Science.gov

Sample records for aerosol source term

  1. Evaluation of source-term data for plutonium aerosolization

    SciTech Connect

    Haschke, J.M.

    1992-07-01

    Relevant data are reviewed and evaluated in an effort to define the time dependence and maximum value of the source term for plutonium aerosolization during a fuel fire. The rate of plutonium oxidation at high temperatures is a major determinant of the time dependence. Analysis of temperature-time data for oxidation of plutonium shows that the rate is constant (0.2 g PUO{sub 2}/cm{sup 2} of metal surface per min) and independent of temperature above 500{degrees}C. Total mass and particle distributions are derived for oxide products formed by reactions of plutonium metal and hydride. The mass distributions for products of all metal-gas reactions are remarkably similar with approximately 0.07 mass% of the oxide particles having geometric diameters {le} 10 {mu}m. In comparison, 25 mass% of the oxide formed by the PuH{sub 2}+O{sub 2} reaction is in this range. Experimental values of mass fractions released during oxidation are evaluated and factors that alter the release fraction are discussed.

  2. LMFBR source term experiments in the Fuel Aerosol Simulant Test (FAST) facility

    SciTech Connect

    Petrykowski, J.C.; Longest, A.W.

    1985-01-01

    The transport of uranium dioxide (UO/sub 2/) aerosol through liquid sodium was studied in a series of ten experiments in the Fuel Aerosol Simulant Test (FAST) facility at Oak Ridge National Laboratory (ORNL). The experiments were designed to provide a mechanistic basis for evaluating the radiological source term associated with a postulated, energetic core disruptive accident (CDA) in a liquid metal fast breeder reactor (LMFBR). Aerosol was generated by capacitor discharge vaporization of UO/sub 2/ pellets which were submerged in a sodium pool under an argon cover gas. Measurements of the pool and cover gas pressures were used to study the transport of aerosol contained by vapor bubbles within the pool. Samples of cover gas were filtered to determine the quantity of aerosol released from the pool. The depth at which the aerosol was generated was found to be the most critical parameter affecting release. The largest release was observed in the baseline experiment where the sample was vaporized above the sodium pool. In the nine ''undersodium'' experiments aerosol was generated beneath the surface of the pool at depths varying from 30 to 1060 mm. The mass of aerosol released from the pool was found to be a very small fraction of the original specimen. It appears that the bulk of aerosol was contained by bubbles which collapsed within the pool. 18 refs., 11 figs., 4 tabs.

  3. Source term experiments project (STEP): aerosol characterization system

    SciTech Connect

    Schlenger, B.J.; Dunn, P.F.

    1985-01-01

    A series of four experiments is being conducted at Argonne National Laboratory's TREAT Reactor. They have been designed to provide some of the necessary data regarding magnitude and release rates of fission products from degraded fuel pins, physical and chemical characteristics of released fission products, and aerosol formation and transport phenomena. These are in-pile experiments, whereby the test fuel is heated by neutron induced fission and subsequent clad oxidation in steam environments that simulate as closely as practical predicted reactor accident conditions. The test sequences cover a range of pressure and fuel heatup rate, and include the effect of Ag/In/Cd control rod material.

  4. Environmental radiation safety: source term modification by soil aerosols. Interim report

    SciTech Connect

    Moss, O.R.; Allen, M.D.; Rossignol, E.J.; Cannon, W.C.

    1980-08-01

    The goal of this project is to provide information useful in estimating hazards related to the use of a pure refractory oxide of /sup 238/Pu as a power source in some of the space vehicles to be launched during the next few years. Although the sources are designed and built to withstand re-entry into the earth's atmosphere, and to impact with the earth's surface without releasing any plutonium, the possibility that such an event might produce aerosols composed of soil and /sup 238/PuO/sub 2/ cannot be absolutely excluded. This report presents the results of our most recent efforts to measure the degree to which the plutonium aerosol source term might be modified in a terrestrial environment. The five experiments described represent our best effort to use the original experimental design to study the change in the size distribution and concentration of a /sup 238/PuO/sub 2/ aerosol due to coagulation with an aerosol of clay or sandy loam soil.

  5. Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

    PubMed

    Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

    2015-09-15

    To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013. PMID:25958364

  6. A long term source apportionment study of wood burning and traffic aerosols for three measurement sites in Switzerland

    NASA Astrophysics Data System (ADS)

    Herich, Hanna; Hüglin, Christoph; Buchmann, Brigitte

    2010-05-01

    Besides their effects on radiative forcing soot aerosols have been found to cause health effects as they are carcinogenic. Diesel engines and incomplete biomass burning are the major emission sources of soot particles. Especially during winter, the wood burning (WB) emissions from residential heating have been found to contribute significantly to the total carbonaceous material (CM). To investigate the contribution of fossil fuel (FF) and WB emissions seven-wavelength aethalometers have been deployed in previous studies (Sandradewi et al. 2008, Favez et al. 2009). In these studies, the stronger light absorption of WB aerosols in the blue and ultraviolet compared to the light absorption of aerosols from FF combustion was used. Linear regression modelling of CM against the light absorption coefficient of FF combustion aerosols in the infrared (950 nm) and the light absorption coefficient of WB aerosols in the blue (470 nm) was proposed for source apportionment. In this study we present long term aethalometer measurements at two rural and one urban background measurement stations in Switzerland from 2008 - 2010. At these stations organic (OC) and elemental carbon (EC) were also measured by thermochemical analysis providing estimates for total CM. Above described linear regession modelling was applied for determination of the contribution of FF and WB emissions to total CM. Sensitivity tests for different regression models and for varying light absorption exponents were performed. It was found that the regression modelling approach is only limited suitable for long term datasets because of significant fractions of CM resulting from sources and processes other than FF and WB. Thus in a different approach we focused on black carbon (BC). The contribution of WB and FF to BC was directly determined from the absorption coefficients of FF and WB aerosols which were calculated with the use of absorption exponents taken from literature. First results show that in winter the

  7. Aerosol climatology at Delhi in the western Indo-Gangetic Plain: Microphysics, long-term trends, and source strengths

    NASA Astrophysics Data System (ADS)

    Lodhi, Neelesh K.; Beegum, S. Naseema; Singh, Sachchidanand; Kumar, Krishan

    2013-02-01

    present the climatology of aerosol microphysics, its trends, and impact of potential sources based on the long term measurements (for a period of 11.5 years from December 2001 to May 2012) of aerosol optical depths (AOD) in the spectral range 340-1020 nm from an urban center Delhi (28.6°N, 77.3°E, 238 m mean sea level) in the western Indo-Gangetic Plain (IGP). The study is the first ever long-term characterization of aerosols over the western IGP from the ground-based measurements. AODs are known to affect the air quality, visibility, radiative balance, and cloud microphysics of the region and IGP is one of the highest populated and polluted regions of the world. Our measurements show consistently high AOD during the entire period of observation. The seasonal variations of spectral AODs and Angstrom parameters are generally consistent every year. The AODs show a weak but statistically significant (in 95% confidence level) decreasing trend approximately -0.02/year at 500 nm, possibly, modulated by the pre-monsoon heavy dust loading during the first half of the observation period. The climatological monthly mean AOD at shorter wavelengths peaks twice, during June and November, while at longer wavelengths it shows only one peak in June. The annual variations of Angstrom exponent, α and its derivative, α' suggest the prevalence of multi-modal aerosol size distributions at Delhi. The coarse-mode aerosols dominate during summer (March-June) and monsoon (July-September) seasons, whereas fine/accumulation mode enhances during post-monsoon (October-November) and winter (December-February) seasons. Potential advection pathways have been identified using concentration weighted trajectory (CWT) analysis of the 5 day isentropic air mass back trajectories at the observation site and their seasonal variations are discussed.

  8. AERONET - Aerosol Climatology From Megalopolis Aerosol Source Regions

    NASA Astrophysics Data System (ADS)

    Holben, B. N.; Eck, T. F.; Dubovik, O.; Smirnov, A.; Slutsker, I.; Artaxo, P.; Leyva, A.; Lu, D.; Sano, I.; Singh, R. P.; Quel, E.; Tanre, D.; Zibordi, G.

    2002-05-01

    AERONET is a globally distributed network of ~170 identical sun and sky scanning spectral radiometers expanded by federation with collaborating investigators that contribute to the AERONET public domain data-base. We will detail the current distribution and plans for expanded collaboration. Recent products available through the project database are important for assessment of human health as well as climate forcing issues. We will illustrate a summary of aerosol optical properties measured in Indian, East Asian, North American, South American and European megalopolis source regions. We will present monthly mean fine and coarse particle aerosol optical depth, particle size distributions and single scattering albedos. Each region represents a population in excess of 10 million inhabitants within a 200 km radius of the observation site that dictate the anthropogenic aerosol sources contributing to significantly diverse aerosol properties as a function of economic development and seasonally dependent meteorological processes. The diversity of the measured optical properties of urban aerosols illustrates the need for long-term regional monitoring that contribute to comparative assessments for health and climate change investigations.

  9. Long-term real-time measurements of aerosol particle composition in Beijing, China: seasonal variations, meteorological effects, and source analysis

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Wang, Z. F.; Du, W.; Zhang, Q.; Wang, Q. Q.; Fu, P. Q.; Pan, X. L.; Li, J.; Jayne, J.; Worsnop, D. R.

