. Atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.

The Dominant Snow-forming Process in Warm and Cold Mixed-phase Orographic Clouds: Effects of Cloud Condensation Nuclei and Ice Nuclei

Science.gov (United States)

Fan, J.; Rosenfeld, D.; Leung, L. R.; DeMott, P. J.

2014-12-01

Mineral dust aerosols often observed over California in winter and spring from long-range transport can be efficient ice nuclei (IN) and enhance snow precipitation in mixed-phase orographic clouds. On the other hand, local pollution particles can serve as good CCN and suppress warm rain, but their impacts on cold rain processes are uncertain. The main snow-forming mechanism in warm and cold mixed-phase orographic clouds (refer to as WMOC and CMOC, respectively) could be very different, leading to different precipitation response to CCN and IN. We have conducted 1-km resolution model simulations using the Weather Research and Forecasting (WRF) model coupled with a spectral-bin cloud microphysical model for WMOC and CMOC cases from CalWater2011. We investigated the response of cloud microphysical processes and precipitation to CCN and IN with extremely low to extremely high concentrations using ice nucleation parameterizations that connect with dust and implemented based on observational evidences. We find that riming is the dominant process for producing snow in WMOC while deposition plays a more important role than riming in CMOC. Increasing IN leads to much more snow precipitation mainly due to an increase of deposition in CMOC and increased rimming in WMOC. Increasing CCN decreases precipitation in WMOC by efficiently suppressing warm rain, although snow is increased. In CMOC where cold rain dominates, increasing CCN significantly increases snow, leading to a net increase in precipitation. The sensitivity of supercooled liquid to CCN and IN has also been analyzed. The mechanism for the increased snow by CCN and caveats due to uncertainties in ice nucleation parameterizations will be discussed.

Aerosol Optical Depth Distribution in Extratropical Cyclones over the Northern Hemisphere Oceans

Science.gov (United States)

Naud, Catherine M.; Posselt, Derek J.; van den Heever, Susan C.

2016-01-01

Using Moderate Resolution Imaging Spectroradiometer and an extratropical cyclone database,the climatological distribution of aerosol optical depth (AOD) in extratropical cyclones is explored based solely on observations. Cyclone-centered composites of aerosol optical depth are constructed for the Northern Hemisphere mid-latitude ocean regions, and their seasonal variations are examined. These composites are found to be qualitatively stable when the impact of clouds and surface insolation or brightness is tested. The larger AODs occur in spring and summer and are preferentially found in the warm frontal and in the post-cold frontal regions in all seasons. The fine mode aerosols dominate the cold sector AODs, but the coarse mode aerosols display large AODs in the warm sector. These differences between the aerosol modes are related to the varying source regions of the aerosols and could potentially have different impacts on cloud and precipitation within the cyclones.

Aerosols and their Impact on Radiation, Clouds, Precipitation & Severe Weather Events

Energy Technology Data Exchange (ETDEWEB)

Li, Zhanqing; Rosenfeld, Daniel; Fan, Jiwen

2017-09-22

Aerosols, the tiny particles suspended in the atmosphere, have been in the forefront of environmental and climate change sciences as the primary atmospheric pollutant and external force affecting Earth’s weather and climate. There are two dominant mechanisms by which aerosols affect weather and climate: aerosol-radiation interactions (ARI) and aerosol-cloud interactions (ACI). ARI arises from aerosol scattering and absorption, which alters the radiation budgets of the atmosphere and surface, while ACI is rooted to the fact that aerosols serve as cloud condensation nuclei and ice nuclei. Both ARI and ACI are coupled with atmospheric dynamics to produce a chain of complex interactions with a large range of meteorological variables that influence both weather and climate. Elaborated here are the impacts of aerosols on the radiation budget, clouds (microphysics, structure, and lifetime), precipitation, and severe weather events (lightning, thunderstorms, hail, and tornados). Depending on environmental variables and aerosol properties, the effects can be both positive and negative, posing the largest uncertainties in the external forcing of the climate system. This has considerably hindered our ability in projecting future climate changes and in doing accurate numerical weather predictions.

Nuclear microprobe analysis and source apportionment of individual atmospheric aerosol particles

International Nuclear Information System (INIS)

Artaxo, P.; Rabello, M.L.C.; Watt, F.; Grime, G.; Swietlicki, E.

1993-01-01

In atmospheric aerosol reserach, one key issue is to determine the sources of the airborne particles. Bulk PIXE analysis coupled with receptor modeling provides a useful, but limited view of the aerosol sources influencing one particular site or sample. The scanning nuclear microprobe (SNM) technique is a microanalytical technique that gives unique information on individual aerosol particles. In the SNM analyses a 1.0 μm size 2.4 MeV proton beam from the Oxford SNM was used. The trace elements with Z>11 were measured by the particle induced X-ray emission (PIXE) method with detection limits in the 1-10 ppm range. Carbon, nitrogen and oxygen are measured simultaneously using Rutherford backscattering spectrometry (RBS). Atmospheric aerosol particles were collected at the Brazilian Antarctic Station and at biomass burning sites in the Amazon basin tropical rain forest in Brazil. In the Antarctic samples, the sea-salt aerosol particles were clearly predominating, with NaCl and CaSO 4 as major compounds with several trace elements as Al, Si, P, K, Mn, Fe, Ni, Cu, Zn, Br, Sr, and Pb. Factor analysis of the elemental data showed the presence of four components: 1) Soil dust particles; 2) NaCl particles; 3) CaSO 4 with Sr; and 4) Br and Mg. Strontium, observed at 20-100 ppm levels, was always present in the CaSO 4 particles. The hierarchical cluster procedure gave results similar to the ones obtained through factor analysis. For the tropical rain forest biomass burning aerosol emissions, biogenic particles with a high organic content dominate the particle population, while K, P, Ca, Mg, Zn, and Si are the dominant elements. Zinc at 10-200 ppm is present in biogenic particles rich in P and K. The quantitative aspects and excellent detection limits make SNM analysis of individual aerosol particles a very powerful analytical tool. (orig.)

Mechanisms of Formation of Secondary Organic Aerosols and Implications for Global Radiative Forcing

Energy Technology Data Exchange (ETDEWEB)

Seinfeld, John H. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

2011-12-02

Organic material constitutes about 50% of global atmospheric aerosol mass, and the dominant source of organic aerosol is the oxidation of volatile hydrocarbons, to produce secondary organic aerosol (SOA). Understanding the formation of SOA is crucial to predicting present and future climate effects of atmospheric aerosols. The goal of this program is to significantly increase our understanding of secondary organic aerosol (SOA) formation in the atmosphere. Ambient measurements indicate that the amount of SOA in the atmosphere exceeds that predicted in current models based on existing laboratory chamber data. This would suggest that either the SOA yields measured in laboratory chambers are understated or that all major organic precursors have not been identified. In this research program we are systematically exploring these possibilities.

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

Energy Technology Data Exchange (ETDEWEB)

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

2017-06-01

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

Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

Science.gov (United States)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-04-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

CATS Aerosol Typing and Future Directions

Science.gov (United States)

McGill, Matt; Yorks, John; Scott, Stan; Palm, Stephen; Hlavka, Dennis; Hart, William; Nowottnick, Ed; Selmer, Patrick; Kupchock, Andrew; Midzak, Natalie;

Predicting the Mineral Composition of Dust Aerosols. Part 2; Model Evaluation and Identification of Key Processes with Observations

Science.gov (United States)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

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

Science.gov (United States)

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

2009-04-01

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

COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel A. [Univ. of Washington, Seattle, WA (United States); Worsnop, Douglas [Aerodyne Research, Billerica, MA (United States)

2016-09-22

This project was part of a collaborative campaign, including the participation of scientists from seven research groups as part of the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London to study wintertime sources of urban particulate matter. The UW contribution by PI Thornton’s group was to make the first deployment of a chemical ionization mass spectrometer instrument (MOVI-CI-ToFMS) to measure both particle and gas phase organic acids. The new instrument ran nearly continuously during the ClearfLo WINTER IOP at the Detling site, producing a first-ever data set of molecular composition information that can be used for source apportionment and process studies. The UW group published a paper in Environmental Science and Technology and contributed to another (Bohnenstengel et al BAMS 2015) detailing a direct molecular connection between biomass/biofuel burning particles and aerosol light absorption. The ES&T paper (Mohr, et al ES&T 2013) has received 42 citations in just 3 years indicative of its significant impact on the field. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal.

Fractionation of Stable Isotopes in Atmospheric Aerosol Reactions

DEFF Research Database (Denmark)

Meusinger, Carl

-independent) fractionation processes of stable isotopes of C, N, O and S in order to investigate three different systems related to aerosols: 1. Post-depositional processes of nitrate in snow that obscure nitrate ice core records 2. Formation and aging of secondary organic aerosol generated by ozonolysis of X...... reactions and undergo complex chemical and physical changes during their lifetimes. In order to assess processes that form and alter aerosols, information provided by stable isotopes can be used to help constrain estimates on the strength of aerosol sources and sinks. This thesis studies (mass...... as required. The kndings provide important results for the studies' respective felds, including a description of the isotopic fractionation and quantum yield of nitrate photolysis in snow, equilibrium fractionation in secondary organic aerosol and fractionation constants of different oxidation pathways of SO2....

UCLALES-SALSA v1.0: a large-eddy model with interactive sectional microphysics for aerosol, clouds and precipitation

Science.gov (United States)

Tonttila, Juha; Maalick, Zubair; Raatikainen, Tomi; Kokkola, Harri; Kühn, Thomas; Romakkaniemi, Sami

2017-01-01

Challenges in understanding the aerosol-cloud interactions and their impacts on global climate highlight the need for improved knowledge of the underlying physical processes and feedbacks as well as their interactions with cloud and boundary layer dynamics. To pursue this goal, increasingly sophisticated cloud-scale models are needed to complement the limited supply of observations of the interactions between aerosols and clouds. For this purpose, a new large-eddy simulation (LES) model, coupled with an interactive sectional description for aerosols and clouds, is introduced. The new model builds and extends upon the well-characterized UCLA Large-Eddy Simulation Code (UCLALES) and the Sectional Aerosol module for Large-Scale Applications (SALSA), hereafter denoted as UCLALES-SALSA. Novel strategies for the aerosol, cloud and precipitation bin discretisation are presented. These enable tracking the effects of cloud processing and wet scavenging on the aerosol size distribution as accurately as possible, while keeping the computational cost of the model as low as possible. The model is tested with two different simulation set-ups: a marine stratocumulus case in the DYCOMS-II campaign and another case focusing on the formation and evolution of a nocturnal radiation fog. It is shown that, in both cases, the size-resolved interactions between aerosols and clouds have a critical influence on the dynamics of the boundary layer. The results demonstrate the importance of accurately representing the wet scavenging of aerosol in the model. Specifically, in a case with marine stratocumulus, precipitation and the subsequent removal of cloud activating particles lead to thinning of the cloud deck and the formation of a decoupled boundary layer structure. In radiation fog, the growth and sedimentation of droplets strongly affect their radiative properties, which in turn drive new droplet formation. The size-resolved diagnostics provided by the model enable investigations of these

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

Directory of Open Access Journals (Sweden)

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

Hygroscopic Properties and Chemical Composition of Aerosol Particles at the High Alpine Site Jungfraujoch

Energy Technology Data Exchange (ETDEWEB)

Weingarter, E.; Gysel, M.; Sjoegren, S.; Baltesperger, U.; Alfarra, R.; Bower, K.; Coe, H.

2004-03-01

The hygroscopic properties of aerosols play a significant role in atmospheric phenomena such as acid deposition, visibility degradation and climate change. Due to the hygroscopic growth of the particles, water is often the dominant component of the ambient aerosol at high relative humidity (RH) conditions. The ability to absorb water depends on the particle chemical composition, dry size, and shape. The aim of this study is to link the chemical composition of the atmospheric aerosol to its hygroscopic properties. (author)

Narrowing the Gap in Quantification of Aerosol-Cloud Radiative Effects

Science.gov (United States)

Feingold, G.; McComiskey, A. C.; Yamaguchi, T.; Kazil, J.; Johnson, J. S.; Carslaw, K. S.

2016-12-01

Despite large advances in our understanding of aerosol and cloud processes over the past years, uncertainty in the aerosol-cloud radiative effect/forcing is still of major concern. In this talk we will advocate a methodology for quantifying the aerosol-cloud radiative effect that considers the primacy of fundamental cloud properties such as cloud amount and albedo alongside the need for process level understanding of aerosol-cloud interactions. We will present a framework for quantifying the aerosol-cloud radiative effect, regime-by-regime, through process-based modelling and observations at the large eddy scale. We will argue that understanding the co-variability between meteorological and aerosol drivers of the radiative properties of the cloud system may be as important an endeavour as attempting to untangle these drivers.

Aerosol typing - key information from aerosol studies

Science.gov (United States)

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

2016-04-01

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

Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data

Directory of Open Access Journals (Sweden)

A. P. Grieshop

2009-03-01

Full Text Available Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit-mass-resolution quadrupole Aerosol Mass Spectrometer (AMS. The results highlight how photochemical processing can lead to considerable evolution of the mass, volatility and level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the OA mass after a few hours of aging under typical summertime conditions. Aging also decreased the volatility of the OA and made it progressively more oxygenated. The results also illustrate strengths of, and challenges with, using AMS data for source apportionment analysis. For example, the mass spectra of fresh and aged BBOA are distinct from fresh motor-vehicle emissions. The mass spectra of the secondary OA produced from aging wood smoke are very similar to those of the oxygenated OA (OOA that dominates ambient AMS datasets, further reinforcing the connection between OOA and OA formed from photo-chemistry. In addition, aged wood smoke spectra are similar to those from OA created by photo-oxidizing dilute diesel exhaust. This demonstrates that the OOA observed in the atmosphere can be produced by photochemical aging of dilute emissions from different types of combustion systems operating on fuels with modern or fossil carbon. Since OOA is frequently the dominant component of ambient OA, the similarity of spectra of aged emissions from different sources represents an important challenge for AMS-based source apportionment studies.

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

Modal Bin Hybrid Model: A surface area consistent, triple-moment sectional method for use in process-oriented modeling of atmospheric aerosols

Science.gov (United States)

Kajino, Mizuo; Easter, Richard C.; Ghan, Steven J.

2013-09-01

triple-moment sectional (TMS) aerosol dynamics model, Modal Bin Hybrid Model (MBHM), has been developed. In addition to number and mass (volume), surface area is predicted (and preserved), which is important for aerosol processes and properties such as gas-to-particle mass transfer, heterogeneous reaction, and light extinction cross section. The performance of MBHM was evaluated against double-moment sectional (DMS) models with coarse (BIN4) to very fine (BIN256) size resolutions for simulating evolution of particles under simultaneously occurring nucleation, condensation, and coagulation processes (BINx resolution uses x sections to cover the 1 nm to 1 µm size range). Because MBHM gives a physically consistent form of the intrasectional distributions, errors and biases of MBHM at BIN4-8 resolution were almost equivalent to those of DMS at BIN16-32 resolution for various important variables such as the moments Mk (k: 0, 2, 3), dMk/dt, and the number and volume of particles larger than a certain diameter. Another important feature of MBHM is that only a single bin is adequate to simulate full aerosol dynamics for particles whose size distribution can be approximated by a single lognormal mode. This flexibility is useful for process-oriented (multicategory and/or mixing state) modeling: Primary aerosols whose size parameters would not differ substantially in time and space can be expressed by a single or a small number of modes, whereas secondary aerosols whose size changes drastically from 1 to several hundred nanometers can be expressed by a number of modes. Added dimensions can be applied to MBHM to represent mixing state or photochemical age for aerosol mixing state studies.

Impacts of Aerosol Direct Effects on the South Asian climate: Assessment of Radiative Feedback Processes Using Model Simulations and Satellite/surface Measurements

Science.gov (United States)

Wang, S.; Gautam, R.; Lau, W. K.; Tsay, S.; Sun, W.; Kim, K.; Chern, J.; Colarco, P. R.; Hsu, N. C.; Lin, N.

2011-12-01

Current assessment of aerosol radiative effect is hindered by our incomplete knowledge of aerosol optical properties, especially absorption, and our current inability to quantify physical and microphysical processes. In this research, we investigate direct aerosol radiative effect over heavy aerosol loading areas (e.g., Indo-Gangetic Plains, South/East Asia) and its feedbacks on the South Asian climate during the pre-monsoon season (March-June) using the Purdue Regional Climate Model (PRCM) with prescribed aerosol data derived by the NASA Goddard Earth Observing System Model (GEOS-5). Our modeling domain covers South and East Asia (60-140E and 0-50N) with spatial resolutions of 45 km in horizontal and 28 layers in vertical. The model is integrated from 15 February to 30 June 2008 continuously without nudging (i.e., only forced by initial/boundary conditions). Two numerical experiments are conducted with and without the aerosol-radiation effects. Both simulations are successful in reproducing the synoptic patterns on seasonal-to-interannual time scales and capturing a pre-monsoon feature of the northward rainfall propagation over Indian region in early June which shown in Tropical Rainfall Measuring Mission (TRMM) observation. Preliminary result suggests aerosol-radiation interactions mainly alter surface-atmosphere energetics and further result in an adjustment of the vertical temperature distribution in lower atmosphere (below 700 hPa). The modifications of temperature and associated rainfall and circulation feedbacks on the regional climate will be discussed in the presentation. In addition to modeling study, we will also present the most recent results on aerosol properties, regional aerosol absorption, and radiative forcing estimation based on NASA's operational satellite and ground-based remote sensing. Observational results show spatial gradients in aerosol loading and solar absorption accounting over Indo-Gangetic Plains during the pre-monsoon season. The

High formation of secondary organic aerosol from the photo-oxidation of toluene

OpenAIRE

L. Hildebrandt; N. M. Donahue; S. N. Pandis

2009-01-01

Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA) precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental co...

Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2009-03-05

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Compact Layers of Hybrid Halide Perovskites Fabricated via the Aerosol Deposition Process-Uncoupling Material Synthesis and Layer Formation.

Science.gov (United States)

Panzer, Fabian; Hanft, Dominik; Gujar, Tanaji P; Kahle, Frank-Julian; Thelakkat, Mukundan; Köhler, Anna; Moos, Ralf

2016-04-08

We present the successful fabrication of CH₃NH₃PbI₃ perovskite layers by the aerosol deposition method (ADM). The layers show high structural purity and compactness, thus making them suitable for application in perovskite-based optoelectronic devices. By using the aerosol deposition method we are able to decouple material synthesis from layer processing. Our results therefore allow for enhanced and easy control over the fabrication of perovskite-based devices, further paving the way for their commercialization.

Aerosol chemical and optical properties over the Paris area within ESQUIF project

Directory of Open Access Journals (Sweden)

A. Hodzic

2006-01-01

Full Text Available Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%, and inorganic aerosol fraction (40% including nitrate (8%, sulfate (22% and ammonium (10%. The secondary organic aerosols (SOA represent 12% of the total aerosol mass, while the

Characterization of selenium in ambient aerosols and primary emission sources.

Science.gov (United States)

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

2014-08-19

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

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

International Nuclear Information System (INIS)

Grotti, Marco; Lagomarsino, Cristina; Frache, Roberto

2004-01-01

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

Aerosol influence on energy balance of the middle atmosphere of Jupiter.

Science.gov (United States)

Zhang, Xi; West, Robert A; Irwin, Patrick G J; Nixon, Conor A; Yung, Yuk L

2015-12-22

Aerosols are ubiquitous in planetary atmospheres in the Solar System. However, radiative forcing on Jupiter has traditionally been attributed to solar heating and infrared cooling of gaseous constituents only, while the significance of aerosol radiative effects has been a long-standing controversy. Here we show, based on observations from the NASA spacecraft Voyager and Cassini, that gases alone cannot maintain the global energy balance in the middle atmosphere of Jupiter. Instead, a thick aerosol layer consisting of fluffy, fractal aggregate particles produced by photochemistry and auroral chemistry dominates the stratospheric radiative heating at middle and high latitudes, exceeding the local gas heating rate by a factor of 5-10. On a global average, aerosol heating is comparable to the gas contribution and aerosol cooling is more important than previously thought. We argue that fractal aggregate particles may also have a significant role in controlling the atmospheric radiative energy balance on other planets, as on Jupiter.

Individual aerosol particles in and below clouds along a Mt. Fuji slope: Modification of sea-salt-containing particles by in-cloud processing

Science.gov (United States)

Ueda, S.; Hirose, Y.; Miura, K.; Okochi, H.

2014-02-01

Sizes and compositions of atmospheric aerosol particles can be altered by in-cloud processing by absorption/adsorption of gaseous and particulate materials and drying of aerosol particles that were formerly activated as cloud condensation nuclei. To elucidate differences of aerosol particles before and after in-cloud processing, aerosols were observed along a slope of Mt. Fuji, Japan (3776 m a.s.l.) during the summer in 2011 and 2012 using a portable laser particle counter (LPC) and an aerosol sampler. Aerosol samples for analyses of elemental compositions were obtained using a cascade impactor at top-of-cloud, in-cloud, and below-cloud altitudes. To investigate composition changes via in-cloud processing, individual particles (0.5-2 μm diameter) of samples from five cases (days) collected at different altitudes under similar backward air mass trajectory conditions were analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. For most cases (four cases), most particles at all altitudes mainly comprised sea salts: mainly Na with some S and/or Cl. Of those, in two cases, sea-salt-containing particles with Cl were found in below-cloud samples, although sea-salt-containing particles in top-of-cloud samples did not contain Cl. This result suggests that Cl in the sea salt was displaced by other cloud components. In the other two cases, sea-salt-containing particles on samples at all altitudes were without Cl. However, molar ratios of S to Na (S/Na) of the sea-salt-containing particles of top-of-cloud samples were higher than those of below-cloud samples, suggesting that sulfuric acid or sulfate was added to sea-salt-containing particles after complete displacement of Cl by absorption of SO2 or coagulation with sulfate. The additional volume of sulfuric acid in clouds for the two cases was estimated using the observed S/Na values of sea-salt-containing particles. The estimation revealed that size changes by in

Importance of relative humidity in the oxidative ageing of organic aerosols: case study of the ozonolysis of maleic acid aerosol

Directory of Open Access Journals (Sweden)

P. J. Gallimore

2011-12-01

Full Text Available Many important atmospheric aerosol processes depend on the chemical composition of the aerosol, e.g. water uptake and particle cloud interactions. Atmospheric ageing processes, such as oxidation reactions, significantly and continuously change the chemical composition of aerosol particles throughout their lifetime. These ageing processes are often poorly understood. In this study we utilize an aerosol flow tube set up and an ultra-high resolution mass spectrometer to explore the effect of relative humidity (RH in the range of <5–90% on the ozonolysis of maleic acid aerosol which is employed as model organic aerosol system. Due to the slow reaction kinetics relatively high ozone concentrations of 160–200 ppm were used to achieve an appreciable degree of oxidation of maleic acid. The effect of oxidative ageing on the hygroscopicity of maleic acid particles is also investigated using an electrodynamic balance and thermodynamic modelling. RH has a profound effect on the oxidation of maleic acid particles. Very little oxidation is observed at RH < 50% and the only observed reaction products are glyoxylic acid and formic acid. In comparison, when RH > 50% there are about 15 oxidation products identified. This increased oxidation was observed even when the particles were exposed to high humidities long after a low RH ozonolysis reaction. This result might have negative implications for the use of water as an extraction solvent for the analysis of oxidized organic aerosols. These humidity-dependent differences in the composition of the ozonolyzed aerosol demonstrate that water is both a key reactant in the oxidation scheme and a determinant of particle phase and hence diffusivity. The measured chemical composition of the processed aerosol is used to model the hygroscopic growth, which compares favourably with water uptake results from the electrodynamic balance measurements. A reaction mechanism is presented which takes into account the RH dependent

Aerosol chemical composition at Cabauw, The Netherlands as observed in two intensive periods in May 2008 and March 2009

Science.gov (United States)

Mensah, A. A.; Holzinger, R.; Otjes, R.; Trimborn, A.; Mentel, Th. F.; ten Brink, H.; Henzing, B.; Kiendler-Scharr, A.

2012-05-01

Observations of aerosol chemical composition in Cabauw, the Netherlands, are presented for two intensive measurement periods in May 2008 and March 2009. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and is compared to observations from aerosol size distribution measurements as well as composition measurements with a Monitor for AeRosol and GAses (MARGA) based instrument and a Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS). An overview of the data is presented and the data quality is discussed. In May 2008 enhanced pollution was observed with organics contributing 40% to the PM1 mass. In contrast the observed average mass loading was lower in March 2009 and a dominance of ammonium nitrate (42%) was observed. The semi-volatile nature of ammonium nitrate is evident in the diurnal cycles with maximum concentrations observed in the morning hours in May 2008 and little diurnal variation observed in March 2009. Size dependent composition data from AMS measurements are presented and show a dominance of organics in the size range below 200 nm. A higher O:C ratio of the organics is observed for May 2008 than for March 2009. Together with the time series of individual tracer ions this shows the dominance of OOA over HOA in May 2008.

Pulmonary aerosol delivery and the importance of growth dynamics.

Science.gov (United States)

Haddrell, Allen E; Lewis, David; Church, Tanya; Vehring, Reinhard; Murnane, Darragh; Reid, Jonathan P

2017-12-01

Aerosols are dynamic systems, responding to variations in the surrounding environmental conditions by changing in size, composition and phase. Although, widely used in inhalation therapies, details of the processes occurring on aerosol generation and during inhalation have received little attention. Instead, research has focused on improvements to the formulation of the drug prior to aerosolization and the resulting clinical efficacy of the treatment. Here, we highlight the processes that occur during aerosol generation and inhalation, affecting aerosol disposition when deposited and, potentially, impacting total and regional doses. In particular, we examine the response of aerosol particles to the humid environment of the respiratory tract, considering both the capacity of particles to grow by absorbing moisture and the timescale for condensation to occur. [Formula: see text].

Radiative Importance of Aerosol-Cloud Interaction

Science.gov (United States)

Tsay, Si-Chee

1999-01-01

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have

Unveiling aerosol-cloud interactions - Part 2: Minimising the effects of aerosol swelling and wet scavenging in ECHAM6-HAM2 for comparison to satellite data

Science.gov (United States)

Neubauer, David; Christensen, Matthew W.; Poulsen, Caroline A.; Lohmann, Ulrike

2017-11-01

Aerosol-cloud interactions (ACIs) are uncertain and the estimates of the ACI effective radiative forcing (ERFaci) magnitude show a large variability. Within the Aerosol_cci project the susceptibility of cloud properties to changes in aerosol properties is derived from the high-resolution AATSR (Advanced Along-Track Scanning Radiometer) data set using the Cloud-Aerosol Pairing Algorithm (CAPA) (as described in our companion paper) and compared to susceptibilities from the global aerosol climate model ECHAM6-HAM2 and MODIS-CERES (Moderate Resolution Imaging Spectroradiometer - Clouds and the Earth's Radiant Energy System) data. For ECHAM6-HAM2 the dry aerosol is analysed to mimic the effect of CAPA. Furthermore the analysis is done for different environmental regimes. The aerosol-liquid water path relationship in ECHAM6-HAM2 is systematically stronger than in AATSR-CAPA data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM2 the strength of the susceptibilities of liquid water path, cloud droplet number concentration and cloud albedo as well as ERFaci agree much better with those of AATSR-CAPA or MODIS-CERES. When comparing satellite-derived to model-derived susceptibilities, this study finds it more appropriate to use dry aerosol in the computation of model susceptibilities. We further find that the statistical relationships inferred from different satellite sensors (AATSR-CAPA vs. MODIS-CERES) as well as from ECHAM6-HAM2 are not always of the same sign for the tested environmental conditions. In particular the susceptibility of the liquid water path is negative in non-raining scenes for MODIS-CERES but positive for AATSR-CAPA and ECHAM6-HAM2. Feedback processes like cloud-top entrainment that are missing or not well represented in the model are therefore not well

Papers of the 15. french congress on the aerosols CFA 99; Actes du 15. congres francais sur les aerosols CFA 99

Energy Technology Data Exchange (ETDEWEB)

NONE

2000-07-01

This french congress on the aerosols took place in Paris the 8 and 9 december 1999. It was presented in four main themes: bio-aerosols and filtering; the aerosols metrology; the aerosols in the environment; aerosols physic and applications. Seven papers have been analyzed in INIS data base for their specific interest in the nuclear industry. They concern the aerosol capture simulation, the aerosols sampling in workplace environment, a ring-effect ion generator development for the charge and the neutralization of an aerosol cloud, the radon 222 characterization in a house, a particle re-entrainment, the electrical charge process of beta emitter radioactive aerosols, the simulation of air flows in many filters. The other ones are analyzed in the ETDE data base. (A.L.B.)