    2015-09-01

    High concentrations of fine particles (PM2.5) are frequently observed during all seasons in Beijing, China, leading to severe air pollution and human health problems in this megacity. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) species (sulfate, nitrate, ammonium, chloride, and organics) in Beijing using an Aerodyne Aerosol Chemical Speciation Monitor for 1 year, from July 2011 to June 2012. This is the first long-term, highly time-resolved (~ 15 min) measurement of fine particle composition in China. The seasonal average (±1σ) mass concentration of NR-PM1 ranged from 52 (±49) μg m-3 in the spring season to 62 (±49) μg m-3 in the summer season, with organics being the major fraction (40-51 %), followed by nitrate (17-25 %) and sulfate (12-17 %). Organics and chloride showed pronounced seasonal variations, with much higher concentrations in winter than in the other seasons, due to enhanced coal combustion emissions. Although the seasonal variations of secondary inorganic aerosol (SIA, i.e., sulfate + nitrate + ammonium) concentrations were not significant, higher contributions of SIA were observed in summer (57-61 %) than in winter (43-46 %), indicating that secondary aerosol production is a more important process than primary emissions in summer. Organics presented pronounced diurnal cycles that were similar among all seasons, whereas the diurnal variations of nitrate were mainly due to the competition between photochemical production and gas-particle partitioning. Our data also indicate that high concentrations of NR-PM1 (> 60 μg m-3) are usually associated with high ambient relative humidity (RH) (> 50 %) and that severe particulate pollution is characterized by different aerosol composition in different seasons. All NR-PM1 species showed evident concentration gradients as a function of wind direction, generally with higher values associated with wind from the south, southeast or east. This was consistent

  10. Mechanistic facility safety and source term analysis

    SciTech Connect

    PLYS, M.G.

    1999-06-09

    A PC-based computer program was created for facility safety and source term analysis at Hanford The program has been successfully applied to mechanistic prediction of source terms from chemical reactions in underground storage tanks, hydrogen combustion in double contained receiver tanks, and proccss evaluation including the potential for runaway reactions in spent nuclear fuel processing. Model features include user-defined facility room, flow path geometry, and heat conductors, user-defined non-ideal vapor and aerosol species, pressure- and density-driven gas flows, aerosol transport and deposition, and structure to accommodate facility-specific source terms. Example applications are presented here.

  11. Long-term Observations of Carbonaceous Aerosols (including C isotope) at Alert: Inferring Emission Sources of Black Carbon Transported to the Arctic

    NASA Astrophysics Data System (ADS)

    Huang, Lin; Sharma, Sangeeta; Zhang, Wendy; Brook, Jeff; Leaitch, Richard; He, Kebin; Duan, Fengkui; Yang, Fumo

    2015-04-01

    Black carbon is a major component of carbonaceous aerosols and formed by incomplete combustion of fossil fuels and biomass burning (including biofuels and open fires). It plays unique roles in Earth's climate system through both direct and indirect effects. Identifying and attributing its emission sources, tracking source changes with time and relating them to radiative forcing are important for understanding the impacts of BC on climate at the global and regional levels, as well as necessary for the strategies targeted to reduce BC emission. However, there are many challenges and uncertainties regarding those aspects, particularly for BC aerosols transported to the Arctic region. To address the concerns of BC in the Arctic, carbonaceous aerosol observations, including elemental carbon (EC) content as BC mass, C isotopes as a source tracer, and light absorption coefficient as BC's optical property, have been conducted at Alert, a WMO GAW station (82° 27'N, 62° 31'W) since the early 2000s. In this presentation, nearly a decade of measurements will be presented, with a focus on the isotope results in EC (corresponding data from Beijing will also be shown for the purpose of comparison). Seasonal and inter-annual variations in δ13C (EC) have been characterized, inferring emission sources and suggesting source changes over last 5-6 years. Based on the C isotope results, the possible emission sources of BC contributed to the Arctic will be also discussed.

  12. Long-Term Observations on Aerosol Elemental Carbon and Mass Concentrations in Winter-Time in New Delhi: Implications for Local Source Changes

    NASA Astrophysics Data System (ADS)

    Aggarwal, S. G.; Singh, K.; Singh, N.; Gupta, P. K.

    2009-12-01

    Fossil-fuel and bio-fuel burning are the two major sources identified for high carbonaceous aerosol loadings in several mega cities in India. In the last decade, according to a report from the Central Pollution Control Board (CPCB, 1999), the vehicular emission (mostly diesel-powered engines) was contributed to ~67% of the total air pollution load in New Delhi. Therefore, a policy decision was taken by the government, and most of the diesel-powered engines were converted to compressed natural gas (CNG) -powered engines by 2003. To better understand the effect of these changes on air quality, we collected high volume aerosol samples (total suspended particles, TSP) mostly for a day basis at our institute building in New Delhi almost everyday during winter season (November to January) from 2002 to 2008. We found very high mean aerosol loading, i.e., 488±47 μg m-3 in 2002 winter, which dropped significantly to 280±73 μg m-3 in 2003 winter. Thereafter, a steadily increased trend of aerosol mass loadings was observed, i.e., 339±112, 339±120, 412±107 and 444±55 μg m-3 in 2004, 2005, 2006 and 2007 winters, respectively. Similar trend was also observed for elemental carbon (EC) concentration in TSP, which was peaked in 2002 (47±11 μg m-3) and minimized in 2003 (32±6 μg m-3), and then gradually increased to 41±8 μg m-3 in 2007 winter. These decline trends of aerosol mass and EC concentrations in 2003 can be explained well, because of the conversion of diesel engine to CNG engines of public transport facilities. However, again increase in aerosol mass and EC concentrations possibly because of a high increase in road traffic in recent years. According to the economic survey of New Delhi 2008-09, the number of vehicles (which includes all types of engines, i.e., petrol, diesel and CNG) has grown from ~3.3 millions in 1997-98 to ~5.6 millions in 2007-08. The influence of engine types and vehicle population on aerosol loading can also be explained well by SO2 and

  13. ISS Ambient Air Quality: Updated Inventory of Known Aerosol Sources

    NASA Technical Reports Server (NTRS)

    Meyer, Marit

    2014-01-01

    Spacecraft cabin air quality is of fundamental importance to crew health, with concerns encompassing both gaseous contaminants and particulate matter. Little opportunity exists for direct measurement of aerosol concentrations on the International Space Station (ISS), however, an aerosol source model was developed for the purpose of filtration and ventilation systems design. This model has successfully been applied, however, since the initial effort, an increase in the number of crewmembers from 3 to 6 and new processes on board the ISS necessitate an updated aerosol inventory to accurately reflect the current ambient aerosol conditions. Results from recent analyses of dust samples from ISS, combined with a literature review provide new predicted aerosol emission rates in terms of size-segregated mass and number concentration. Some new aerosol sources have been considered and added to the existing array of materials. The goal of this work is to provide updated filtration model inputs which can verify that the current ISS filtration system is adequate and filter lifetime targets are met. This inventory of aerosol sources is applicable to other spacecraft, and becomes more important as NASA considers future long term exploration missions, which will preclude the opportunity for resupply of filtration products.

  14. Novel measurement technologies for ambient and combustion source aerosols

    EPA Science Inventory

    Thie presentaiton examines the chemical properties of atmospheric and combustion source aerosols. It describes the aerosol chemical fractions and the specific chemical constituents in these aerosols. The presentation will cover (i) the limitatins and benefits of hyphenated chroma...

  15. An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

    NASA Technical Reports Server (NTRS)

    Giles, David M.; Holben, Brent N.; Eck, Thomas F.; Sinyuk, Aliaksandr; Smirnov, Alexander; Slutsker, Ilya; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

    2012-01-01

    Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 < delta omega (sub 0) <= 0.02 decrease) than in previous work and optical mixtures of pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

  16. Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela - sources, impacts and interannual variability

    NASA Astrophysics Data System (ADS)

    Hamburger, T.; Matisāns, M.; Tunved, P.; Ström, J.; Calderon, S.; Hoffmann, P.; Hochschild, G.; Gross, J.; Schmeissner, T.; Wiedensohler, A.; Krejci, R.

    2013-10-01

    First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm-3, refractory particle number concentrations (at 300 °C) 510±420 cm-3 and the absorption coefficient 0.91±1.2 Mm-1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm-3, 150±94 cm-3 and 0.15±0.26 Mm-1. A decrease of particle concentrations during the dry seasons from 2007-2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño-Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.

  17. Chernobyl source term estimation

    SciTech Connect

    Gudiksen, P.H.; Harvey, T.F.; Lange, R.

    1990-09-01

    The Chernobyl source term available for long-range transport was estimated by integration of radiological measurements with atmospheric dispersion modeling and by reactor core radionuclide inventory estimation in conjunction with WASH-1400 release fractions associated with specific chemical groups. The model simulations revealed that the radioactive cloud became segmented during the first day, with the lower section heading toward Scandinavia and the upper part heading in a southeasterly direction with subsequent transport across Asia to Japan, the North Pacific, and the west coast of North America. By optimizing the agreement between the observed cloud arrival times and duration of peak concentrations measured over Europe, Japan, Kuwait, and the US with the model predicted concentrations, it was possible to derive source term estimates for those radionuclides measured in airborne radioactivity. This was extended to radionuclides that were largely unmeasured in the environment by performing a reactor core radionuclide inventory analysis to obtain release fractions for the various chemical transport groups. These analyses indicated that essentially all of the noble gases, 60% of the radioiodines, 40% of the radiocesium, 10% of the tellurium and about 1% or less of the more refractory elements were released. These estimates are in excellent agreement with those obtained on the basis of worldwide deposition measurements. The Chernobyl source term was several orders of magnitude greater than those associated with the Windscale and TMI reactor accidents. However, the {sup 137}Cs from the Chernobyl event is about 6% of that released by the US and USSR atmospheric nuclear weapon tests, while the {sup 131}I and {sup 90}Sr released by the Chernobyl accident was only about 0.1% of that released by the weapon tests. 13 refs., 2 figs., 7 tabs.

  18. On the Aerosol Source Livestock Raising

    NASA Astrophysics Data System (ADS)

    Schneider, F. E.; Brüggemann, E.; Gnauk, T.; Lammel, G.; Müller, F.; Plewka, A.; Röhrl, A.; Wieser, P. H.