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

Science.gov (United States)

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

2017-04-01

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

Diagnosing causes of extreme aerosol optical depth events

Science.gov (United States)

Bernstein, D. N.; Sullivan, R.; Crippa, P.; Thota, A.; Pryor, S. C.

2017-12-01

Aerosol burdens and optical properties exhibit substantial spatiotemporal variability, and simulation of current and possible future aerosol burdens and characteristics exhibits relatively high uncertainty due to uncertainties in emission estimates and in chemical and physical processes associated with aerosol formation, dynamics and removal. We report research designed to improve understanding of the causes and characteristics of extreme aerosol optical depth (AOD) at the regional scale, and diagnose and attribute model skill in simulating these events. Extreme AOD events over the US Midwest are selected by identifying all dates on which AOD in a MERRA-2 reanalysis grid cell exceeds the local seasonally computed 90th percentile (p90) value during 2004-2016 and then finding the dates on which the highest number of grid cells exceed their local p90. MODIS AOD data are subsequently used to exclude events dominated by wildfires. MERRA-2 data are also analyzed within a synoptic classification to determine in what ways the extreme AOD events are atypical and to identify possible meteorological `finger-prints' that can be detected in regional climate model simulations of future climate states to project possible changes in the occurrence of extreme AOD. Then WRF-Chem v3.6 is applied at 12-km resolution and regridded to the MERRA-2 resolution over eastern North America to quantify model performance, and also evaluated using in situ measurements of columnar AOD (AERONET) and near-surface PM2.5 (US EPA). Finally the sensitivity to (i) spin-up time (including procedure used to spin-up the chemistry), (ii) modal versus sectional aerosol schemes, (iii) meteorological nudging, (iv) chemistry initial and boundary conditions, and (v) anthropogenic emissions is quantified. Despite recent declines in mean AOD, supraregional (> 1000 km) extreme AOD events continue to occur. During these events AOD exceeds 0.6 in many Midwestern grid cells for multiple consecutive days. In all

Chemical Characterization of Submicron Aerosol Particles in São Paulo, Brazil

Science.gov (United States)

Ferreira De Brito, J.; Rizzo, L. V.; Godoy, J.; Godoy, M. L.; de Assunção, J. V.; Alves, N. D.; Artaxo, P.

2013-12-01

pattern allows characterization of organic aerosol processing, e.g., m/z 43 (C2H3O+ and/or C3H7+, depending on the source and level or processing) and m/z 44 (mostly CO2+). The parameter f43 and f44, defined as the signal on the corresponding m/z relative to total organic, provides a metric for aerosol processing. As such, the organic aerosol sampled at the University site has shown to be considerably more processed than at the Downtown site, with the parameter f44=0.19 in the former and 0.14 in the latter. Interestingly, little difference has been observed in the f43 parameter, being 0.035 at the University site and 0.036 at the Downtown site. PMF analysis indicates large dominance of SOA relative to POA on both sites. This study shall provide an overview of the atmospheric dynamics of this megacity and its unique fleet, never characterized in such details before.

Simulation of Cloud-aerosol Lidar with Orthogonal Polarization (CALIOP Attenuated Backscatter Profiles Using the Global Model of Aerosol Processes (GLOMAP

Directory of Open Access Journals (Sweden)

Young Stuart

2016-01-01

Full Text Available To permit the calculation of the radiative effects of atmospheric aerosols, we have linked our aerosol-chemical transport model (CTMGLOMAP to a new radiation module (UKCARADAER. In order to help assess and improve the accuracy of the radiation code, in particular the height dependence of the predicted scattering, we have developed a module that simulates attenuated backscatter (ABS profiles that would be measured by the satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP if it were to sample an atmosphere with the same aerosol loading as predicted by the CTM. Initial results of our comparisons of the predicted ABS profiles with actual CALIOP data are encouraging but some differences are noted, particularly in marine boundary layers where the scattering is currently under-predicted and in dust layers where it is often over-predicted. The sources of these differences are being investigated.

Sea Spray Aerosol Production over the North Atlantic

Science.gov (United States)

Bates, T. S.; Quinn, P.

2017-12-01

Breaking waves on the ocean surface generate air bubbles that scavenge organic matter from the surrounding seawater. When injected into the atmosphere, these bubbles burst, yielding sea spray aerosol (SSA), a mixture of organic and inorganic compounds with the organic matter enriched relative to seawater. SSA mass is well documented as the dominant component of aerosol light scattering over the remote oceans. The importance of SSA number to marine boundary layer cloud condensation nuclei (CCN) is much less certain. During the Western Atlantic Climate Study cruises (WACS-1 - August 2012 and WACS-2 - May-June 2014) and the North Atlantic Aerosols and Marine Ecosystem Study cruises (NAAMES-1 - November 2015, NAAMES-2 - May 2016, and NAAMES-3 - September 2017), we generated and measured freshly emitted SSA using the Sea Sweep SSA generator. During the 2017 cruise we also generated SSA with a Marine Aerosol Reference Tank (MART). Using the data generated on these 5 cruises and a large database of remote marine boundary layer aerosol measurements we will address three questions during this presentation: 1 - Do phytoplankton ecosystems affect the organic enrichment of freshly emitted SSA?, 2 - Do plankton ecosystems affect the number production flux of SSA?, and 3 - Is SSA a significant source of atmospheric CCN?

Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

Directory of Open Access Journals (Sweden)

D. K. Farmer

2011-06-01

Full Text Available Although laboratory studies show that biogenic volatile organic compounds (VOCs yield substantial secondary organic aerosol (SOA, production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR PM₁ fluxes. Average deposition velocities for total NR-PM₁ aerosol at noon were 2.05 ± 0.04 mm s⁻¹. Using a high resolution measurement of the NH₂⁺ and NH₃⁺ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s⁻¹ and are dominated by deposition of ammonium sulphate.

Optical, microphysical and radiative properties of aerosols over a tropical rural site in Kenya, East Africa: Source identification, modification and aerosol type discrimination

Science.gov (United States)

Boiyo, Richard; Kumar, K. Raghavendra; Zhao, Tianliang

2018-03-01

A better understanding of aerosol optical, microphysical and radiative properties is a crucial challenge for climate change studies. In the present study, column-integrated aerosol optical and radiative properties observed at a rural site, Mbita (0.42°S, 34.20 °E, and 1125 m above sea level) located in Kenya, East Africa (EA) are investigated using ground-based Aerosol Robotic Network (AERONET) data retrieved during January, 2007 to December, 2015. The annual mean aerosol optical depth (AOD500 nm), Ångström exponent (AE440-870 nm), fine mode fraction of AOD500 nm (FMF500 nm), and columnar water vapor (CWV, cm) were found to be 0.23 ± 0.08, 1.01 ± 0.16, 0.60 ± 0.07, and 2.72 ± 0.20, respectively. The aerosol optical properties exhibited a unimodal distribution with substantial seasonal heterogeneity in their peak values being low (high) during the local wet (dry) seasons. The observed data showed that Mbita and its environs are significantly influenced by various types of aerosols, with biomass burning and/or urban-industrial (BUI), mixed (MXD), and desert dust (DDT) aerosol types contributing to 37.72%, 32.81%, and 1.40%, respectively during the local dry season (JJA). The aerosol volume size distribution (VSD) exhibited bimodal lognormal structure with a geometric mean radius of 0.15 μm and 3.86-5.06 μm for fine- and coarse-mode aerosols, respectively. Further, analysis of single scattering albedo (SSA), asymmetry parameter (ASY) and refractive index (RI) revealed dominance of fine-mode absorbing aerosols during JJA. The averaged aerosol direct radiative forcing (ARF) retrieved from the AERONET showed a strong cooling effect at the bottom of the atmosphere (BOA) and significant warming within the atmosphere (ATM), representing the important role of aerosols played in this rural site of Kenya. Finally, the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model revealed that aerosols from distinct sources resulted in enhanced loading

Aerosol counterflow two-jets unit for continuous measurement of the soluble fraction of atmospheric aerosols.

Science.gov (United States)

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

A new type of aerosol collector employing a liquid at laboratory temperature for continuous sampling of atmospheric particles is described. The collector operates on the principle of a Venturi scrubber. Sampled air flows at high linear velocity through two Venturi nozzles "atomizing" the liquid to form two jets of a polydisperse aerosol of fine droplets situated against each other. Counterflow jets of droplets collide, and within this process, the aerosol particles are captured into dispersed liquid. Under optimum conditions (air flow rate of 5 L/min and water flow rate of 2 mL/min), aerosol particles down to 0.3 microm in diameter are quantitatively collected in the collector into deionized water while the collection efficiency of smaller particles decreases. There is very little loss of fine aerosol within the aerosol counterflow two-jets unit (ACTJU). Coupling of the aerosol collector with an annular diffusion denuder located upstream of the collector ensures an artifact-free sampling of atmospheric aerosols. Operation of the ACTJU in combination with on-line detection devices allows in situ automated analysis of water-soluble aerosol species (e.g., NO2-, NO3-)with high time resolution (as high as 1 s). Under the optimum conditions, the limit of detection for particulate nitrite and nitrate is 28 and 77 ng/m(3), respectively. The instrument is sufficiently rugged for its application at routine monitoring of aerosol composition in the real time.

Polar organic marker compounds in atmospheric aerosols during the LBA-SMOCC 2002 biomass burning experiment in Rondônia, Brazil: sources and source processes, time series, diel variations and size distributions

Directory of Open Access Journals (Sweden)

M. Claeys

2010-10-01

Full Text Available Measurements of polar organic marker compounds were performed on aerosols that were collected at a pasture site in the Amazon basin (Rondônia, Brazil using a high-volume dichotomous sampler (HVDS and a Micro-Orifice Uniform Deposit Impactor (MOUDI within the framework of the 2002 LBA-SMOCC (Large-Scale Biosphere Atmosphere Experiment in Amazônia – Smoke Aerosols, Clouds, Rainfall, and Climate: Aerosols From Biomass Burning Perturb Global and Regional Climate campaign. The campaign spanned the late dry season (biomass burning, a transition period, and the onset of the wet season (clean conditions. In the present study a more detailed discussion is presented compared to previous reports on the behavior of selected polar marker compounds, including levoglucosan, malic acid, isoprene secondary organic aerosol (SOA tracers and tracers for fungal spores. The tracer data are discussed taking into account new insights that recently became available into their stability and/or aerosol formation processes. During all three periods, levoglucosan was the most dominant identified organic species in the PM_2.5 size fraction of the HVDS samples. In the dry period levoglucosan reached concentrations of up to 7.5 μg m⁻³ and exhibited diel variations with a nighttime prevalence. It was closely associated with the PM mass in the size-segregated samples and was mainly present in the fine mode, except during the wet period where it peaked in the coarse mode. Isoprene SOA tracers showed an average concentration of 250 ng m⁻³ during the dry period versus 157 ng m⁻³ during the transition period and 52 ng m⁻³ during the wet period. Malic acid and the 2-methyltetrols exhibited a different size distribution pattern, which is consistent with different aerosol formation processes (i.e., gas-to-particle partitioning in the case of malic acid and heterogeneous formation from gas-phase precursors in the case of

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

Science.gov (United States)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

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

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

Lidar investigations of atmospheric aerosols over Sofia

International Nuclear Information System (INIS)

Dreischuh, T.; Deleva, A.; Peshev, Z.; Grigorov, I.; Kolarov, G.; Stoyanov, D.

2016-01-01

An overview is given of the laser remote sensing of atmospheric aerosols and related processes over the Sofia area performed in the Institute of Electronics, Bulgarian Academy of Sciences, during the last three years. Results from lidar investigations of the optical characteristics of atmospheric aerosols obtained in the frame of the European Aerosol Research Lidar Network, as well as from the lidar mapping of near-surface aerosol fields for remote monitoring of atmospheric pollutants are presented and discussed in this paper.

Processing methods for operation test data of radioactive aerosols monitor based on accumulation techniques

International Nuclear Information System (INIS)

Fu Cuiming; Xi Pingping; Ma Yinghao; Tan Linglong; Shen Fu

2011-01-01

This article introduces a radioactive aerosol continuous monitor based on accumulation sampling and measuring and three methods for processing the operation data. The monitoring results are processed by the 3 methods which are applied both under the conditions of natural background and at workplaces of a nuclear facility. How the monitoring results are assessed and how to calculate the detection limit when using the 3 different methods are explained. Moreover, the advantages and disadvantages of the 3 methods are discussed. (authors)

Attachment of radon progeny to cigarette-smoke aerosols

International Nuclear Information System (INIS)

Biermann, A.H.; Sawyer, S.R.