    2002-12-01

    Agriculture is a prime stakeholder in the atmospheric and climate changes as on one hand side it will be strongly affected by a changing climate and yet is today by air pollution while on the other hand, through her emissions agriculture is also driving these changes. Particulate matter is important for air pollution / human health. Very little is known about the mass flux and composition of the particulate matter emitted from livestock farming. We report on the design and results of a pilot study investigating the aerosol source livestock farming undertaken at the experimental farm Talgut Lindenhof of the University of Hohenheim, in a hilly region in Southern Germany. Particulate matter was sampled for off-line chemical analyses and physically characterized in-situ close to the animal housings as well as through simultaneous measurements upwind and downwind of the farm. Off-line analyses comprised particulate matter mass, inorganic ion content, carbon fractions, total element content, single particle analyses, besides other. Estimates on the emission term are made.

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

    NASA Astrophysics Data System (ADS)

    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.

  20. Particle size distribution of indoor aerosol sources

    SciTech Connect

    Shah, K.B.

    1990-10-24

    As concern about Indoor Air Quality (IAQ) has grown in recent years, it has become necessary to determine the nature of particles produced by different indoor aerosol sources and the typical concentration that these sources tend to produce. These data are important in predicting the dose of particles to people exposed to these sources and it will also enable us to take effective mitigation procedures. Further, it will also help in designing appropriate air cleaners. A new state of the art technique, DMPS (Differential Mobility Particle Sizer) System is used to determine the particle size distributions of a number of sources. This system employs the electrical mobility characteristics of these particles and is very effective in the 0.01--1.0 {mu}m size range. A modified system that can measure particle sizes in the lower size range down to 3 nm was also used. Experimental results for various aerosol sources is presented in the ensuing chapters. 37 refs., 20 figs., 2 tabs.

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

    NASA Astrophysics Data System (ADS)

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

    2014-08-01

    Aerosol particles were characterized by an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) along with various collocated instruments in Beijing, China to investigate the aerosol composition and sources during the Chinese Spring Festival, 2013. Three fireworks (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 showed major impacts on non-refractory potassium, chloride, sulfate, and organics in PM1, of which the FW organics appeared to be mainly secondary with its mass spectrum resembling to 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 PM1 accounting for 63-82% during the nine PEs observed. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than that during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impacts of reduced anthropogenic emissions on aerosol chemistry in the city. The primary species showed ubiquitous reductions during the holiday period with the largest reduction for cooking OA (69%), nitrogen monoxide (54%), and coal combustion OA (28%). The secondary sulfate, however, remained minor change, and the SOA and the total PM2.5 even slightly increased. These results have significant implications that controlling local primary source emissions, e.g., cooking and traffic activities, might have limited effects on improving air quality during PEs when SPM that is formed over regional scales dominates aerosol particle composition.

  2. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; Prévôt, A. S. H.; El Haddad, I.

    2015-08-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make impractical its deployment at sufficient sites to determine regional characteristics. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, PM10) collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g. AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon, oxygen containing and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g. filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially-resolved long-term datasets.

  3. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; El Haddad, I.; Prévôt, A. S. H.

    2016-01-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.

  4. Sources, Transport, and Climate Impacts of Biomass Burning Aerosols

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2010-01-01

    In this presentation, I will first talk about fundamentals of modeling of biomass burning emissions of aerosols, then show the results of GOCART model simulated biomass burning aerosols. I will compare the model results with observations of satellite and ground-based network in terms of total aerosol optical depth, aerosol absorption optical depth, and vertical distributions. Finally the long-range transport of biomass burning aerosols and the climate effects will be addressed. I will also discuss the uncertainties associated with modeling and observations of biomass burning aerosols

  5. AEROSOL Characterization in SW Asia from long-term AERONET Observations

    NASA Astrophysics Data System (ADS)

    Holben, B. N.

    2005-12-01

    The Arabian Gulf is a focus of aerosol sources and transport in Southwest Asia owing to arid landscapes modified by land degradation, a highly developed fossil fuel industry and the unique meteorology of the region. The aerosol properties were well characterized in the gulf during the UAE2 campaign but their impact on the greater South and Southwest Asia aerosol environment is not well known. The AERONET program has a well established network in the gulf region with a growing distribution in SW Asia including India, Israel, Chad, and SE Africa and Indian Ocean island sites. This presentation will compare the UAE2 campaign and longer term gulf region aerosol characterizations from AERONET to the wider subcontinental and oceanic aerosol properties measured by AERONET over the last decade. These long-term point observations will be supported by backtrajectories and selected MODIS and MISR data since 2001.

  6. Sources and composition of urban aerosol particles

    NASA Astrophysics Data System (ADS)

    Vogt, M.; Johansson, C.; Mårtensson, M.; Struthers, H.; Ahlm, L.; Nilsson, D.

    2011-09-01

    From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp) from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass <1 μm Dp (PM1) with water soluble soil contributing 11% and water insoluble soil 47%. Carbonaceous compounds were at the most 27% of PM1 mass. It was found that heating the air from the tower to 200 °C resulted in the loss of approximately 60% of the aerosol volume at 0.25 μm Dp whereas only 40% of the aerosol volume was removed at 0.6 μm Dp. Further heating to 300 °C caused very little additional losses <0.6 μm Dp. The chemical analysis did not include carbonaceous compounds, but based on the difference between the total mass concentration and the sum of the analyzed non-carbonaceous materials, it can be assumed that the non-volatile particulate material (heated to 300 °C) consists mainly of carbonaceous compounds, including elemental carbon. Furthermore, it was found that the non-volatile particle fraction <0.6 μm Dp correlated (r2 = 0.4) with the BC concentration at roof level in the city, supporting the assumption that the non-volatile material consists of carbonaceous compounds. The average diurnal cycles of the BC emissions from road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles <0.6 μm Dp to be 2.4±1.4 mg veh-1 km-1 based on either CO2 fluxes or traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and

  7. Long term aerosol and trace gas measurements in Central Amazonia

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Barbosa, Henrique M. J.; Ferreira de Brito, Joel; Carbone, Samara; Rizzo, Luciana V.; Andreae, Meinrat O.; Martin, Scot T.

    2016-04-01

    The central region of the Amazonian forest is a pristine region in terms of aerosol and trace gases concentrations. In the wet season, Amazonia is actually one of the cleanest continental region we can observe on Earth. A long term observational program started 20 years ago, and show important features of this pristine region. Several sites were used, between then ATTO (Amazon Tall Tower Observatory) and ZF2 ecological research site, both 70-150 Km North of Manaus, receiving air masses that traveled over 1500 km of pristine tropical forests. The sites are GAW regional monitoring stations. Aerosol chemical composition (OC/EC and trace elements) is being analysed using filters for fine (PM2.5) and coarse mode aerosol as well as Aerodyne ACSM (Aerosol Chemical Speciation Monitors). VOCs are measured using PTR-MS, while CO, O3 and CO2 are routinely measured. Aerosol absorption is being studied with AE33 aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using TSI and Ecotech nephelometers. Aerosol size distribution is determined using scanning mobility particle sizer at each site. Lidars measure the aerosol column up to 12 Km providing the vertical profile of aerosol extinction. The aerosol column is measures using AERONET sun photometers. In the wet season, organic aerosol comprises 75-85% of fine aerosol, and sulfate and nitrate concentrations are very low (1-3 percent). Aerosols are dominated by biogenic primary particles as well as SOA from biogenic precursors. Black carbon in the wet season accounts for 5-9% of fine mode aerosol. Ozone in the wet season peaks at 10-12 ppb at the middle of the day, while carbon monoxide averages at 50-80 ppb. Aerosol optical thickness (AOT) is a low 0.05 to 0.1 at 550 nm in the wet season. Sahara dust transport events sporadically enhance the concentration of soil dust aerosols and black carbon. In the dry season (August-December), long range transported

  8. Natural Radionuclides and Isotopic Signatures for Determining Carbonaceous Aerosol Sources, Aerosol Lifetimes, and Washout Processes

    SciTech Connect

    Gaffney, Jeffrey

    2012-12-12

    This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

  9. Source apportionment of absorbing aerosols in the central Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Vaishya, Aditya; Singh, Prayagraj; Rastogi, Shantanu; Babu, S. Suresh

    2016-05-01

    Atmospheric aerosols in the Indo-Gangetic Plain (IGP) depicts high spatial and temporal heterogeneity in their radiative properties. Despite the fact that significant advancement in terms of characterizing aerosols radiative and physiochemical properties in the IGP have been made, information regarding the organic content towards total absorbing aerosol budget is lacking. In the present study we have analyzed two years of aerosol spectral light absorption measurements from the central-IGP, Gorakhpur (26.75°N, 83.38°E, 85m amsl), in order to study their seasonal behavior and to quantify their magnitude in terms of absorbing aerosols loading and source speciation. Remote sensing data in the form of 'Cloud corrected Fire Count' from MODIS Terra and 'Absorption Aerosol Index' from OMI satellites platform have been used to identify absorbing aerosol source regions. Spectral absorption analysis reveals a four-fold enhancement in absorption in the winter (W) and the post-monsoon (PoM) seasons at UV wavelengths as compared to 880 nm on account of increased biomass aerosol contribution to total absorbing aerosol load. Despite having higher fire events and absorption aerosol index, both indicating high biomass burning activities, in the pre-monsoon (PM) season, aerosols from the biomass sources contribute ~ 27% during the W and the PoM seasons as against ~17% in the PM season to the total absorbing aerosol content. This is due to near stagnant wind conditions and shallow height of air masses travelling to the central IGP in the W and the PoM seasons.

  10. Sources of Size Segregated Sulfate Aerosols in the Arctic Summer

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhadgharelar, R.; Norman, A. L.; Abbatt, J.; Levasseur, M.

    2015-12-01

    Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor fitted to a high volume sampler was used for this study and was modified to permit collection of SO2 after aerosols were removed from the gas stream. The isotopic composition of sulfate aerosols and SO2 was measured and apportionment calculations have been performed to quantify the contribution of biogenic as well as anthropogenic sources to the growth of different aerosol size fractions in the atmosphere. The presence of sea salt sulfate aerosols was especially high in coarse mode aerosols as expected. The contribution of biogenic sulfate concentration in this study was higher than anthropogenic sulfate. Around 70% of fine aerosols (<0.49 μm) and 86% of SO2 were from biogenic sources. Concentrations of biogenic sulfate for fine aerosols, ranging from 18 to 625 ng/m3, were five times higher than total biogenic sulfate concentrations measured during Fall in the same region (Rempillo et al., 2011). A comparison of the isotope ratio for SO2 and fine aerosols offers a way to determine aerosol growth from local SO2 oxidation. For some samples, the values for SO2 and fine aerosols were close together suggesting the same source for SO2 and aerosol sulfur.Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor

  11. Aerosol Source Attributions and Source-Receptor Relationships Across the Northern Hemisphere

    NASA Technical Reports Server (NTRS)

    Bian, Huisheng; Chin, Mian; Kucsera, Tom; Pan, Xiaohua; Darmenov, Anton; Colarco, Peter; Torres, Omar; Shults, Michael

    2014-01-01

    Emissions and long-range transport of air pollution pose major concerns on air quality and climate change. To better assess the impact of intercontinental transport of air pollution on regional and global air quality, ecosystems, and near-term climate change, the UN Task Force on Hemispheric Transport of Air Pollution (HTAP) is organizing a phase II activity (HTAP2) that includes global and regional model experiments and data analysis, focusing on ozone and aerosols. This study presents the initial results of HTAP2 global aerosol modeling experiments. We will (a) evaluate the model results with surface and aircraft measurements, (b) examine the relative contributions of regional emission and extra-regional source on surface PM concentrations and column aerosol optical depth (AOD) over several NH pollution and dust source regions and the Arctic, and (c) quantify the source-receptor relationships in the pollution regions that reflect the sensitivity of regional aerosol amount to the regional and extra-regional emission reductions.

  12. Approximate factorization with source terms

    NASA Technical Reports Server (NTRS)

    Shih, T. I.-P.; Chyu, W. J.

    1991-01-01

    A comparative evaluation is made of three methodologies with a view to that which offers the best approximate factorization error. While two of these methods are found to lead to more efficient algorithms in cases where factors which do not contain source terms can be diagonalized, the third method used generates the lowest approximate factorization error. This method may be preferred when the norms of source terms are large, and transient solutions are of interest.

  13. The short-term association of selected components of fine particulate matter and mortality in the Denver Aerosol Sources and Health (DASH) study

    EPA Science Inventory

    Associations of short-term exposure to fine particulate matter (PM2.5) with daily mortality may be due to specific PM2.5 chemical components. Objectives: Daily concentrations of PM2.5 chemical species were measured over five consecutive years in Denver, CO to investigate whethe...

  14. Aerosol nitrate from lightning - from sources to impacts

    NASA Astrophysics Data System (ADS)

    Tost, Holger

    2016-04-01

    Particulate nitrate is a key component on the inorganic atmospheric aerosol composition. Due to its semi-volatility, an accurate description of the budget and the impacts of nitrate aerosol are still somewhat uncertain. To address some of the impacts of nitrate, in this study we explicitly analyse the impact of aerosol nitrate from a natural source, namely lightning. As the lightning NOx emissions are only a contribution to the total NOx emissions, this example does not resemble a typical annihilation scenario, which might substantially misjudge the effect of aerosol nitrate due to the high non-linearity in the nitrate budget, but also other directly connected compounds, but tries to shed light onto the sensitivity of aerosol nitrate and its effects. On the other hand, lightning represents an emission source of NOx, which is partly injected directly in the upper troposphere, where due to its longer lifetime and the temperature dependent stability of NH4NO3 aerosol nitrate can form much easier and has a longer lifetime against decomposition. This study uses a comprehensive chemistry climate model to track the evolution of aerosol nitrate from the lightning NOx emission, via chemical processing and gas-aerosol partitioning, aerosol microphyiscal processes down to the climatic impacts of the nitrate aerosol particles via direct aerosol-radiation and aerosol-cloud interactions. All of these processes are explicitly considered with the help of state-of-the-art (parameterisation) schemes, including a comprehensive multi-phase chemistry configuration, a microphysical and chemical composition aerosol model, aerosol optical properties and a two-moment cloud microphysical scheme with explicit activation of aerosol particles into cloud droplets and the consideration of aerosol particles in ice formation processes. Furthermore, some uncertainty with respect to cloud droplet formation has been considered by using two different aerosol activation schemes. To estimate the

  15. SOURCES OF ORGANIC AEROSOL: SEMIVOLATILE EMISSIONS AND PHOTOCHEMICAL AGING

    EPA Science Inventory

    The proposed research integrates emissions testing, smog chamber experiments, and regional chemical transport models (CTMs) to investigate the sources of organic aerosol in urban and regional environments.

  16. Long-term memory of atmospheric aerosols over India

    NASA Astrophysics Data System (ADS)

    B, A.

    2014-12-01

    Long-term memory of atmospheric variables is a least understood facet in atmospheric science. The temporal and spatial distribution of atmospheric aerosols depends largely on the atmospheric parameters. Time series analysis using a stochastic model reveals that atmospheric aerosols over India exhibit a long-term memory. Our analysis confirms that by using Autoregressive Integrated Moving Average (ARIMA) model we can parsimoniously model the aerosol optical depth (AOD) over the Indian region with a reasonably good accuracy. This major advantage of this method is that by using past observations we were able to generate forecasts for next 3 years. The forecasts thus generate shows a good fit with the observations. This persistence is due to the presence of temporal dependence between successive observations.

  17. Aerosol Source Plume Physical Characteristics from Space-based Multiangle Imaging

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.; Li, W.-H.; Moroney, Catherine; Diner, David J.; Martonchik, John V.; Fishbein, Evan

    2007-01-01

    Models that assess aerosol effects on regional air quality and global climate parameterize aerosol sources in terms of amount, type, and injection height. The multiangle imaging spectroradiometer (MISR) aboard NASA's Terra satellite retrieves total column aerosol optical thickness (AOT), and aerosol type over cloud-free land and water. A stereo-matching algorithm automatically retrieves reflecting-layer altitude wherever clouds or aerosol plumes have discernable spatial contrast, with about 500-m accuracy, at 1.1-km horizontal resolution. Near-source biomass burning smoke, volcanic effluent, and desert dust plumes are observed routinely, providing information about aerosol amount, particle type, and injection height useful for modeling applications. Compared to background aerosols, the plumes sampled have higher AOT, contain particles having expected differences in Angstrom exponent, size, single-scattering albedo, and for volcanic plume and dust cloud cases, particle shape. As basic thermodynamics predicts, thin aerosol plumes lifted only by regional winds or less intense heat sources are confined to the boundary layer. However, when sources have sufficient buoyancy, the representative plumes studied tend to concentrate within discrete, high-elevation layers of local stability; the aerosol is not uniformly distributed up to a peak altitude, as is sometimes assumed in modeling. MISR-derived plume heights, along with meteorological profile data from other sources, make it possible to relate radiant energy flux observed by the moderate resolution imaging spectroradiometer (MODIS), also aboard the Terra spacecraft, to convective heat flux that plays a major role in buoyant plume dynamics. A MISR climatology of plume behavior based on these results is being developed.

  18. Do anthropogenic, continental or coastal aerosol sources impact on a marine aerosol signature at Mace Head?

    NASA Astrophysics Data System (ADS)

    O'Dowd, C.; Ceburnis, D.; Ovadnevaite, J.; Vaishya, A.; Rinaldi, M.; Facchini, M. C.

    2014-10-01

    Atmospheric aerosols have been sampled and characterised at the Mace Head north-east (NE) Atlantic atmospheric research station since 1958, with many interesting phenomena being discovered. However, with the range of new discoveries and scientific advances, there has been a range of concomitant criticisms challenging the representativeness of aerosol sampled at the station compared to that of aerosol over the pristine open-ocean. Two recurring criticisms relate to the lack of representativeness due to potentially enhanced coastal sources, possibly leading to artificially high values of aerosol concentrations, and to the influence of long-range transport of anthropogenic or continental aerosol and its potential dominance over, or perturbation of, a natural marine aerosol signal. Here, we review the results of previous experimental studies on marine aerosols over the NE Atlantic and at Mace Head with the aim of evaluating their representativeness relative to that of a pristine open-ocean aerosol, i.e. with negligible anthropogenic/continental influence. Particular focus is given to submicron organic matter (OM) aerosol. In summary, no correlation was found between OM and black carbon (BC) in marine air conforming to clean-air sampling criteria, either at BC levels of 0-15 or 15-50 ng m-3, suggesting that OM concentrations, up to observed peak values of 3.8 μg m-3, are predominantly natural in origin. Sophisticated carbon isotope analysis and aerosol mass spectral finger printing techniques corroborate the conclusion that there is a predominant natural source of OM, with 80% biogenic source apportionment being observed for general clean-air conditions, rising to ∼98% during specific primary marine organic plumes when peak OM mass concentrations > 3 μg m-3 are observed. Similarly, a maximum contribution of 20% OM mass coming from non-marine sources was established by dual carbon isotope analysis. Further, analysis of a series of experiments conducted at Mace Head

  19. Multi-Decadal Variation of Aerosols: Sources, Transport, and Climate Effects

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Diehl, Thomas; Bian, Huisheng; Streets, David

    2008-01-01

    We present a global model study of multi-decadal changes of atmospheric aerosols and their climate effects using a global chemistry transport model along with the near-term to longterm data records. We focus on a 27-year time period of satellite era from 1980 to 2006, during which a suite of aerosol data from satellite observations, ground-based measurements, and intensive field experiments have become available. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which involves a time-varying, comprehensive global emission dataset that we put together in our previous investigations and will be improved/extended in this project. This global emission dataset includes emissions of aerosols and their precursors from fuel combustion, biomass burning, volcanic eruptions, and other sources from 1980 to the present. Using the model and satellite data, we will analyze (1) the long-term global and regional aerosol trends and their relationship to the changes of aerosol and precursor emissions from anthropogenic and natural sources, (2) the intercontinental source-receptor relationships controlled by emission, transport pathway, and climate variability.