1995-05-01

The daughter products of radon gas are now recognized as a significant contributor to radiation exposure to the general public. It is also suspected that a synergistic effect exists with the combination cigarette smoking and radon exposure. We have conducted an experimental investigation to determine the physical nature of radon progeny interactions with cigarette smoke aerosols. The size distributions of the aerosols are characterized and attachment rates of radon progeny to cigarette-smoke aerosols are determined. Both the mainstream and sidestream portions of the smoke aerosol are investigated. Unattached radon progeny are very mobile and, in the presence of aerosols, readily attach to the particle surfaces. In this study, an aerosol chamber is used to contain the radon gas, progeny and aerosol mixture while allowing the attachment process to occur. The rate of attachment is dependent on the size distribution, or diffusion coefficient, of the radon progeny as well as the aerosol size distribution. The size distribution of the radon daughter products is monitored using a graded-screen diffusion battery. The diffusion battery also enables separation of the unattached radon progeny from those attached to the aerosol particles. Analysis of the radon decay products is accomplished using alpha spectrometry. The aerosols of interest are size fractionated with the aid of a differential mobility analyzer and cascade impactor. The measured attachment rates of progeny to the cigarette smoke are compared to those found in similar experiments using an ambient aerosol. The lowest attachment coefficients observed, ∼10 -6 cm 3 /s, occurred for the ambient aerosol. The sidestream and mainstream smoke aerosols exhibited higher attachment rates in that order. The results compared favorably with theories describing the coagulation process of aerosols

Interaction of Microphysical Aerosol Processes with Hydrodynamics Mixing

KAUST Repository

Alshaarawi, Amjad

2015-01-01

) streams owing from opposite nozzles. A mixing layer is established across a stagnation plane in the center where nucleation and other aerosol dynamics are triggered. The second is homogeneous isotropic turbulence in a three-dimensional periodic domain

Geochemical, Sulfur Isotopic Characteristics and Source Contributions of Size-Aggregated Aerosols Collected in Baring Head, New Zealand.

Science.gov (United States)

Li, J.; Michalski, G. M.; Davy, P.; Harvey, M.; Wilkins, B. P.; Katzman, T. L.

2017-12-01

Sulfate aerosols are critical to the climate, human health, and the hydrological cycle in the atmosphere, yet the sources of sulfate in aerosols are not completely understood. In this work, we evaluated the sources of sulfate in size-aggregated aerosols from the Southern Pacific Ocean and the land of New Zealand using geochemical and isotopic analyses. Aerosols were collected at Baring Head, New Zealand between 6/30/15 to 8/4/16 using two collectors, one only collects Southern Pacific Ocean derived aerosols (open-ocean collector), the other collects aerosols from both the ocean and the land (all-direction collector). Each collector is equipped with two filters to sample size-aggregated aerosols (fine aerosols: NSS-SO42-, 70%), while coarse aerosols are dominated by sea-salt sulfate. However, some NSS-SO42- was also observed in coarse aerosols collected in summer, suggesting the presence of accumulation mode NSS-SO42- aerosols, which is possibly due to high summer biogenic DMS flux. The sources of sulfur in NSS-SO42- could be further determined by their d34S values. DMS emission is likely the sole sulfur source in the open-ocean collector as it shows constant DMS-like d34S signatures (15-18‰) throughout the year. Meanwhile, the d34S of NSS-SO42- in the all-direction collector display a seasonal trend: summer time d34S values are higher and DMS-like (15-18‰), indicating DMS emission is the dominant sulfur source; winter time d34S values are lower ( 6-12‰), therefore the sulfur is likely sourced from both DMS emission and terrestrial S input with low d34S values, such as volcanic activities, fossil fuel and wood burning.

Assessing physical models used in nuclear aerosol transport models

International Nuclear Information System (INIS)

McDonald, B.H.

1987-01-01

Computer codes used to predict the behaviour of aerosols in water-cooled reactor containment buildings after severe accidents contain a variety of physical models. Special models are in place for describing agglomeration processes where small aerosol particles combine to form larger ones. Other models are used to calculate the rates at which aerosol particles are deposited on building structures. Condensation of steam on aerosol particles is currently a very active area in aerosol modelling. In this paper, the physical models incorporated in the current available international codes for all of these processes are reviewed and documented. There is considerable variation in models used in different codes, and some uncertainties exist as to which models are superior. 28 refs

Steam condensation modelling in aerosol codes

International Nuclear Information System (INIS)

Dunbar, I.H.

1986-01-01

The principal subject of this study is the modelling of the condensation of steam into and evaporation of water from aerosol particles. These processes introduce a new type of term into the equation for the development of the aerosol particle size distribution. This new term faces the code developer with three major problems: the physical modelling of the condensation/evaporation process, the discretisation of the new term and the separate accounting for the masses of the water and of the other components. This study has considered four codes which model the condensation of steam into and its evaporation from aerosol particles: AEROSYM-M (UK), AEROSOLS/B1 (France), NAUA (Federal Republic of Germany) and CONTAIN (USA). The modelling in the codes has been addressed under three headings. These are the physical modelling of condensation, the mathematics of the discretisation of the equations, and the methods for modelling the separate behaviour of different chemical components of the aerosol. The codes are least advanced in area of solute effect modelling. At present only AEROSOLS/B1 includes the effect. The effect is greater for more concentrated solutions. Codes without the effect will be more in error (underestimating the total airborne mass) the less condensation they predict. Data are needed on the water vapour pressure above concentrated solutions of the substances of interest (especially CsOH and CsI) if the extent to which aerosols retain water under superheated conditions is to be modelled. 15 refs

Quantifying enhancement in aerosol radiative forcing during 'extreme aerosol days' in summer at Delhi National Capital Region, India.

Science.gov (United States)

Kumar, Sumant; Dey, Sagnik; Srivastava, Arun

2016-04-15

Changes in aerosol characteristics (spectral aerosol optical depth, AOD and composition) are examined during the transition from 'relatively clean' to 'extreme' aerosol days in the summer of 2012 at Delhi National Capital Region (NCR), India. AOD smaller than 0.54 (i.e. 12-year mean AOD-1σ) represents 'relatively clean' days in Delhi during the summer. 'Extreme' days are defined by the condition when AOD0.5 exceeds 12-year mean AOD+1 standard deviation (σ). Mean (±1σ) AOD increases to 1.2±0.12 along with a decrease of Angstrom Exponent from 0.54±0.09 to 0.22±0.12 during the 'extreme' days. Aerosol composition is inferred by fixing the number concentrations of various individual species through iterative tweaking when simulated (following Mie theory) AOD spectrum matches with the measured one. Contribution of coarse mode dust to aerosol mass increased from 76.8% (relatively clean) to 96.8% (extreme events), while the corresponding contributions to AOD0.5 increased from 35.0% to 70.8%. Spectrally increasing single scattering albedo (SSA) and CALIPSO aerosol sub-type information support the dominant presence of dust during the 'extreme' aerosol days. Aerosol direct radiative forcing (ADRF) at the top-of-the-atmosphere increases from 21.2Wm(-2) (relatively clean) to 56.6Wm(-2) (extreme), while the corresponding change in surface ADRF is from -99.5Wm(-2) to -153.5Wm(-2). Coarse mode dust contributes 60.3% of the observed surface ADRF during the 'extreme' days. On the contrary, 0.4% mass fraction of black carbon (BC) translates into 13.1% contribution to AOD0.5 and 33.5% to surface ADRF during the 'extreme' days. The atmospheric heating rate increased by 75.1% from 1.7K/day to 2.96K/day during the 'extreme' days. Copyright © 2016 Elsevier B.V. All rights reserved.

Determination of the columnar aerosol size distribution by inversion of spectral aerosol optical depth measurements at different areas in Egypt

International Nuclear Information System (INIS)

EI-Metwally, M.; Madkour, M.A.

2006-01-01

Aerosols have a great effects on nuclear safety calculations and atmospheric environment. The aerosol optical depth measurements are carried out at four areas in Egypt: Cairo and Helwan as urban/industrial areas, Aswan as an arid area and Mansoura as an agricultural area covering the period from Jun 1992 to May 1993. These measurements were recorded by ground-based pyrheliometers with large band-pass filters. Monthly average values of aerosol optical depth (AOD) showed a pronounced temporal trend, with a maximum AOD during summer and the transition seasons (spring and autumn) at all sites. Levels of AODs are higher at both urban and industrial areas than at other areas. Variation of Angstrom exponent a with the AOD was clear at most sites and the a value depends on the spectral range used in its determination. The mean contribution of anthropogenic sources to AOD over Cairo was at the range of 25.1-54.3%, whereas those values in Helwan were at the range of 34.5-59.8%. Finally, columnar aerosol size distributions have been inferred by inverting particularly AOD measurements as a function of wavelength. The Junge (type I) and bimodal (type III) distributions are dominant at urban and arid areas (Cairo and Aswan), whereas mono dispersion distribution (type II) are dominant in industrial and agricultural areas (Helwan and Mansoura). In Cairo and Aswan, the peak of columnar size distribution for the fine mode at radius r is around 0.1 and 0.2 μm respectively, while it is around 1.0 and 2.0 μm for the coarse mode. .Also, the peak of size distribution for the mono dispersion mode was marked at radius around 0.2 μm at both Helwan and Mansoura. A comprehensive comparison of our results with literature size distributions is very sparse, nevertheless, our size distributions in general agree with them

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.

Impact of anthropogenic aerosols on present and future climate

International Nuclear Information System (INIS)

Deandreis, C.

2008-03-01

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

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

Directory of Open Access Journals (Sweden)

W. T. Morgan

2010-09-01

Full Text Available A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM. Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models.

The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where

Atmospheric residence times of continental aerosols

International Nuclear Information System (INIS)

Balkanski, Y.J.

1991-01-01

The global atmospheric distributions of Rn-222 are simulated with a three-dimensional model of atmospheric transport based on the meteorology of the NASA Goddard Institute for Space Studies (GISS) general circulation model. The short-lived radioactive gas Rn-222 (half-life = 3.8d) is emitted almost exclusively from land, at a relatively uniform rate; hence it is an excellent tracer of continental influences. Lead-210 is produced by decay of Rn-222 and immediately condenses to preexisting aerosol surfaces. It provides an excellent measure of aerosol residence times in the atmosphere because its source is accurately defined by the Rn-222 distribution. Results from the three-dimensional model are compared to measurements of Rn-222 and Pb-210 atmospheric concentrations to evaluate model's long-range transport over oceanic regions and to study the deposition mechanisms of atmospheric aerosols. Model results for Rn-222 are used to examine the long-range transport of continental air over two selected oceanic regions, the subantarctic Indian Ocean and the North Pacific. It is shown that the fast transport of air from southern Africa causes substantial continental pollution at southern mid-latitudes, a region usually regarded as pristine. Air over the North Pacific is heavily impacted by continental influences year round, but the altitude at which the transport occurs varies seasonally. Observations of aerosols at island sites, which are commonly used as diagnostics of continental influences, may be misleading because they do not account for influences at high altitude and because aerosols are efficiently scavenged by deposition during transport. The study of Pb-210 focuses on defining the residence times of submicron aerosols in the troposphere. Scavenging in wet convective updrafts is found to provide the dominant sink on a global scale

A statistical analysis of North East Atlantic (submicron aerosol size distributions

Directory of Open Access Journals (Sweden)

M. Dall'Osto

2011-12-01

Full Text Available The Global Atmospheric Watch research station at Mace Head (Ireland offers the possibility to sample some of the cleanest air masses being imported into Europe as well as some of the most polluted being exported out of Europe. We present a statistical cluster analysis of the physical characteristics of aerosol size distributions in air ranging from the cleanest to the most polluted for the year 2008. Data coverage achieved was 75% throughout the year. By applying the Hartigan-Wong k-Means method, 12 clusters were identified as systematically occurring. These 12 clusters could be further combined into 4 categories with similar characteristics, namely: coastal nucleation category (occurring 21.3 % of the time, open ocean nucleation category (occurring 32.6% of the time, background clean marine category (occurring 26.1% of the time and anthropogenic category (occurring 20% of the time aerosol size distributions. The coastal nucleation category is characterised by a clear and dominant nucleation mode at sizes less than 10 nm while the open ocean nucleation category is characterised by a dominant Aitken mode between 15 nm and 50 nm. The background clean marine aerosol exhibited a clear bimodality in the sub-micron size distribution, with although it should be noted that either the Aitken mode or the accumulation mode may dominate the number concentration. However, peculiar background clean marine size distributions with coarser accumulation modes are also observed during winter months. By contrast, the continentally-influenced size distributions are generally more monomodal (accumulation, albeit with traces of bimodality. The open ocean category occurs more often during May, June and July, corresponding with the North East (NE Atlantic high biological period. Combined with the relatively high percentage frequency of occurrence (32.6%, this suggests that the marine biota is an important source of new nano aerosol particles in NE Atlantic Air.

Aerosol optical properties at rural background area in Western Saudi Arabia

Science.gov (United States)

Lihavainen, H.; Alghamdi, M. A.; Hyvärinen, A.; Hussein, T.; Neitola, K.; Khoder, M.; Abdelmaksoud, A. S.; Al-Jeelani, H.; Shabbaj, I. I.; Almehmadi, F. M.

2017-11-01

To derive the comprehensive aerosol in situ characteristics at a rural background area in Saudi Arabia, an aerosol measurements station was established to Hada Al Sham, 60 km east from the Red Sea and the city of Jeddah. The present sturdy describes the observational data from February 2013 to February 2015 of scattering and absorption coefficients, Ångström exponents and single scattering albedo over the measurement period. The average scattering and absorption coefficients at wavelength 525 nm were 109 ± 71 Mm- 1 (mean ± SD, at STP conditions) and 15 ± 17 Mm- 1 (at STP conditions), respectively. As expected, the scattering coefficient was dominated by large desert dust particles with low Ångström scattering exponent, 0.49 ± 0.62. Especially from February to June the Ångström scattering exponent was clearly lower (0.23) and scattering coefficients higher (124 Mm- 1) than total averages because of the dust outbreak season. Aerosol optical properties had clear diurnal cycle. The lowest scattering and absorption coefficients and aerosol optical depths were observed around noon. The observed diurnal variation is caused by wind direction and speed, during night time very calm easterly winds are dominating whereas during daytime the stronger westerly winds are dominating (sea breeze). Positive Matrix Factorization mathematical tool was applied to the scattering and absorption coefficients and PM2.5 and coarse mode (PM10-PM2.5) mass concentrations to identify source characteristics. Three different factors with clearly different properties were found; anthropogenic, BC source and desert dust. Mass absorption efficiencies for BC source and desert dust factors were, 6.0 m2 g- 1 and 0.4 m2 g- 1, respectively, and mass scattering efficiencies for anthropogenic (sulphate) and desert dust, 2.5 m2 g- 1 and 0.8 m2 g- 1, respectively.