  20. Season - dependent and source-influenced aerosol in Northern Siberia

    NASA Astrophysics Data System (ADS)

    Popovicheva, Olga; Makshtas, Alexander; Bogorodsky, Peter; Eleftheriadis, Kostantinos; Diapouli, Evangelia; Shonia, Natalia; Uttal, Taneil

    2016-04-01

    Aerosol may serve as a tracer of arctic pollution, allowing a link to climate response if its major characteristics relating to natural and anthropogeneous sources are defined. It has been shown that BC and sulfates are the most important aerosol constituents measured in the Arctic boundary layer; these species demonstrate similar seasonal variations with a peak during winter to early spring and a minimum in summer. Long - time gap in consistent aerosol observations in the Russian Arctic strongly limits the assessment of air pollution and climate impacts. On-line monitoring, sampling, and analyses of atmospheric aerosols were carried out at the Tiksi Hydrometeorological Observatory, Northern Siberia, during one year from September 2014 to 2015. Physico-chemical characterization combining aethalometry, thermo-optical analysis, and analytical chemistry was used in order to identify the seasonal variability of aerosols and to link their composition to possible sources, as well as to characterize the differences in aerosol chemical composition between natural background conditions and BC-pollution episodes. The present study reports the first results from the Tiksi Observatory on season-dependent and source-influenced characteristics of aerosol species, such as carbon fractions (OC, EC), inorganic and organic functionalities of chemical compounds, sulfates, nitrates and other ion components, and elements. In addition, data obtained by individual particles analysis provide insight into micromarkers of combustion sources. Aerosol at the Tiksi Observatory is found to be originated from natural marine, biogenic, and continental sources as well as influenced by local residential activity and regional pollution. Characterization of aerosols during OC and BC-pollution episodes, combined with analysis of the wind direction, atmosphere stability, and air mass trajectories, allows for the identification of the sources which are responsible for the emission of hazardous compounds

  1. Aeronet-based Microphysical and Optical Properties of Smoke-dominated Aerosol near Source Regions and Transported over Oceans, and Implications for Satellite Retrievals of Aerosol Optical Depth

    NASA Technical Reports Server (NTRS)

    Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

    2013-01-01

    Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad families of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA 0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA 0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savanna at Mongu (Zambia), with average SSA 0.85 in the midvisible. These can serve as candidate sets of aerosol microphysicaloptical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

  2. Long-Term Measurements of Carbon Monoxide and Aerosols at the ZOTTO tall tower, Siberia

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Birmili, W.; Chi, X.; Heimann, M.; Heintzenberg, J.; Mikhailov, E.; Panov, A.

    2012-04-01

    The Zotino Tall Tower Observatory (ZOTTO), operated by the Max Planck Institutes for Biogeochemistry and Chemistry and the Institute of Forest (Krasnoyarsk), is located at 89.35°E, 60.80°N, 114 m asl. at a very remote continental site in Siberia, Russia. It centers on a 300-m tower designed for scientific measurements of chemical (trace gases, aerosol) and physical (meteorological) properties. The instrumentation at the observatory includes a CO Monitor, a Particle Soot Absorption Photometer (PSAP) for determining the aerosol absorption coefficient, a nephelometer for the determination of the aerosol scattering coefficient, and a Differential Mobility Particle Sizer (DMPS) to measure the aerosol number size distribution. We present measurements made from October 2006 until March 2011, with some interruptions due to technical reasons. An annual cycle of the background CO mixing rations was observed with summer minima around 90 ppb and winter maxima of about 175 ppb. Amplitude and phase of the annual cycle were generally similar to that reported by NOAA-ESRL for latitude 61°N, but showed an earlier onset of the elevated winter values. Episodes of elevated CO and aerosol concentrations, typically lasting for several days, are superimposed on the background seasonal cycle. During winter, these pollution episodes are usually associated with air masses that have passed over the central Siberian region around Omsk and Novosibirsk - a heavily industrialized area. During spring and summer, elevated levels of CO and aerosols are often caused by agricultural fires in southern Siberia and Kazakhstan or by forest fires in boreal Siberia. The optical properties of the aerosol showed more pronounced seasonal variability than the aerosol mass and number concentrations. Wintertime aerosols were highly absorbing, with single scattering albedos (SSA) around 0.85, consistent with a dominant fossil fuel combustion source. In contrast, summertime aerosols had very low absorption

  3. Do anthropogenic or coastal aerosol sources impact on a clean marine aerosol signature at Mace Head?

    NASA Astrophysics Data System (ADS)

    O'Dowd, C.; Ceburnis, D.; Ovadnevaite, J.; Rinaldi, M.; Facchini, M. C.

    2013-03-01

    Atmospheric aerosols have been sampled and characterised at the Mace Head North East (N.E.) Atlantic atmospheric research station since 1958, with many interesting phenomena being discovered. However, with the range of new discoveries and scientific advances, there has been a range of concomitant criticisms challenging the representativeness of aerosol sampled at the station to that of aerosol over the open ocean. Two recurring criticisms relate to the lack of representativeness due to enhanced coastal sources, thereby leading to artificially high values to aerosol parameters, and to the influence of long-range transport of anthropogenic aerosol and its potential dominance over, or drowning-out of, a natural marine aerosol signal. Here we review the results of previous experimental studies into marine aerosols over the N.E. Atlantic and at Mace Head with the aim of evaluating their representativeness relative to that of an open ocean aerosol with negligible anthropogenic influence. Particular focus is given to organic matter (OM) aerosol. In summary, no correlation was found between OM and black carbon (BC) either at BC levels of 0-15 or 15-50 ng m-3, suggesting that OM concentrations up to peak values of 3.8 μg m-3 are predominantly natural in origin. Sophisticated carbon isotope analysis and aerosol mass spectral finger printing corroborate the natural source of OM with 80% biogenic source apportionment being observed for general clean air conditions, rising to 98% during specific primary marine organic plumes when peak concentrations >3 μg m-3 are observed. A range of other experiments are discussed which corroborate the dominance of a marine signal under Mace Head clean air criteria along. Further, analysis of a series of experiments conducted at Mace Head conclude that negligible coastal, surf zone, or tidal effects are discernible in the submicron size range for sampling heights of 7 m and above. The Mace Head clean air criteria ensures anthropogenic and

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

    NASA Astrophysics Data System (ADS)

    Dron, J.; El Haddad, I.; Temime-Roussel, B.; Jaffrezo, J.-L.; Wortham, H.; Marchand, N.

    2010-04-01

    The functional group composition of various organic aerosols (OA) is being investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS). The determinations of the three functional groups' contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups) and precursor ion (nitro groups) 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 photo-oxidation 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 accounted for 1.7% (vehicular) to 13.5% (o-xylene photo-oxidation) of the organic carbon. The diagnostic functional group ratios are then used to tentatively differentiate 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 distinguish the 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 assesses a wood burning organic carbon contribution of about 60%. Finally, examples of functional group mass spectra of all

  5. Source, significance, and control of indoor microbial aerosols: human health aspects.

    PubMed Central

    Spendlove, J C; Fannin, K F

    1983-01-01

    The usual profile of indoor microbial aerosols probably has little meaning to healthy people. However, hazardous microbial aerosols can penetrate buildings or be generated within them; in either case, they can have significant adverse effects on human health. These aerosols can be controlled to some extent by eliminating or reducing their sources. In this regard, careful consideration should be given in building construction to the design of ventilation and air-conditioning systems and to the flooring material, so that these systems and the flooring material will not act as microbial reservoirs. It is evident that in spite of the considerable body of data available on indoor microbial aerosols, little is known of their true significance to human health except in terms of overt epidemic disease. Continued research is needed in this area, particularly in respect to situations of high risk in such locations as hospitals and schools for young children. PMID:6867255

  6. A large source of low-volatility secondary organic aerosol.

    PubMed

    Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F

    2014-02-27

    Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally. PMID:24572423

  7. A large source of low-volatility secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B.; Jørgensen, Solvejg; Kjaergaard, Henrik G.; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R.; Wildt, Jürgen; Mentel, Thomas F.

    2014-02-01

    Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

  8. Investigating Types and Sources of Organic Aerosol in Rocky Mountain National Park Using Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L.

    2011-12-01

    The Rocky Mountain Atmospheric Nitrogen and Sulfur Study (RoMANS) focuses on identifying pathways and sources of nitrogen deposition in Rocky Mountain National Park (RMNP). Past work has combined measurements from a range of instrumentation such as annular denuders, PILS-IC, Hi-Vol samplers, and trace gas analyzers. Limited information from early RoMANS campaigns is available regarding organic aerosol. While prior measurements have produced a measure of total organic carbon mass, high time resolution measures of organic aerosol concentration and speciation are lacking. One area of particular interest is characterizing the types, sources, and amounts of organic nitrogen aerosol. Organic nitrogen measurements in RMNP wet deposition reveal a substantial contribution to the total reactive nitrogen deposition budget. In this study an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in summer 2010 at RMNP to investigate organic aerosol composition and its temporal variability. The species timeline and diurnal species variations are combined with meteorological data to investigate local transport events and chemistry; transport from the Colorado Front Range urban corridor appears to be more significant for inorganic species than for the overall organic aerosol mass. Considerable variation in organic aerosol concentration is observed (0.5 to 20 μg/m3), with high concentration episodes lasting between hours and two days. High resolution AMS data are analyzed for organic aerosol, including organic nitrogen species that might be expected from local biogenic emissions, agricultural activities, and secondary reaction products of combustion emissions. Positive matrix factorization reveals that semi-volatile oxidized OA, low-volatility oxidized OA, and biomass burning OA comprise most organic mass; the diurnal profile of biomass burning OA peaks at four and nine pm and may arise from local camp fires, while constant concentrations of

  9. Short-term Aerosol Trends: Reality or Myth?

    NASA Technical Reports Server (NTRS)

    Leptoukh, Gregory; Zubko, Viktor

    2009-01-01

    The main questions addressed in this slide presentation involve short-term trends of MODIS aerosol optical thickness (AOT) over 6 years: (1) Why are the trends different in different regions? (2) How are these trends so high? (3) Why are they "coherent" in many areas? (4) Are these changes in aerosol concentrations real, i.e., are they monotonic changes in emissions? Several views of the Spatial Distribution of AOT from Terra are shown. In conclusion there are several trends: (1) There is a broad spatial inhomogenueity in AOT trends over 6 years of MODIS Terra and Aqua (2) Some of the areas demonstrate clear positive trends related to increase of emission (e.g., Eastern China) (3) Strong trends in some other areas are superficial and might be attributed, in part, to: (3a) Least squares linear trend sensitivity to outliers (need to use more robust linear fitting method) (3b) Spatial and temporal shifts or trends in meteorological conditions, especially in wind patterns responsible for aerosol transport (6) Aerosol trends should be studied together with changes in meteorology patterns as they might closely linked together

  10. On the source of organic acid aerosol layers above clouds.

    PubMed

    Sorooshian, Armin; Lu, Miao-Ling; Brechtel, Fred J; Jonsson, Haflidi; Feingold, Graham; Flagan, Richard C; Seinfeld, John H

    2007-07-01

    During the July 2005 Marine Stratus/Stratocumulus Experiment (MASE) and the August-September 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed aerosols and cumulus clouds in the eastern Pacific Ocean off the coast of northern California and in southeastern Texas, respectively. An on-board particle-into-liquid sampler (PILS) quantified inorganic and organic acid species with < or = 5-min time resolution. Ubiquitous organic aerosol layers above cloud with enhanced organic acid levels were observed in both locations. The data suggest that aqueous-phase reactions to produce organic acids, mainly oxalic acid, followed by droplet evaporation is a source of elevated organic acid aerosol levels above cloud. Oxalic acid is observed to be produced more efficiently relative to sulfate as the cloud liquid water content increases, corresponding to larger and less acidic droplets. As derived from large eddy simulations of stratocumulus underthe conditions of MASE, both Lagrangian trajectory analysis and diurnal cloudtop evolution provide evidence that a significant fraction of the aerosol mass concentration above cloud can be accounted for by evaporated droplet residual particles. Methanesulfonate data suggest that entrainment of free tropospheric aerosol can also be a source of organic acids above boundary layer clouds. PMID:17695910

  11. Lead Isotopic Composition and Trace Metals in Aerosols for Source Apportionment

    NASA Astrophysics Data System (ADS)

    Chien, C. T.; Paytan, A.

    2014-12-01

    Transported thousands of miles away from their source, aerosols can be dispersed and deposition throughout the Earth's surface. Aerosols from natural and industrial sources have different characteristics and health impacts thus it is important to identify their sources. The lead isotopic composition and trace metals in aerosol samples collected in different regions and periods around the world can help us better understand spatial and seasonal variation of aerosol sources. Aerosol samples collected in California, Bermuda, China and the Red Sea have been analyzed. The trace metal and Pb isotopes in these samples provide information regarding the various sources of aerosols to these sites.

  12. Solubility of aerosol trace elements: sources and deposition fluxes in the Canary Region

    NASA Astrophysics Data System (ADS)

    Gelado-Caballero, María Dolores; López-García, Patricia; Patey, Matthew; Prieto, Sandra; Collado, Cayetano; Santana, Desire; Hernández-Brito, Joaquín

    2013-04-01

    To date there have been no long-term aerosol studies in the Canary Basin, and current estimates of soluble fluxes of Al, Mn, Fe, P and N for the region are based on limited data available from several oceanographic research cruises which have crossed the region during large transects of the Atlantic Ocean. In this study, aerosol samples have been collected at two stations on the island of Gran Canaria regularly since 2006 (Taliarte, at sea level, and Pico de la Gorra, at 1930 m altitude). Samples have been analysed for total and soluble trace metals (Al, Mn, Fe, Co, Cu and Ti). The high temporal resolution of this dataset represents a valuable contribution to the understanding of aerosol deposition of trace metals to the region. Solubility measurements from acetate buffer leaching experiments showed the same tendency in the percentage of soluble metals in the samples: a higher percentage solubility of metals in anthropogenic aerosols and at low dust loading. Moreover, categorisation of aerosol samples with a continental African origin according to air-mass back-trajectories (North of Africa, Central and Western Sahara and Sahel) showed a decreasing tendency in the percentage of soluble Al and Fe to the south. In addition, factors that can affect the percentage solubility values for crustal elements and comparisons with different methods were studied. Freezing the samples stored affects the measurements of Al and Fe solubility. This last result is important for the design of future aerosol sampling programmes and aerosol solubility experiments. Flux estimates for aerosol-derived soluble metals reveal that phosphate is highly depleted relative to Fe and N when compared with Redfield values. It appears that aerosol deposition is an important source of N and trace metals (Fe, Co, Mn and Al) to the NE subtropical Atlantic Ocean. This work has been supported by the European Commission FEDER funds (PCT MAC 2007-2013, ESTRAMAR Mac/3/C177).

  13. Temporal variations and sources of Eastern Mediterranean aerosols based on a 9-year observation

    NASA Astrophysics Data System (ADS)

    Öztürk, F.; Zararsız, A.; Dutkiewicz, V. A.; Husain, L.; Hopke, P. K.; Tuncel, G.

    2012-12-01

    Concentrations of 48 elements, NO3-, SO42-, Cl-, NH4+, and black carbon (BC) were determined in PM10 aerosols collected daily at a rural Eastern Mediterranean (EM) site (Antalya, 30.34°E, 36.47°N) from 1993 to 2001. Temporal variations (daily, seasonal and long term), sources and source regions of EM aerosols were delineated. Concentrations of elements with marine and crustal origin were more episodic as compared to anthropogenic ones. Most of the variables showed well defined seasonal cycles. Concentrations of crustal elements increased in summer while winter concentrations of marine elements were considerably higher than in summer. Trends in concentrations were analyzed using the Kendall test. Essentially, all elements showed decreasing trends. Sen's slope was applied to find the magnitude of the trends. The annual rate of decrease was found to change from 0.001 to 209 ng m-3. A receptor-based model, Positive Matrix Factorization (PMF), resolved five factors influencing the chemical composition of EM aerosols as airborne dust, oil combustion, coal combustion, motor vehicle emissions and sea salt. Potential Source Contribution Function (PSCF) analysis was performed to identify the likely areas influencing the chemical composition of aerosol samples. Local and remote sources were detected for the factors resolved by PMF. PSCF maps including backward trajectories at starting height of 900 hPa have indicated that North Africa is the major source contributing to the concentrations of variables associated with dust factor.

  14. A biogenic source of oxalic acid in marine aerosol

    NASA Astrophysics Data System (ADS)

    Facchini, M.; Rinaldi, M.; Ceburnis, D.; O'Dowd, C.; Sciare, J.; Burrows, J. P.

    2010-12-01

    Oxalic acid has been often observed in marine aerosol, nevertheless, given the ubiquitous character and the high concentrations found in polluted environments, its origin has often been attributed to continental sources. In this work, we present the results of oxalic acid analyses, on aerosol samples collected at Mace Head (Ireland, 53°20’N, 9°54’W) and Amsterdam Island (Indian Ocean, 37°48’S, 77°34’E), supporting the existence of a biogenic source of oxalic acid over the oceans. Measurements cover the year 2006, at the Northern Hemisphere site, and the period 2003-2007, at the Southern Hemisphere one. Aerosol oxalic acid was detected in clean marine air masses in concentrations ranging from 2.7 to 39 ng m-3, at Mace Head, and from 0.31 to 17 ng m-3, at Amsterdam Island. In both hemispheres, oxalic acid concentration showed a clear seasonal trend, with maxima in spring-summer and minima in the fall-winter period, in analogy with other marine biogenic aerosol components (e.g., MSA and amines). Oxalic acid was distributed along the whole aerosol size spectrum, with the major contribution given by the 1.0-2.0 µm size range, and by the lower accumulation mode (0.25-0.5 µm). Given the observed size distributions, marine aerosol oxalic acid can be assumed as the result of the combination of different formation processes, among which in-cloud oxidation of gaseous precursors [1] and photochemical degradation of biogenic unsaturated fatty acids [2] are likely the most important. Among aerosol oxalic acid precursors, glyoxal is the most likely candidate in the marine boundary layer, as a source of glyoxal over the oceans has recently been discovered by satellite observations [3] and confirmed by in situ measurements [4]. In support of this hypothesis, SCIAMACHY satellite retrieved glyoxal column concentrations, over the two sampling sites, resulted characterized by a clear seasonal trend, resembling the aerosol oxalic acid one. [1] Warneck, Atmospheric

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

    NASA Astrophysics Data System (ADS)

    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

  16. Natural sources of atmospheric aerosols influencing air quality across Europe.

    PubMed

    Viana, M; Pey, J; Querol, X; Alastuey, A; de Leeuw, F; Lükewille, Anke

    2014-02-15

    Atmospheric aerosols are emitted by natural and anthropogenic sources. Contributions from natural sources to ambient aerosols vary widely with time (inter-annual and seasonal variability) and as a function of the distance to source regions. This work aims to identify the main natural sources of atmospheric aerosols affecting air quality across Europe. The origin, frequency, magnitude, and spatial and temporal variability of natural events were assessed for the years 2008 and 2009. The main natural sources of atmospheric aerosols identified were African dust, sea spray and wildfires. Primary biological particles were not included in the present work. Volcanic eruptions did not affect air quality significantly in Europe during the study period. The impact of natural episodes on air quality was significant in Southern and Western Europe (Cyprus, Spain, France, UK, Greece, Malta, Italy and Portugal), where they contributed to surpass the PM10 daily and annual limit values. In Central and Northern Europe (Germany, Austria and Latvia) the impact of these events was lower, as it resulted in the exceedance of PM daily but not annual limit values. Contributions from natural sources to mean annual PM10 levels in 2008 and 2009 ranged between 1 and 2 μg/m(3) in Italy, France and Portugal, between 1 and 4 μg/m(3) in Spain (10 μg/m(3) when including the Canary Islands), 5 μg/m(3) in UK, between 3 and 8 μg/m(3) in Greece, and reached up to 13 μg/m(3) in Cyprus. The evaluation of the number of monitoring stations per country reporting natural exceedances of the daily limit value (DLV) is suggested as a potential tool for air quality monitoring networks to detect outliers in the assessment of natural contributions. It is strongly suggested that a reference methodology for the identification and quantification of African dust contributions should be adopted across Europe. PMID:24342088

  17. Aerosol source attributions and source-receptor relationships across the Northern Hemisphere ---- initial results from HTAP2 model experiments

    NASA Astrophysics Data System (ADS)

    Bian, H.; Chin, M.; Kucsera, T. L.; Torres, O.; Pan, X.