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

Adiabatic and diabatic aerosol transport to the Jungfraujoch

Energy Technology Data Exchange (ETDEWEB)

Lugauer, M.; Baltensperger, U.; Furger, M.; Jost, D.T.; Schwikowski, M.; Gaeggeler, H.W. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1997-09-01

Synoptic scale vertical motion, here detected by the geopotential height of the 500 hPa surface, mainly accounts for the aerosol transport to the Jungfraujoch in winter. In summer, diabatic convection provides the dominant vertical transport mechanism. Nevertheless, synoptic scale adiabatic motion still determines whether diabatic convection can develop. (author) 2 figs., 2 refs.

Classifying Aerosols Based on Fuzzy Clustering and Their Optical and Microphysical Properties Study in Beijing, China

Directory of Open Access Journals (Sweden)

Wenhao Zhang

2017-01-01

Full Text Available Classification of Beijing aerosol is carried out based on clustering optical properties obtained from three Aerosol Robotic Network (AERONET sites. The fuzzy c-mean (FCM clustering algorithm is used to classify fourteen-year (2001–2014 observations, totally of 6,732 records, into six aerosol types. They are identified as fine particle nonabsorbing, two kinds of fine particle moderately absorbing (fine-MA1 and fine-MA2, fine particle highly absorbing, polluted dust, and desert dust aerosol. These aerosol types exhibit obvious optical characteristics difference. While five of them show similarities with aerosol types identified elsewhere, the polluted dust aerosol has no comparable prototype. Then the membership degree, a significant parameter provided by fuzzy clustering, is used to analyze internal variation of optical properties of each aerosol type. Finally, temporal variations of aerosol types are investigated. The dominant aerosol types are polluted dust and desert dust in spring, fine particle nonabsorbing aerosol in summer, and fine particle highly absorbing aerosol in winter. The fine particle moderately absorbing aerosol occurs during the whole year. Optical properties of the six types can also be used for radiative forcing estimation and satellite aerosol retrieval. Additionally, methodology of this study can be applied to identify aerosol types on a global scale.

Aerosol chemical composition at Cabauw, The Netherlands as observed in two intensive periods in May 2008 and March 2009

Directory of Open Access Journals (Sweden)

A. A. Mensah

2012-05-01

Full Text Available Observations of aerosol chemical composition in Cabauw, the Netherlands, are presented for two intensive measurement periods in May 2008 and March 2009. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS and is compared to observations from aerosol size distribution measurements as well as composition measurements with a Monitor for AeRosol and GAses (MARGA based instrument and a Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS. An overview of the data is presented and the data quality is discussed. In May 2008 enhanced pollution was observed with organics contributing 40% to the PM₁ mass. In contrast the observed average mass loading was lower in March 2009 and a dominance of ammonium nitrate (42% was observed. The semi-volatile nature of ammonium nitrate is evident in the diurnal cycles with maximum concentrations observed in the morning hours in May 2008 and little diurnal variation observed in March 2009. Size dependent composition data from AMS measurements are presented and show a dominance of organics in the size range below 200 nm. A higher O:C ratio of the organics is observed for May 2008 than for March 2009. Together with the time series of individual tracer ions this shows the dominance of OOA over HOA in May 2008.

Laboratory Investigation of Contact Freezing and the Aerosol to Ice Crystal Transformation Process

Energy Technology Data Exchange (ETDEWEB)

Shaw, Raymond A. [Michigan Technological Univ., Houghton, MI (United States)

2014-10-28

This project has been focused on the following objectives: 1. Investigations of the physical processes governing immersion versus contact nucleation, specifically surface-induced crystallization; 2. Development of a quadrupole particle trap with full thermodynamic control over the temperature range 0 to –40 °C and precisely controlled water vapor saturation ratios for continuous, single-particle measurement of the aerosol to ice crystal transformation process for realistic ice nuclei; 3. Understanding the role of ice nucleation in determining the microphysical properties of mixed-phase clouds, within a framework that allows bridging between laboratory and field measurements.

Characteristics of Aerosol Transport from Asia to the West Coast of North America

Science.gov (United States)

Brock, C. A.; Bahreini, R.; Middlebrook, A. M.; Atlas, E. L.; Blake, D. R.; Brioude, J.; Cooper, O. R.; de Gouw, J. A.; Holloway, J. S.; Lack, D. A.; Langridge, J. M.; Meinardi, S.; Nowak, J. B.; Peischl, J.; Perring, A.; Pollack, I. B.; Roberts, J. M.; Ryerson, T. B.; Schwarz, J. P.; Spackman, J. R.; Trainer, M.; Trytko, J.; Warneke, C.

2010-12-01

During the CalNex field program of May and June 2010, the NOAA WP-3D aircraft observed several layers of enhanced trace gas mixing ratios and aerosol concentrations at altitudes ranging from 1 to 4 km over southern and central California. The submicron aerosol composition within these layers was dominated by partially neutralized sulfate, while nitrate, organic matter and black carbon were only minor constituents. The particle layers were associated with trace gases, such as benzene and sulfur dioxide, consistent with anthropogenic fossil fuel emissions, and were not associated with enhancements of the biomass burning tracer acetonitrile. The particle size distribution was dominated by a single accumulation mode that is characteristic of a well aged aerosol. Transport modeling indicates an Asian source for these layers of pollution. Dew point temperatures within the layers were less than -15 degrees Celsius, indicating desiccation by precipitation during transport. Taken together, these observations are consistent with those from earlier studies in which was diagnosed the removal of primary and organic particles by precipitation scavenging during uplift from the polluted Asian boundary layer into the free troposphere. Oxidation of residual sulfur dioxide that remained following transport through the cloud system may have resulted in the observed sulfate-rich aerosol. The repeated observation of such layers suggests that wet scavenging frequently modifies the chemical and optical characteristics of aerosols emitted in urban regions in Asia and transported in the free troposphere across the Pacific.

The economics and ethics of aerosol geoengineering strategies

Science.gov (United States)

Goes, Marlos; Keller, Klaus; Tuana, Nancy

2010-05-01

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

Deposition of aerosol particles in bent pipe

International Nuclear Information System (INIS)

Matsui, Hiroshi; Ohhata, Tsutomu

1989-01-01

An equation to estimate deposition fraction of aerosol particles in a bent pipe is derived and the validity is verified experimentally. The equation is obtained by assuming that the resultant acceleration of the gravity and the centrifugal force induced in the bend acts on the aerosol particles, and is found to give a relatively accurate estimation of the deposition fraction if a certain correction factor is introduced to the equation. The deposition fraction has a minimum against Reynold number, and the deposition due to centrifugal force dominates at greater Reynolds number than that at the minimum deposition fraction. On the other hand, the smaller the radius of curvature of the bend is, the larger the deposition fraction due to the centrifugal force is. (author)

Removal of Aerosol Particles Generated from Vitrification Process for High-Level Liquid Wastes

OpenAIRE

加藤 功

1990-01-01

The vitrification technology has been developed for the high-level liquid waste (HLLW) from reprocessing nuclear spent fuel in PNC. The removal performance of the aerosol particles generated from the melting process was studied in a nonradioactive full-scale mock-up test facility (MTF). The off-gas treatment system consists of submerged bed scrubber (SBS), venturi scrubber, NOx absorber, high efficiency mist eliminater (HEME). Deoomtamination factors (DFs) were derived from the mass ratio of ...

Aerosol-Cloud-Precipitation Interactions in WRF Model:Sensitivity to Autoconversion Parameterization

Institute of Scientific and Technical Information of China (English)

解小宁; 刘晓东

2015-01-01

Cloud-to-rain autoconversion process is an important player in aerosol loading, cloud morphology, and precipitation variations because it can modulate cloud microphysical characteristics depending on the par-ticipation of aerosols, and aff ects the spatio-temporal distribution and total amount of precipitation. By applying the Kessler, the Khairoutdinov-Kogan (KK), and the Dispersion autoconversion parameterization schemes in a set of sensitivity experiments, the indirect eff ects of aerosols on clouds and precipitation are investigated for a deep convective cloud system in Beijing under various aerosol concentration backgrounds from 50 to 10000 cm−3. Numerical experiments show that aerosol-induced precipitation change is strongly dependent on autoconversion parameterization schemes. For the Kessler scheme, the average cumulative precipitation is enhanced slightly with increasing aerosols, whereas surface precipitation is reduced signifi-cantly with increasing aerosols for the KK scheme. Moreover, precipitation varies non-monotonically for the Dispersion scheme, increasing with aerosols at lower concentrations and decreasing at higher concentrations. These diff erent trends of aerosol-induced precipitation change are mainly ascribed to diff erences in rain wa-ter content under these three autoconversion parameterization schemes. Therefore, this study suggests that accurate parameterization of cloud microphysical processes, particularly the cloud-to-rain autoconversion process, is needed for improving the scientifi c understanding of aerosol-cloud-precipitation interactions.

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

Science.gov (United States)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

Aerosol effects on the photochemistry in Mexico City during MCMA-2006/MILAGRO campaign

Directory of Open Access Journals (Sweden)

G. Li

2011-06-01

Full Text Available In the present study, the impact of aerosols on the photochemistry in Mexico City is evaluated using the WRF-CHEM model for the period from 24 to 29 March during the MCMA-2006/MILAGRO campaign. An aerosol radiative module has been developed with detailed consideration of aerosol size, composition, and mixing. The module has been coupled into the WRF-CHEM model to calculate the aerosol optical properties, including optical depth, single scattering albedo, and asymmetry factor. Calculated aerosol optical properties are in good agreement with the surface observations and aircraft and satellite measurements during daytime. In general, the photolysis rates are reduced due to the absorption by carbonaceous aerosols, particularly in the early morning and late afternoon hours with a long aerosol optical path. However, with the growth of aerosol particles and the decrease of the solar zenith angle around noontime, aerosols can slightly enhance photolysis rates when ultraviolet (UV radiation scattering dominates UV absorption by aerosols at the lower-most model layer. The changes in photolysis rates due to aerosols lead to about 2–17 % surface ozone reduction during daytime in the urban area in Mexico City with generally larger reductions during early morning hours near the city center, resulting in a decrease of OH level by about 9 %, as well as a decrease in the daytime concentrations of nitrate and secondary organic aerosols by 5–6 % on average. In addition, the rapid aging of black carbon aerosols and the enhanced absorption of UV radiation by organic aerosols contribute substantially to the reduction of photolysis rates.

Simulation of processes of water aerosol coagulation-condensation growth using a combination of methods of groups and fractions

International Nuclear Information System (INIS)

Alexander G Godizov; Alexander D Efanov; Alexander A Lukianov; Olga V Supotnitskaya

2005-01-01

Full text of publication follows: To describe the phenomena involving aerosol, the model in lumped parameters is used, which is based on the kinetic integral-differential equation for the function of particle distribution of size and content of soluble and insoluble impurities with sources and collision integrals. By the function of particle size distribution, the integral parameters of aerosol can be determined: water content (mass of condensed moisture in a unit of volume), dust content (mass of insoluble condensation nuclei in a unit of volume), calculational concentration and the mean radius of particles. In the aerosol transfer problem being considered, the thermodynamic fields are the external data obtained with a thermal-hydraulic computer code. For numerical simulation of the kinetic equation describing aerosol behavior in coagulation-condensation processes, a hybrid method is used, which combines the method of groups and the method of fractions. To solve the complete equation of aerosol transfer, the method of fractions is used. The integral equation describing aerosol coagulation is solved by means of the group method. The group method based on the representation of particle size distribution in terms of a linear combination of δ-functions with time-dependent arguments makes it possible to calculate the integral parameters of spectrum: the moments of distribution function at a small number of groups. The test calculations were performed by giving the particle spectrum as a lognormal distribution and Γ- function. The hybrid method combined with the thermal-hydraulic computer code enables one to simulate volume condensation of steam at varying thermal-hydraulic conditions. (authors)

Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

Directory of Open Access Journals (Sweden)

F. Freutel

2013-01-01

Full Text Available During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m⁻³, 2 μg m⁻³, 2 μg m⁻³, and 7 μg m⁻³, respectively were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m⁻³, 0.2 μg m⁻³, 0.4 μg m⁻³, and 1–3 μg m⁻³, respectively. For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NO_x it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be

Submicron aerosol distributions and CCN activity measured in and around the Korean Peninsula during KORUS-AQ

Science.gov (United States)

Park, M.; Kim, N.; Yum, S. S.; Thornhill, K. L., II; Anderson, B. E.; Kim, D. S.; Kim, H. J.; Jeon, H. E.; Park, Y. S.; Lee, S. B.