    2014-12-01

    Emissions and long-range transport of air pollution pose major concerns on air quality and climate change. To better assess the impact of intercontinental transport of air pollution on regional and global air quality, ecosystems, and near-term climate change, the UN Task Force on Hemispheric Transport of Air Pollution (HTAP) is organizing a phase II activity (HTAP2) that includes global and regional model experiments and data analysis, focusing on ozone and aerosols. This study presents the initial results of HTAP2 global aerosol modeling experiments. We will (a) evaluate the model results with surface and aircraft measurements, (b) examine the relative contributions of regional emission and extra-regional source on surface PM concentrations and column aerosol optical depth (AOD) over several NH pollution and dust source regions and the Arctic, and (c) quantify the source-receptor relationships in the pollution regions that reflect the sensitivity of regional aerosol amount to the regional and extra-regional emission reductions.

  18. Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

    2015-11-01

    To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

  19. The long-term global record on Aerosol Absorption Optical Depth from TOMS and OMI observations

    NASA Astrophysics Data System (ADS)

    Torres, O.; Bhartia, P.; Ahn, C.; Veefkind, P.

    2006-12-01

    Carbonaceous aerosols from biomass burning and boreal forest fires, and desert dust lofted by the winds from the world major arid and semi-arid areas are among the most long-lived aerosol types in the Earth's atmosphere, since they often reach the free troposphere and are sometimes transported thousands of kilometers from their original sources. A lot has been learned about the global distribution of aerosol sources, and the transport patterns of these aerosol types since the development of the near-UV methods of aerosol detection and characterization using data from the TOMS series of instruments. Because both smoke and desert dust aerosols absorb UV-radiation, the TOMS aerosol sensing technique is specially suited for tracking these aerosol types over variety of surfaces including clouds and snow. TOMS aerosol observations, for instance, have been fundamental in discovering that carbonaceous aerosols associated with wild fires at mid and high latitudes often reach the lower stratosphere, and travel as far as the remote polar regions. We have recently completed the development of an improved algorithm to derive quantitative information about aerosol absorption optical depth using near-UV data. We will discuss the multi- decadal global record on aerosol absorption optical depth produced using TOMS and OMI sensors, and review the multiple contributions of the TOMS-OMI record to the current understanding of the factors that govern the observed temporal and spatial distribution of smoke and desert dust aerosols.

  20. Modelled radiative effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, Antti-Ilari; Dunne, Eimear M.; Bergman, Tommi; Laakso, Anton; Kokkola, Harri; Ovadnevaite, Jurgita; Sogacheva, Larisa; Baisnée, Dominique; Sciare, Jean; Manders, Astrid; O'Dowd, Colin; de Leeuw, Gerrit; Korhonen, Hannele

    2014-05-01

    Sea spray aerosol particles have significant effects on global climate by scattering solar radiation (direct effect) and modifying cloud properties (indirect effect). Sea spray consists mainly of sea salt, but in biologically active regions, major fraction of sea spray may come in the form of primary marine organic matter (PMOM). Traditionally, sea spray flux has been parameterized in global models in terms of wind speed, and organic fraction of sea spray in terms of chlorophyll-a concentration. In this study, we have incorporated recently developed parameterizations for the sea spray aerosol source flux into the global aerosol-climate model ECHAM-HAMMOZ. The parameterizations encapsulate the wave state via Reynolds number, and predict the organic fraction of the sea spray aerosol source flux. The model was then used to investigate the direct and indirect effects of sea spray aerosol particles. We compared simulated sea spray concentrations with in-situ measurements from Mace Head (North Atlantic), Point Reyes (North Pacific), and Amsterdam Island (Southern Indian Ocean). Aerosol optical depth (AOD) was compared with satellite measurements from PARASOL. Modelled annual mean global emissions of sea salt and PMOM were 805 Tg yr-1 (uncertainty range of 378-1233 Tg yr-1) and 1.1 Tg yr-1 (0.5-1.8 Tg yr-1), respectively. Sea salt emissions were considerably lower than the majority of previous estimates, but PMOM was in the range of previous studies. The model captured sea salt concentrations fairly well in the smaller size ranges at Mace Head (annual normalized mean bias of -13% for particles with vacuum aerodynamic diameter Dva

  1. Performance of personal inhalable aerosol samplers in very slowly moving air when facing the aerosol source.

    PubMed

    Witschger, O; Grinshpun, S A; Fauvel, S; Basso, G

    2004-06-01

    While personal aerosol samplers have been characterized primarily based on wind tunnel tests conducted at relatively high wind speeds, modern indoor occupational environments are usually represented by very slow moving air. Recent surveys suggest that elevated levels of occupational exposure to inhalable airborne particles are typically observed when the worker, operating in the vicinity of the dust source, faces the source. Thus, the first objective of this study was to design and test a new, low cost experimental protocol for measuring the sampling efficiency of personal inhalable aerosol samplers in the vicinity of the aerosol source when the samplers operate in very slowly moving air. In this system, an aerosol generator, which is located in the centre of a room-sized non-ventilated chamber, continuously rotates and omnidirectionally disperses test particles of a specific size. The test and reference samplers are equally distributed around the source at the same distance from the centre and operate in parallel (in most of our experiments, the total number of simultaneously operating samplers was 15). Radial aerosol transport is driven by turbulent diffusion and some natural convection. For each specific particle size and the sampler, the aerosol mass concentration is measured by weighing the collection filter. The second objective was to utilize the new protocol to evaluate three widely used aerosol samplers: the IOM Personal Inhalable Sampler, the Button Personal Inhalable Aerosol Sampler and the 25 mm Millipore filter holder (closed-face C25 cassette). The sampling efficiencies of each instrument were measured with six particle fractions, ranging from 6.9 to 76.9 micro m in their mass median aerodynamic diameter. The Button Sampler efficiency data demonstrated a good agreement with the standard inhalable convention and especially with the low air movement inhalabilty curve. The 25 mm filter holder was found to considerably under-sample the particles larger

  2. Development of alternate methods of determining integrated SMR source terms

    SciTech Connect

    Barry, Kenneth

    2014-06-10

    The Nuclear Energy Institute (NEI) Small Modular Reactor (SMR) Licensing Task Force (TF) has been evaluating licensing issues unique and important to iPWRs, ranking these issues, and developing NEI position papers for submittal to the U.S. Nuclear Regulatory Commission (NRC) during the past three years. Papers have been developed and submitted to the NRC in a range of areas including: Price-Anderson Act, NRC annual fees, security, modularity, and staffing. In December, 2012, NEI completed a draft position paper on SMR source terms and participated in an NRC public meeting presenting a summary of this paper, which was subsequently submitted to the NRC. One important conclusion of the source term paper was the evaluation and selection of high importance areas where additional research would have a significant impact on source terms. The highest ranked research area was iPWR containment aerosol natural deposition. The NRC accepts the use of existing aerosol deposition correlations in Regulatory Guide 1.183, but these were developed for large light water reactor (LWR) containments. Application of these correlations to an iPWR design has resulted in greater than a ten-fold reduction of containment airborne aerosol inventory as compared to large LWRs. Development and experimental justification of containment aerosol natural deposition correlations specifically for the unique iPWR containments is expected to result in a large reduction of design basis and beyond-design-basis accident source terms with concomitantly smaller dose to workers and the public. Therefore, NRC acceptance of iPWR containment aerosol natural deposition correlations will directly support the industry’s goal of reducing the Emergency Planning Zone (EPZ) for SMRs. Based on the results in this work, it is clear that thermophoresis is relatively unimportant for iPWRs. Gravitational settling is well understood, and may be the dominant process for a dry environment. Diffusiophoresis and enhanced

  3. Characterization of aerosol composition and sources in the greater Atlanta area by aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Ng, N. L.; Xu, L.; Suresh, S.; Weber, R. J. J.; Baumann, K.; Edgerton, E. S.

    2014-12-01

    An important and uncertain aspect of biogenic secondary organic aerosol (SOA) formation is that it is often associated with anthropogenic pollution tracers. Prior studies in Atlanta suggested that 70-80% of the carbon in water-soluble organic carbon (WSOC) is modern, yet it is well-correlated with the anthropogenic CO. In this study, we deployed a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) at multiple sites in different seasons (May 2012-February 2013) to characterize the sources and chemical composition of aerosols in the greater Atlanta area. This area in the SE US is ideal to investigate anthropogenic-biogenic interactions due to high natural and anthropogenic emissions. These extensive field studies are part of the Southeastern Center for Air Pollution and Epidemiology study (SCAPE). The HR-ToF-AMS is deployed at four sites (~ 3 weeks each) in rotation: Jefferson Street (urban), Yorkville (rural), roadside site (near Highway 75/85), and Georgia Tech site (campus), with the urban and rural sites being part of the SEARCH network. We obtained seven HR-ToF-AMS datasets in total. During the entire measurement period, the ACSM is stationary at the GIT site and samples continuously. We perform positive matrix factorization (PMF) analysis on the HR-ToF-AMS and ACSM data to deconvolve the OA into different components. While the diurnal cycle of the total OA is flat as what have been previously observed, the OA factors resolved by PMF analysis show distinctively different diurnal trends. We find that the "more-oxidized oxygenated OA" (MO-OOA) constitutes a major fraction of OA at all sites. In summer, OA is dominated by SOA, e.g., isoprene-OA and OOA with different degrees of oxidation. In contrary, biomass burning OA is more prominent in winter data. By comparing HR-ToF-AMS and ACSM data during the same sampling periods, we find that the aerosol time series are highly correlated, indicating the

  4. Sources and geographical origins of fine aerosols in Paris (France)

    NASA Astrophysics Data System (ADS)

    Bressi, M.; Sciare, J.; Ghersi, V.; Mihalopoulos, N.; Petit, J.-E.; Nicolas, J. B.; Moukhtar, S.; Rosso, A.; Féron, A.; Bonnaire, N.; Poulakis, E.; Theodosi, C.