2017-12-01

KORUS-AQ is a field campaign aimed at investigating formation of ozone and aerosol and interactions between chemistry, transport and various sources in the Korean Peninsula which is the region affected both by long-range transport and local emission. Aerosol number concentration and size distribution, and CCN number concentration were measured on board the NASA DC-8 research aircraft and at a ground site at Olympic Park in Seoul, capital city of Korea during the KORUS-AQ campaign (May 2nd to June 10th, 2017). There were 20 flights during the KORUS-AQ campaign and total flight time was about 150 hours. CCN counter (CCNC) on the airborne platform was operated at the fixed internal supersaturation of 0.6% and CCNC at the ground site was operated at five different supersaturations (0.2%, 0.4%, 0.6%, 0.8%, and 1.0%). Aerosol hygroscopic parameter κ was also estimated from CCN number concentration and aerosol size distribution. Airborne measurements showed a large spatio-temporal variation of aerosol number concentration and CCN activity in and around the Korean peninsula, and the ground measurements also showed a large temporal variation. The campaign period can be classified into long-range transport dominant cases, local emission dominant cases due to stagnant air mass, and others. Aerosol number concentration in the Korean Peninsula measured in stagnant air mass period was higher than those in long-range transport period, but CCN number concentration showed an opposite tendency. Both aerosol and CCN number concentrations over the Yellow Sea in local emission period were slightly higher than those in long-range transport period. Since CCN activity is different depending on time and space, our focus is on understanding how CCN activity and aerosol hygroscopicity vary with the source of aerosol. Comprehensive analysis results will be shown at the conference.

Impact of springtime biomass-burning aerosols on radiative forcing over northern Thailand during the 7SEAS campaign

Science.gov (United States)

Pani, Shantanu Kumar; Wang, Sheng-Hsiang; Lin, Neng-Huei; Lee, Chung-Te; Tsay, Si-Chee; Holben, Brent; Janjai, Serm; Hsiao, Ta-Chih; Chuang, Ming-Tung; Chantara, Somporn

2016-04-01

Biomass-burning (BB) aerosols are the significant contributor to the regional/global aerosol loading and radiation budgets. BB aerosols affect the radiation budget of the earth and atmosphere by scattering and absorbing directly the incoming solar and outgoing terrestrial radiation. These aerosols can exert either cooling or warming effect on climate, depending on the balance between scattering and absorption. BB activities in the form of wildland forest fires and agricultural crop burning are very pronounced in the Indochina peninsular regions in Southeast Asia mainly in spring (late February to April) season. The region of interest includes Doi Ang Khang (19.93° N, 99.05° E, 1536 msl) in northern Thailand, as part of the Seven South East Asian Studies (7-SEAS)/BASELInE (Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles & Interactions Experiment) campaign in 2013. In this study, for the first time, the direct aerosol radiative effects of BB aerosols over near-source BB emissions, during the peak loading spring season, in northern Indochina were investigated by using ground-based physical, chemical, and optical properties of aerosols as well as the aerosol optical and radiative transfer models. Information on aerosol parameters in the field campaign was used in the OPAC (Optical Properties of Aerosols and Clouds) model to estimate various optical properties corresponding to aerosol compositions. Clear-sky shortwave direct aerosol radiative effects were further estimated with a raditive transfer model SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer). The columnar aerosol optical depth (AOD500) was found to be ranged from 0.26 to 1.13 (with the mean value 0.71 ± 0.24). Fine-mode (fine mode fraction ≈0.98, angstrom exponent ≈1.8) and significantly absorbing aerosols (columnar single-scattering albedo ≈0.89, asymmetry-parameter ≈0.67 at 441 nm wavelength) dominated in this region. Water soluble and black carbon (BC) aerosols mainly

MISR Aerosol Product Attributes and Statistical Comparisons with MODIS

Science.gov (United States)

Kahn, Ralph A.; Nelson, David L.; Garay, Michael J.; Levy, Robert C.; Bull, Michael A.; Diner, David J.; Martonchik, John V.; Paradise, Susan R.; Hansen, Earl G.; Remer, Lorraine A.

2009-01-01

In this paper, Multi-angle Imaging SpectroRadiometer (MISR) aerosol product attributes are described, including geometry and algorithm performance flags. Actual retrieval coverage is mapped and explained in detail using representative global monthly data. Statistical comparisons are made with coincident aerosol optical depth (AOD) and Angstrom exponent (ANG) retrieval results from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument. The relationship between these results and the ones previously obtained for MISR and MODIS individually, based on comparisons with coincident ground-truth observations, is established. For the data examined, MISR and MODIS each obtain successful aerosol retrievals about 15% of the time, and coincident MISR-MODIS aerosol retrievals are obtained for about 6%-7% of the total overlap region. Cloud avoidance, glint and oblique-Sun exclusions, and other algorithm physical limitations account for these results. For both MISR and MODIS, successful retrievals are obtained for over 75% of locations where attempts are made. Where coincident AOD retrievals are obtained over ocean, the MISR-MODIS correlation coefficient is about 0.9; over land, the correlation coefficient is about 0.7. Differences are traced to specific known algorithm issues or conditions. Over-ocean ANG comparisons yield a correlation of 0.67, showing consistency in distinguishing aerosol air masses dominated by coarse-mode versus fine-mode particles. Sampling considerations imply that care must be taken when assessing monthly global aerosol direct radiative forcing and AOD trends with these products, but they can be used directly for many other applications, such as regional AOD gradient and aerosol air mass type mapping and aerosol transport model validation. Users are urged to take seriously the published product data-quality statements.

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

Sources of anions in aerosols in northeast Greenland during late winter

Directory of Open Access Journals (Sweden)

M. Fenger

2013-02-01

Full Text Available The knowledge of climate effects of atmospheric aerosols is associated with large uncertainty, and a better understanding of their physical and chemical properties is needed, especially in the Arctic environment. The objective of the present study is to improve our understanding of the processes affecting the composition of aerosols in the high Arctic. Therefore size-segregated aerosols were sampled at a high Arctic site, Station Nord (Northeast Greenland, in March 2009 using a Micro Orifice Uniform Deposit Impactor. The aerosol samples were extracted in order to analyse three water-soluble anions: chloride, nitrate and sulphate. The results are discussed based on possible chemical and physical transformations as well as transport patterns.

The total concentrations of the ions at Station Nord were 53–507 ng m⁻³, 2–298 ng m⁻³ and 535–1087 ng m⁻³ for chloride (Cl⁻, nitrate (NO₃⁻ and sulphate (SO₄²⁻, respectively. The aerosols in late winter/early spring, after polar sunrise, are found to be a mixture of long-range transported and regional to local originating aerosols. Fine particles, smaller than 1 μm, containing SO₄²⁻, Cl⁻ and NO₃⁻, are hypothesized to originate from long-range transport, where SO₄²⁻ is by far the dominating anion accounting for 50–85% of the analyzed mass. The analysis suggests that Cl⁻ and NO₃⁻ in coarser particles (> 1.5 μm originate from local/regional sources. Under conditions where the air mass is transported over sea ice at high wind speeds, very coarse particles (> 18 μm are observed, and it is hypothesized that frost flowers on the sea ice are a source of the very coarse nitrate particles.

Atmospheric Residence Times of Continental Aerosols.

Science.gov (United States)

Balkanski, Yves Jacques

The global atmospheric distributions of ^{222}Rn and ^{210 }Pb are simulated with a three-dimensional model of atmospheric transport based on the meteorology of the NASA GISS^1>=neral circulation model. The short-lived radioactive gas ^ {222}Rn (half-life = 3.8d) is emitted almost exclusively from land, at a relatively uniform rate; hence it is an excellent tracer of continental influences. Lead -210 is produced by decay of ^{222} Rn and immediately condenses to preexisting aerosol surfaces. It provides an excellent measure of aerosol residence times in the atmosphere because its source is accurately defined by the ^{222} Rn distribution. Results from the three-dimensional model are compared to measurements of ^ {222}Rn and ^{210 }Pb atmospheric concentrations to evaluate model's long-range transport over oceanic regions and to study the deposition mechanisms of atmospheric aerosols. Model results for ^{222} Rn are used to examine the long-range transport of continental air over two selected oceanic regions, the subantartic Indian Ocean and the North Pacific. It is shown that fast transport of air from southern Africa causes substantial continental pollution at southern mid-latitudes, a region usually regarded as pristine. Air over the North Pacific is heavily impacted by continental influences year round, but the altitude at which the transport occurs varies seasonally. Observations of aerosols at island sites, which are commonly used as diagnostics of continental influences, may be misleading because they do not account for influences at high altitude and because aerosols are efficiently scavenged by deposition during transport. The study of ^{210}Pb focuses on defining the residence times of submicron aerosols in the troposphere. Scavenging in wet convective updrafts is found to provide the dominant sink on a global scale. The globally averaged residence time for ^{210 }Pb-containing aerosols in the troposphere is 7 days. The average increase in residence time

Climate forcing by anthropogenic aerosols

Energy Technology Data Exchange (ETDEWEB)

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

1992-01-24

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

Climate forcing by anthropogenic aerosols.

Science.gov (United States)

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

1992-01-24

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

Changing transport processes in the stratosphere by radiative heating of sulfate aerosols

Directory of Open Access Journals (Sweden)

U. Niemeier

2017-12-01

Full Text Available The injection of sulfur dioxide (SO2 into the stratosphere to form an artificial stratospheric aerosol layer is discussed as an option for solar radiation management. Sulfate aerosol scatters solar radiation and absorbs infrared radiation, which warms the stratospheric sulfur layer. Simulations with the general circulation model ECHAM5-HAM, including aerosol microphysics, show consequences of this warming, including changes of the quasi-biennial oscillation (QBO in the tropics. The QBO slows down after an injection of 4 Tg(S yr−1 and completely shuts down after an injection of 8 Tg(S yr−1. Transport of species in the tropics and sub-tropics depends on the phase of the QBO. Consequently, the heated aerosol layer not only impacts the oscillation of the QBO but also the meridional transport of the sulfate aerosols. The stronger the injection, the stronger the heating and the simulated impact on the QBO and equatorial wind systems. With increasing injection rate the velocity of the equatorial jet streams increases, and the less sulfate is transported out of the tropics. This reduces the global distribution of sulfate and decreases the radiative forcing efficiency of the aerosol layer by 10 to 14 % compared to simulations with low vertical resolution and without generated QBO. Increasing the height of the injection increases the radiative forcing only for injection rates below 10 Tg(S yr−1 (8–18 %, a much smaller value than the 50 % calculated previously. Stronger injection rates at higher levels even result in smaller forcing than the injections at lower levels.

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

NARCIS (Netherlands)

Karl, M.; Kukkonen, J.; Keuken, M.P.; Lützenkirchen, S.; Pirjola, L.; Hussein, T.

2016-01-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the

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

Directory of Open Access Journals (Sweden)

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.

Respiratory symptoms among industrial workers exposed to water aerosol. A pilot study of process water and air microbial quality

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Bożena Krogulska

2013-02-01

Full Text Available Background: The frequency of respiratory symptoms in workers exposed to water aerosol was evaluated along with the preliminary assessment of microbiological contamination of air and water used in glass processing plants. Material and Methods: A questionnaire survey was conducted in 131 workers from 9 glass processing plants. Questions focused on working conditions, respiratory symptoms and smoking habits. A pilot study of air and water microbiological contamination in one glass processing plant was performed. Water samples were tested for Legionella in accordance with EN ISO 11731-2:2008 and for total colony count according to PN-EN ISO 6222:2004. Air samples were tested for total numbers of molds and mildews. Results: During the year preceding the survey acute respiratory symptoms occurred in 28.2% of participants, while chronic symptoms were reported by 29% of respondents. Increased risks of cough and acute symptoms suggestive of pneumonia were found among the respondents working at a distance up to 20 m from the source of water aerosol compared to other workers (OR = 2.7, with no difference in the frequency of other symptoms. A microbiological analysis of water samples from selected glass plant revealed the presence of L. pneumophila, exceeding 1000 cfu/100 ml. The number of bacteria and fungi detected in air samples (above 1000 cfu/m3 suggested that water aerosol at workplaces can be one of the sources of the air microbial contamination. Conclusions: The questionnaire survey revealed an increased risk of cough and acute symptoms suggestive of pneumonia in the group working at a shortest distance form the source of water aerosol. Med Pr 2013;64(1:47–55

Ultra-processed products are becoming dominant in the global food system.

Science.gov (United States)

Monteiro, C A; Moubarac, J-C; Cannon, G; Ng, S W; Popkin, B

2013-11-01

The relationship between the global food system and the worldwide rapid increase of obesity and related diseases is not yet well understood. A reason is that the full impact of industrialized food processing on dietary patterns, including the environments of eating and drinking, remains overlooked and underestimated. Many forms of food processing are beneficial. But what is identified and defined here as ultra-processing, a type of process that has become increasingly dominant, at first in high-income countries, and now in middle-income countries, creates attractive, hyper-palatable, cheap, ready-to-consume food products that are characteristically energy-dense, fatty, sugary or salty and generally obesogenic. In this study, the scale of change in purchase and sales of ultra-processed products is examined and the context and implications are discussed. Data come from 79 high- and middle-income countries, with special attention to Canada and Brazil. Results show that ultra-processed products dominate the food supplies of high-income countries, and that their consumption is now rapidly increasing in middle-income countries. It is proposed here that the main driving force now shaping the global food system is transnational food manufacturing, retailing and fast food service corporations whose businesses are based on very profitable, heavily promoted ultra-processed products, many in snack form. © 2013 The Authors. Obesity Reviews published by John Wiley & Sons Ltd on behalf of the International Association for the Study of Obesity.

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 ...

Organic aerosols

International Nuclear Information System (INIS)

Penner, J.E.

1994-01-01

Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN

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

Science.gov (United States)

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

2018-04-01

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

Wood combustion, a dominant source of winter aerosol in residential district in proximity to a large automobile factory in Central Europe

Czech Academy of Sciences Publication Activity Database

Hovorka, J.; Pokorná, P.; Hopke, P. K.; Křůmal, Kamil; Mikuška, Pavel; Píšová, M.

2015-01-01

Roč. 113, JUL (2015), s. 98-107 ISSN 1352-2310 R&D Projects: GA ČR(CZ) GBP503/12/G147 Institutional support: RVO:68081715 Keywords : coarse aerosol * fine aerosol * positive matrix factorization Subject RIV: DI - Air Pollution ; Quality Impact factor: 3.459, year: 2015

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

Energy Technology Data Exchange (ETDEWEB)

Jordan, S; Schikarski, W; Schoeck, W [Gesellschaft fuer Kernforschung mbH, Karlsruhe (Germany)

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters.

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

International Nuclear Information System (INIS)

Jordan, S.; Schikarski, W.; Schoeck, W.

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters

Dry season aerosol iron solubility in tropical northern Australia

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V. H. L. Winton

2016-10-01

Full Text Available Marine nitrogen fixation is co-limited by the supply of iron (Fe and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m−3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12 % in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.

Indium oxide deposition on glass by aerosol pyrolysis (Pyrosol (R) process)

International Nuclear Information System (INIS)

Blandenet, G.; Lagarde, Y.; Spitz, J.

1975-01-01

The pyrosol (R) process involves the pyrolysis of an aerosol generated by ultrasonic nebulisation from a solution of organic or inorganic compounds. This technique was used to deposit transparent n-conducting indium oxide films on glass. The electrical and optical properties of these films were studied as a function of the deposition temperature and doping (using tin or fluorine). A deposition temperature of 480 deg C and a Sn/In ratio of about 5% gave the best results. In this case, the transmission in the visible range was 92%, the infrared reflection 84% and the electrical resistivity 1.7x10 -4 ohm.cm [fr

Evidence for a significant proportion of Secondary Organic Aerosol from isoprene above a maritime tropical forest

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N. H. Robinson

2011-02-01

Full Text Available Isoprene is the most abundant non-methane biogenic volatile organic compound (BVOC, but the processes governing secondary organic aerosol (SOA formation from isoprene oxidation are only beginning to become understood and selective quantification of the atmospheric particulate burden remains difficult. Organic aerosol above a tropical rainforest located in Danum Valley, Borneo, Malaysia, a high isoprene emission region, was studied during Summer 2008 using Aerosol Mass Spectrometry and offline detailed characterisation using comprehensive two dimensional gas chromatography. Observations indicate that a substantial fraction (up to 15% by mass of atmospheric sub-micron organic aerosol was observed as methylfuran (MF after thermal desorption. This observation was associated with the simultaneous measurements of established gas-phase isoprene oxidation products methylvinylketone (MVK and methacrolein (MACR. Observations of MF were also made during experimental chamber oxidation of isoprene. Positive matrix factorisation of the AMS organic mass spectral time series produced a robust factor which accounts for an average of 23% (0.18 μg m⁻³, reaching as much as 53% (0.50 μg m⁻³ of the total oraganic loading, identified by (and highly correlated with a strong MF signal. Assuming that this factor is generally representative of isoprene SOA, isoprene derived aerosol plays a significant role in the region. Comparisons with measurements from other studies suggest this type of isoprene SOA plays a role in other isoprene dominated environments, albeit with varying significance.

Cloud processing of gases and aerosols in the Community Multiscale Air Quality (CMAQ) model: Impacts of extended chemistry

Science.gov (United States)

Clouds and fogs can significantly impact the concentration and distribution of atmospheric gases and aerosols through chemistry, scavenging, and transport. This presentation summarizes the representation of cloud processes in the Community Multiscale Air Quality (CMAQ) modeling ...

Potential of secondary aerosol formation from Chinese gasoline engine exhaust.

Science.gov (United States)

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

2018-04-01

Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds (VOCs). However, little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4-5hr simulation, which was estimated to represent more than 10days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol (SOA) production was 426±85mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China. Copyright © 2017. Published by Elsevier B.V.

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.

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

Science.gov (United States)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

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.

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.

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

Impact of Aerosols on Convective Clouds and Precipitation

Science.gov (United States)

Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong; Li, Xiaowen

2012-01-01

Aerosols are a critical.factor in the atmospheric hydrological cycle and radiation budget. As a major agent for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosols have a major impact on the dynamics, microphysics, and electrification properties of continental mixed-phase convective clouds. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing a significant source of cloud condensation nuclei (CCN). Such pollution . effects on precipitation potentially have enormous climatic consequences both in terms of feedbacks involving the land surface via rainfall as well as the surface energy budget and changes in latent heat input to the atmosphere. Basically, aerosol concentrations can influence cloud droplet size distributions, the warm-rain process, the cold-rain process, cloud-top heights, the depth of the mixed-phase region, and the occurrence of lightning. Recently, many cloud resolution models (CRMs) have been used to examine the role of aerosols on mixed-phase convective clouds. These modeling studies have many differences in terms of model configuration (two- or three-dimensional), domain size, grid spacing (150-3000 m), microphysics (two-moment bulk, simple or sophisticated spectral-bin), turbulence (1st or 1.5 order turbulent kinetic energy (TKE)), radiation, lateral boundary conditions (i.e., closed, radiative open or cyclic), cases (isolated convection, tropical or midlatitude squall lines) and model integration time (e.g., 2.5 to 48 hours). Among these modeling studies, the most striking difference is that cumulative precipitation can either increase or decrease in response to higher concentrations of CCN. In this presentation, we review past efforts and summarize our current understanding of the effect of aerosols on convective precipitation processes. Specifically, this paper addresses the following topics

Calibration of aerosol radiometers. Special aerosol sources

International Nuclear Information System (INIS)

Belkina, S.K.; Zalmanzon, Yu.E.; Kuznetsov, Yu.V.; Fertman, D.E.

1988-01-01

Problems of calibration of artificial aerosol radiometry and information-measurement systems of radiometer radiation control, in particular, are considered. Special aerosol source is suggested, which permits to perform certification and testing of aerosol channels of the systems in situ without the dismantling

General solution of the aerosol dynamic equation: growth and diffusion processes

International Nuclear Information System (INIS)

Elgarayhi, A.; Elhanbaly, A.

2004-01-01

The dispersion of aerosol particles in a fluid media is studied considering the main mechanism for condensation and diffusion. This has been done when the technique of Lie is used for solving the aerosol dynamic equation. This method is very useful in sense that it reduces the partial differential equation to some ordinary differential equations. So, different classes of similarity solutions have been obtained. The quantity of well-defined physical interest is the mean particle volume has been calculated

Aerosol optical properties over the Svalbard region of Arctic: ground-based measurements and satellite remote sensing

Science.gov (United States)

Gogoi, Mukunda M.; Babu, S. Suresh

2016-05-01

In view of the increasing anthropogenic presence and influence of aerosols in the northern polar regions, long-term continuous measurements of aerosol optical parameters have been investigated over the Svalbard region of Norwegian Arctic (Ny-Ålesund, 79°N, 12°E, 8 m ASL). This study has shown a consistent enhancement in the aerosol scattering and absorption coefficients during spring. The relative dominance of absorbing aerosols is more near the surface (lower single scattering albedo), compared to that at the higher altitude. This is indicative of the presence of local anthropogenic activities. In addition, long-range transported biomass burning aerosols (inferred from the spectral variation of absorption coefficient) also contribute significantly to the higher aerosol absorption in the Arctic spring. Aerosol optical depth (AOD) estimates from ground based Microtop sun-photometer measurements reveals that the columnar abundance of aerosols reaches the peak during spring season. Comparison of AODs between ground based and satellite remote sensing indicates that deep blue algorithm of Moderate Resolution Imaging Spectroradiometer (MODIS) retrievals over Arctic snow surfaces overestimate the columnar AOD.

Ground-Based Remote Sensing of Aerosol Properties over a Coastal Megacity of Pakistan

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Salman Tariq

2018-01-01

Full Text Available Atmospheric aerosols are considered to be an important constituent of Earth’s atmosphere because of their climatic, environmental, and health effects. Therefore, while studying the global climate change, investigation of aerosol concentrations and properties is essential both at local and regional levels. In this paper, we have used relatively long-term Aerosol Robotic Network (AERONET data during September 2006–August 2014 to analyze aerosol properties such as aerosol optical depth at 500 nm (AOD, Ångström exponent (440–870 nm (AE, refractive index (RI, and asymmetry parameter over Karachi, a coastal megacity of Pakistan. The average annual values of AOD and AE were found to be 0.48 ± 0.20 and 0.59 ± 0.29, respectively. The peak (0.88 ± 0.31 AOD was recorded in July with corresponding AE of 0.30 ± 0.22 representing reasonably higher concentration of coarse size particles over Karachi. The cluster analysis using the scatter plot between absorption AE and extinction AE revealed that desert dust prevailed in the atmosphere of Karachi in spring and summer, while biomass burning aerosols dominate in autumn and winter. The peak values of volume concentrations of coarse and fine-mode particulate matter were found in summer and autumn, respectively. Also, we found significant growing trend in single-scattering albedo with wavelength, indicating the domination of dust particles during summer and spring. The peak value of the real part of the RI was observed in spring (1.53 and modest in winter (1.50. On the contrary, the peak value of the imaginary part of the RI was observed to be constantly elevated in winter and lesser in spring.

Satellite and ground-based remote sensing of aerosols during intense haze event of October 2013 over lahore, Pakistan

Science.gov (United States)

Tariq, Salman; Zia, ul-Haq; Ali, Muhammad

2016-02-01

Due to increase in population and economic development, the mega-cities are facing increased haze events which are causing important effects on the regional environment and climate. In order to understand these effects, we require an in-depth knowledge of optical and physical properties of aerosols in intense haze conditions. In this paper an effort has been made to analyze the microphysical and optical properties of aerosols during intense haze event over mega-city of Lahore by using remote sensing data obtained from satellites (Terra/Aqua Moderate-resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO)) and ground based instrument (AErosol RObotic NETwork (AERONET)) during 6-14 October 2013. The instantaneous highest value of Aerosol Optical Depth (AOD) is observed to be 3.70 on 9 October 2013 followed by 3.12 on 8 October 2013. The primary cause of such high values is large scale crop residue burning and urban-industrial emissions in the study region. AERONET observations show daily mean AOD of 2.36 which is eight times higher than the observed values on normal day. The observed fine mode volume concentration is more than 1.5 times greater than the coarse mode volume concentration on the high aerosol burden day. We also find high values (~0.95) of Single Scattering Albedo (SSA) on 9 October 2013. Scatter-plot between AOD (500 nm) and Angstrom exponent (440-870 nm) reveals that biomass burning/urban-industrial aerosols are the dominant aerosol type on the heavy aerosol loading day over Lahore. MODIS fire activity image suggests that the areas in the southeast of Lahore across the border with India are dominated by biomass burning activities. A Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model backward trajectory showed that the winds at 1000 m above the ground are responsible for transport from southeast region of biomass burning to Lahore. CALIPSO derived sub-types of

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

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H.-H. Lee

2016-07-01

Full Text Available The source-oriented Weather Research and Forecasting chemistry model (SOWC was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol–radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3–5 W m−2 and surface temperature by as much as 0.25 K in the daytime.

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

Science.gov (United States)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

Chemically-resolved aerosol volatility measurements from two megacity field studies

Directory of Open Access Journals (Sweden)

J. A. Huffman

2009-09-01

Full Text Available The volatilities of different chemical species in ambient aerosols are important but remain poorly characterized. The coupling of a recently developed rapid temperature-stepping thermodenuder (TD, operated in the range 54–230°C with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS during field studies in two polluted megacities has enabled the first direct characterization of chemically-resolved urban particle volatility. Measurements in Riverside, CA and Mexico City are generally consistent and show ambient nitrate as having the highest volatility of any AMS standard aerosol species while sulfate showed the lowest volatility. Total organic aerosol (OA showed volatility intermediate between nitrate and sulfate, with an evaporation rate of 0.6%·K⁻¹ near ambient temperature, although OA dominates the residual species at the highest temperatures. Different types of OA were characterized with marker ions, diurnal cycles, and positive matrix factorization (PMF and show significant differences in volatility. Reduced hydrocarbon-like OA (HOA, a surrogate for primary OA, POA, oxygenated OA (OOA, a surrogate for secondary OA, SOA, and biomass-burning OA (BBOA separated with PMF were all determined to be semi-volatile. The most aged OOA-1 and its dominant ion, CO₂⁺, consistently exhibited the lowest volatility, with HOA, BBOA, and associated ions for each among the highest. The similar or higher volatility of HOA/POA compared to OOA/SOA contradicts the current representations of OA volatility in most atmospheric models and has important implications for aerosol growth and lifetime. A new technique using the AMS background signal was demonstrated to quantify the fraction of species up to four orders-of-magnitude less volatile than those detectable in the MS mode, which for OA represent ~5% of the non-refractory (NR OA signal. Our results strongly imply that all OA types should be considered

A 20-year simulated climatology of global dust aerosol deposition.

Science.gov (United States)

Zheng, Yu; Zhao, Tianliang; Che, Huizheng; Liu, Yu; Han, Yongxiang; Liu, Chong; Xiong, Jie; Liu, Jianhui; Zhou, Yike

2016-07-01

Based on a 20-year (1991-2010) simulation of dust aerosol deposition with the global climate model CAM5.1 (Community Atmosphere Model, version 5.1), the spatial and temporal variations of dust aerosol deposition were analyzed using climate statistical methods. The results indicated that the annual amount of global dust aerosol deposition was approximately 1161±31Mt, with a decreasing trend, and its interannual variation range of 2.70% over 1991-2010. The 20-year average ratio of global dust dry to wet depositions was 1.12, with interannual variation of 2.24%, showing the quantity of dry deposition of dust aerosol was greater than dust wet deposition. High dry deposition was centered over continental deserts and surrounding regions, while wet deposition was a dominant deposition process over the North Atlantic, North Pacific and northern Indian Ocean. Furthermore, both dry and wet deposition presented a zonal distribution. To examine the regional changes of dust aerosol deposition on land and sea areas, we chose the North Atlantic, Eurasia, northern Indian Ocean, North Pacific and Australia to analyze the interannual and seasonal variations of dust deposition and dry-to-wet deposition ratio. The deposition amounts of each region showed interannual fluctuations with the largest variation range at around 26.96% in the northern Indian Ocean area, followed by the North Pacific (16.47%), Australia (9.76%), North Atlantic (9.43%) and Eurasia (6.03%). The northern Indian Ocean also had the greatest amplitude of interannual variation in dry-to-wet deposition ratio, at 22.41%, followed by the North Atlantic (9.69%), Australia (6.82%), North Pacific (6.31%) and Eurasia (4.36%). Dust aerosol presented a seasonal cycle, with typically strong deposition in spring and summer and weak deposition in autumn and winter. The dust deposition over the northern Indian Ocean exhibited the greatest seasonal change range at about 118.00%, while the North Atlantic showed the lowest seasonal

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

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K. Zhang

2012-10-01

Full Text Available This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation.

Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in-cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7 between accumulation mode and coarse mode emission fluxes of

Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

Science.gov (United States)

Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-07-01

operational remote-sensing algorithms.Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (M{O/Y}D04). The M{O/Y}D04 product is of course normally produced from M{O/Y}D021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a M{O/Y}D021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source.We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

Science.gov (United States)

Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-01-01

operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity

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G. W. Mann

2014-05-01

Full Text Available Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree

Characterization and source apportionment of organic aerosol at 260 m on a meteorological tower in Beijing, China

Science.gov (United States)

Zhou, Wei; Wang, Qingqing; Zhao, Xiujuan; Xu, Weiqi; Chen, Chen; Du, Wei; Zhao, Jian; Canonaco, Francesco; Prévôt, André S. H.; Fu, Pingqing; Wang, Zifa; Worsnop, Douglas R.; Sun, Yele

2018-03-01

Despite extensive efforts toward the characterization of submicron aerosols at ground level in the megacity of Beijing, our understanding of aerosol sources and processes at high altitudes remains low. Here we conducted a 3-month real-time measurement of non-refractory submicron aerosol (NR-PM1) species at a height of 260 m from 10 October 2014 to 18 January 2015 using an aerosol chemical speciation monitor. Our results showed a significant change in aerosol composition from the non-heating period (NHP) to the heating period (HP). Organics and chloride showed clear increases during HP due to coal combustion emissions, while nitrate showed substantial decreases from 28 to 15-18 %. We also found that NR-PM1 species in the heating season can have average mass differences of 30-44 % under similar emission sources yet different meteorological conditions. Multi-linear engine 2 (ME-2) using three primary organic aerosol (OA) factors as constraints, i.e., fossil-fuel-related OA (FFOA) dominantly from coal combustion emissions, cooking OA (COA), and biomass burning OA (BBOA) resolved from ground high-resolution aerosol mass spectrometer measurements, was applied to OA mass spectra of ACSM. Two types of secondary OA (SOA) that were well correlated with nitrate and chloride-CO, respectively, were identified. SOA played a dominant role in OA during all periods at 260 m although the contributions were decreased from 72 % during NHP to 58-64 % during HP. The SOA composition also changed significantly from NHP to HP. While the contribution of oxygenated OA (OOA) was decreased from 56-63 to 32-40 %, less oxidized OOA (LO-OOA) showed a large increase from 9-16 to 24-26 %. COA contributed a considerable fraction of OA at high altitude, and the contribution was relatively similar across different periods (10-13 %). In contrast, FFOA showed a large increase during HP due to the influences of coal combustion emissions. We also observed very different OA composition between ground level

The background aerosol in the lower stratosphere and the tropospheric aerosol in the Alps. Final report; Das Hintergrundaerosol der unteren Stratosphaere und das troposphaerische Aerosol der Alpen. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Jaeger, H.; Trickl, T.

2001-06-04

As a contribution to the German Aerosol-Lidar Network lidar backscatter measurements have been carried out at Garmisch-Partenkirchen in a wide range of the atmosphere from next to the ground to altitudes beyond 30 km. The investigations, on one hand, were devoted to establishing a climatology of the aerosol extinction coefficient for the northern Alps and to prolonging the long-term measurement series of the stratospheric aerosol. On the other hand, aerosol was used as a tracer of polluted air masses in atmospheric transport studies (orographically induced vertical transport, advection of Saharan dust, as well as aerosol advection from the North american boundary layer and from large-scale wild fire in the United States and Canada). These transport processes given the seasonal cycle of the aerosol throughout the troposphere. In the free troposphere a pronounced spring-time aerosol maximum was found. The stratospheric aerosol concentration had decayed to a background-type level during the reporting period. As a consequence, the influence of smaller aerosol contributions could be distinguished such as the eruption of the volcano Shishaldin (Alaska) and aircraft emissions. (orig.) [German] Im Rahmen des deutschen Aerosollidarnetzes wurden in Garmisch-Partenkirchen Lidar-Rueckstreumessungen in einem weiten Bereich der Atmosphaere von Bodennaehe bis in ueber 30 km Hoehe durchgefuehrt. Die Arbeiten dienten zum einen der Erstellung einer Klimatologie des Aerosol-Extinktionskoeffizienten fuer die Nordalpen sowie der Verlaengerung der seit 1976 erstellten Langzeitmessreihe des stratosphaerischen Aerosols. Zum anderen fanden atmosphaerische Transportstudien statt, bei denen das Aerosol als 'Tracer' fuer Luftverschmutzung verwendet wurde (orographisch induzierter Vertikaltransport, Advektion von Saharastaub und Aerosoladvektion aus der nordamerikanischen Genzschicht und von grossflaechigen Waldbraenden in den U.S.A. und Kanada). Diese Transportprozesse bestimmen den

A study of the attachment of thoron decay products to aerosols using an aerosol centrifuge

International Nuclear Information System (INIS)

Balakrishnan, V.

1979-01-01

The physical attachment of radioactive decay products (particulate, not gas) to polydisperse fluorescein aerosal particles in two size ranges 0.1 μM-0.33 μM radius and 0.25 μM-1.35 μM radius has been studied under dynamic conditions with a view to find the fraction of thoron decay products attached to the aerosals and the particle size distribution of the host aerosols in the atmosphere of uranium mines. The experimental set-up and procedure are described. An aerosol cloud of fluorescein was introduced into a reaction chamber containing a steady source of thoron and decay products were allowed to interact and attach to the aerosols in the chamber. To simulate conditions normally encountered in uranium mining and milling operations, the concentration of aerosol particles was kept high as compared to the number of decay products. The Lovelace Aerosol Particle Separator, which is an advanced, continuous centrifugal aerosol separator, was used to sample and separate the tagged aerosols into various size groups. The radioactivity associated with each group was determined. The results show the same dependence of attachment of decay products on the size of aerosol particles as predicted by the diffusion theory proposed by Lassen and Rau (1960), even though the experimental conditions of the present study do not conform to those required to satisfy the above mentioned diffusion theory. The method employed in this work to study attachment is reproducible and simple and can be adopted in uranium and thorium mines and associated processing industries. (M.G.B.)

Formation and dynamic change of aerosol particles

International Nuclear Information System (INIS)

Kasahara, Mikio

1986-01-01

Processes of aerosol particle nucleation are roughly grouped into two types. In one, aerosol is produced as a result of dispersion of solid or liquid by mechanical force while in the other it is formed through phase transition from gas to solid or liquid due to cohesion caused by cooling, expansion or chemical reaction. This article reviews various aspects of aerosol particle nucleation through the latter type of processes and behaviors of the particles formed. Gas-to-particle conversion processes are divided into those of homogeneous and heterogeneous nucleation, and the former include homogeneous homomolecular and homogeneous heteromolecular nucleation processes. Here, homoneneous homomolecular nucleation is described centering on the theories proposed by Backer and Doring-Zeldovich-Volmer-Frenkel while homogeneous heteromolecular systems are outlined citing the theory developed by Kiang and Stauffer. Heterogeneous nucleation (or heterogeneous condensation) is discussed on the basis of the relationship between the mean free path of air molecules and the particle size. Various theories for particle formation and growth are listed and briefly outlined. Some of them are compared with experimental results. Models are cited to explain behaviors of aerosol particles after being formed. Also described is simulation of particle nucleation and growth in relation to atmospheric pollution and possible accidents of liquid-metal fast breeder reactors. (Nogami, K.)

Perceptions of Secondhand E-Cigarette Aerosol Among Twitter Users.

Science.gov (United States)

Unger, Jennifer B; Escobedo, Patricia; Allem, Jon-Patrick; Soto, Daniel W; Chu, Kar-Hai; Cruz, Tess

2016-04-01

There is considerable debate among the public health community about the health risks of secondhand exposure to the aerosol from electronic cigarettes (e-cigarettes). Despite mounting scientific evidence on the chemical content of e-cigarette aerosol, public perceptions of the relative safety of secondhand e-cigarette aerosol have not been well characterized. This study collected tweets, or messages sent using Twitter, about exposure to secondhand e-cigarette aerosol over a 6-week period in 2015. Tweets were coded on sentiment about e-cigarettes (pro-, anti-, or neutral/unknown) and topic (health, social, advertisement, or unknown). The 1519 tweets included 531 pro-e-cigarette tweets, 392 anti-e-cigarette tweets, and 596 neutral tweets. Social tweets far outnumbered health tweets (747 vs. 182, respectively). Social-focused tweets were predominantly pro-e-cigarette, whereas health-focused tweets were predominantly anti-e-cigarette. Twitter discussions about secondhand vaping are dominated by pro-e-cigarette social tweets, although there is a presence of anti-e-cigarette social tweets and tweets about negative and positive health effects. Public health and regulatory agencies could use social media and traditional media to disseminate the message that e-cigarette aerosol contains potentially harmful chemicals and could be perceived as offensive. This study identifies the prevalent topics and opinions that could be incorporated into health education messages.

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

Science.gov (United States)

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

2018-01-01

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

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

How thermodynamic environments control stratocumulus microphysics and interactions with aerosols

International Nuclear Information System (INIS)

Andersen, Hendrik; Cermak, Jan

2015-01-01

Aerosol–cloud interactions are central to climate system changes and depend on meteorological conditions. This study identifies distinct thermodynamic regimes and proposes a conceptual framework for interpreting aerosol effects. In the analysis, ten years (2003–2012) of daily satellite-derived aerosol and cloud products are combined with reanalysis data to identify factors controlling Southeast Atlantic stratocumulus microphysics. Considering the seasonal influence of aerosol input from biomass burning, thermodynamic environments that feature contrasting microphysical cloud properties and aerosol–cloud relations are classified. While aerosol impact is stronger in unstable environments, it is mostly confined to situations with low aerosol loading (aerosol index AI ≲ 0.15), implying a saturation of aerosol effects. Situations with high aerosol loading are associated with weaker, seasonally contrasting aerosol-droplet size relationships, likely caused by thermodynamically induced processes and aerosol swelling. (letter)

Field and Laboratory Studies of Atmospheric Organic Aerosol

Science.gov (United States)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed

Exposure to parvalbumin allergen and aerosols among herring processing workers.

Science.gov (United States)

Dahlman-Höglund, Anna; Renström, Anne; Acevedo, Fernando; Andersson, Eva

2013-10-01

There are increasing reports of allergies and respiratory symptoms among workers in the fish processing industry, coinciding with an increasing use of high-pressure water in the processing plants. However, few studies have measured exposure in these work environments. The aim of this study was to characterize the occupational exposure of workers to herring antigen and to screen environmental factors at a herring (Clupea harengus) plant in which new and more encapsulated filleting machines had been installed. To assist in this, a method to assess airborne exposure to herring allergen was needed. Exposure to airborne herring antigen, mould spores, and endotoxin were measured during work. Antigen exposure was assessed using a newly developed sensitive (detection limit, 0.1 ng ml(-1)) rabbit polyclonal sandwich enzyme-linked immunosorbent assay against the major herring muscle protein allergen, parvalbumin. Aerosols were measured by mass concentration (DataRAM) and number of particles (Climet I-500). Personal geometric mean herring allergen exposure was 986 ng m(-3) at the old filleting workstations and 725 ng m(-3) at the new workstations (difference not significant). Outside the production room, the level was ~130 ng m(-3). Number of particles and mass concentration were both significantly lower around the new machines than around the old machines (P < 0.001 and P < 0.0001, respectively). The highest particle count was seen for the 0.3-0.5 μm fraction, with more than 400,000 particles per cubic metre air. Endotoxin concentration in the air varied between 3 and 92 EU m(-3), with the highest levels when the catch mainly contained herring that had eaten krill or seaweed. We developed a sensitive method to detect herring antigen. High exposure to herring antigen was measured during filleting work. The particles in the air around the fillet machines were mainly <0.5 μm and the newer encapsulated machines generated fewer particles. It is important to reduce occupational

Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing

Directory of Open Access Journals (Sweden)

J. E. Penner

2009-02-01

Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm⁻² while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm⁻² and −0.16 to −0.12 Wm⁻², respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

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

Science.gov (United States)

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

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

Delay in convection in nocturnal boundary layer due to aerosol-induced cooling

Science.gov (United States)

Singh, Dhiraj Kumar; Ponnulakshmi, V. K.; Subramanian, G.; Sreenivas, K. R.

2012-11-01

Heat transfer processes in the nocturnal boundary layer (NBL) influence the surface energy budget, and play an important role in many micro-meteorological processes including the formation of inversion layers, radiation fog, and in the control of air-quality near the ground. Under calm clear-sky conditions, radiation dominates over other transport processes, and as a result, the air layers just above ground cool the fastest after sunset. This leads to an anomalous post-sunset temperature profile characterized by a minimum a few decimeters above ground (Lifted temperature minimum). We have designed a laboratory experimental setup to simulate LTM, involving an enclosed layer of ambient air, and wherein the boundary condition for radiation is decoupled from those for conduction and convection. The results from experiments involving both ambient and filtered air indicate that the high cooling rates observed are due to the presence of aerosols. Calculated Rayleigh number of LTM-type profiles is of the order 105-107 in the field and of order 103-105 in the laboratory. In the LTM region, there is convective motion when the Rayleigh number is greater than 104 rather than the critical Rayleigh number (Rac = 1709). The diameter of convection rolls is a function of height of minimum of LTM-type profiles. The results obtained should help in the parameterization of transport process in the nocturnal boundary layer, and highlight the need to accounting the effects of aerosols and ground emissivity in climate models.