    2013-12-01

    The present study aims at identifying and apportioning the major sources of fine aerosols in Paris (France) - the second largest megacity in Europe -, and determining their geographical origins. It is based on the daily chemical composition of PM2.5 characterised during one year at an urban background site of Paris (Bressi et al., 2013). Positive Matrix Factorization (EPA PMF3.0) was used to identify and apportion the sources of fine aerosols; bootstrapping was performed to determine the adequate number of PMF factors, and statistics (root mean square error, coefficient of determination, etc.) were examined to better model PM2.5 mass and chemical components. Potential Source Contribution Function (PSCF) and Conditional Probability Function (CPF) allowed the geographical origins of the sources to be assessed; special attention was paid to implement suitable weighting functions. Seven factors named ammonium sulfate (A.S.) rich factor, ammonium nitrate (A.N.) rich factor, heavy oil combustion, road traffic, biomass burning, marine aerosols and metals industry were identified; a detailed discussion of their chemical characteristics is reported. They respectively contribute 27, 24, 17, 14, 12, 6 and 1% of PM2.5 mass (14.7 μg m-3) on the annual average; their seasonal variability is discussed. The A.S. and A.N. rich factors have undergone north-eastward mid- or long-range transport from Continental Europe, heavy oil combustion mainly stems from northern France and the English Channel, whereas road traffic and biomass burning are primarily locally emitted. Therefore, on average more than half of PM2.5 mass measured in the city of Paris is due to mid- or long-range transport of secondary aerosols stemming from continental Europe, whereas local sources only contribute a quarter of the annual averaged mass. These results imply that fine aerosols abatement policies conducted at the local scale may not be sufficient to notably reduce PM2.5 levels at urban background sites in

  5. Sources and geographical origins of fine aerosols in Paris (France)

    NASA Astrophysics Data System (ADS)

    Bressi, M.; Sciare, J.; Ghersi, V.; Mihalopoulos, N.; Petit, J.-E.; Nicolas, J. B.; Moukhtar, S.; Rosso, A.; Féron, A.; Bonnaire, N.; Poulakis, E.; Theodosi, C.

    2014-08-01

    The present study aims at identifying and apportioning fine aerosols to their major sources in Paris (France) - the second most populated "larger urban zone" in Europe - and determining their geographical origins. It is based on the daily chemical composition of PM2.5 examined over 1 year at an urban background site of Paris (Bressi et al., 2013). Positive matrix factorization (EPA PMF3.0) was used to identify and apportion fine aerosols to their sources; bootstrapping was performed to determine the adequate number of PMF factors, and statistics (root mean square error, coefficient of determination, etc.) were examined to better model PM2.5 mass and chemical components. Potential source contribution function (PSCF) and conditional probability function (CPF) allowed the geographical origins of the sources to be assessed; special attention was paid to implement suitable weighting functions. Seven factors, namely ammonium sulfate (A.S.)-rich factor, ammonium nitrate (A.N.)-rich factor, heavy oil combustion, road traffic, biomass burning, marine aerosols and metal industry, were identified; a detailed discussion of their chemical characteristics is reported. They contribute 27, 24, 17, 14, 12, 6 and 1% of PM2.5 mass (14.7 μg m-3) respectively on the annual average; their seasonal variability is discussed. The A.S.- and A.N.-rich factors have undergone mid- or long-range transport from continental Europe; heavy oil combustion mainly stems from northern France and the English Channel, whereas road traffic and biomass burning are primarily locally emitted. Therefore, on average more than half of PM2.5 mass measured in the city of Paris is due to mid- or long-range transport of secondary aerosols stemming from continental Europe, whereas local sources only contribute a quarter of the annual averaged mass. These results imply that fine-aerosol abatement policies conducted at the local scale may not be sufficient to notably reduce PM2.5 levels at urban background sites in

  6. Source contributions to organic aerosol in the eastern United States

    NASA Astrophysics Data System (ADS)

    Lane, Timothy Edward

    Organic aerosols (OA) and elemental carbon (EC) are important components of atmospheric particulate matter (PM), potentially posing health hazards and contributing to global climate change. Secondary organic aerosol (SOA) is formed when condensable products from the oxidation of volatile organic compounds (VOCs) in the gas phase partition into the aerosol phase. Implementation of effective control strategies for organic PM2.5 (organic particles with diameters less than 2.5 mum) requires the quantification of the contribution of each source to the ambient OA and EC concentrations. The overall goal of this work is to determine which sources contribute the most to the organic aerosol concentrations across the eastern US. First, a source-resolved model is developed to predict the contribution of eight different sources to primary organic aerosol concentrations. Primary organic aerosol (OA) and elemental carbon (EC) concentrations are tracked for eight different sources: gasoline vehicles, non-road diesel vehicles, on-road diesel vehicles, biomass burning, wood burning, natural gas combustion, road dust, and all other sources. The results of the source-resolved model are compared to the results of chemical mass balance (CMB) models for Pittsburgh and multiple urban/rural sites from the Southeastern Aerosol Research and Characterization (SEARCH) network. Significant discrepancies exist between the source-resolved model and the CMB model predictions for several of the sources. There is strong evidence that the organic PM emissions from natural gas combustion are overestimated. Other similarities and discrepancies between the source-resolved model and the CMB model for primary OA and EC are discussed along with problems in the current emission inventory for certain sources. Next, the importance of isoprene as a source of SOA is determined using PMCAMx to predict the isoprene SOA concentration across the eastern US. Isoprene, the most abundant non-methane hydrocarbon

  7. HTGR Mechanistic Source Terms White Paper

    SciTech Connect

    Wayne Moe

    2010-07-01

    The primary purposes of this white paper are: (1) to describe the proposed approach for developing event specific mechanistic source terms for HTGR design and licensing, (2) to describe the technology development programs required to validate the design methods used to predict these mechanistic source terms and (3) to obtain agreement from the NRC that, subject to appropriate validation through the technology development program, the approach for developing event specific mechanistic source terms is acceptable

  8. Sources and source processes of organic nitrogen aerosols in the atmosphere

    NASA Astrophysics Data System (ADS)

    Erupe, Mark E.

    The research in this dissertation explored the sources and chemistry of organic nitrogen aerosols in the atmosphere. Two approaches were employed: field measurements and laboratory experiments. In order to characterize atmospheric aerosol, two ambient studies were conducted in Cache Valley in Northern Utah during strong winter inversions of 2004 and 2005. The economy of this region is heavily dependent on agriculture. There is also a fast growing urban population. Urban and agricultural emissions, aided by the valley geography and meteorology, led to high concentrations of fine particles that often exceeded the national ambient air quality standards. Aerosol composition was dominated by ammonium nitrate and organic species. Mass spectra from an aerosol mass spectrometer revealed that the organic ion peaks were consistent with reduced organic nitrogen compounds, typically associated with animal husbandry practices. Although no direct source characterization studies have been undertaken in Cache Valley with an aerosol mass spectrometer, spectra from a study at a swine facility in Ames, Iowa, did not show any evidence of reduced organic nitrogen species. This, combined with temporal and diurnal characteristics of organic aerosol peaks, was a pointer that the organic nitrogen species in Cache Valley likely formed from secondary chemistry. Application of multivariate statistical analyses to the organic aerosol spectra further supported this hypothesis. To quantify organic nitrogen signals observed in ambient studies as well as understand formation chemistry, three categories of laboratory experiments were performed. These were calibration experiments, smog chamber studies, and an analytical method development. Laboratory calibration experiments using standard calibrants indicated that quantifying the signals from organic nitrogen species was dependent on whether they formed through acid-base chemistry or via secondary organic aerosol pathway. Results from smog chamber

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

    NASA Astrophysics Data System (ADS)

    Dron, J.; El Haddad, I.; Temime-Roussel, B.; Jaffrezo, J.-L.; Wortham, H.; Marchand, N.

    2010-08-01

    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 (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-Ŕ 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%. Finally, examples of functional group mass

  10. Characteristics and sources of carbonaceous aerosols from Shanghai, China

    NASA Astrophysics Data System (ADS)

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

    2012-07-01

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

  11. Long-term Measurements of Submicrometer Aerosol Chemistry at the Southern Great Plains (SGP) Using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect

    Parworth, Caroline; Fast, Jerome D.; Mei, Fan; Shippert, Timothy R.; Sivaraman, Chitra; Tilp, Alison; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the U.S. Department of Energy’s Southern Great Plains (SGP) site are discussed. Over the period of 19 months (Nov. 20, 2010 – June 2012) highly time resolved (~30 min.) NR-PM1 data was recorded. Using this dataset the value-added product (VAP) of deriving organic aerosol components (OACOMP) is introduced. With this VAP, multivariate analysis of the measured organic mass spectral matrix can be performed on long term data to return organic aerosol (OA) factors that are associated with distinct sources, evolution processes, and physiochemical properties. Three factors were obtained from this VAP including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when nitrate increased due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations showed little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increased and were mainly associated with local fires. Isoprene and carbon monoxide emission rates were computed by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) to represent the spatial distribution of biogenic and anthropogenic sources, respectively. From this model there is evidence to support that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

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

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu Hemant

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

  13. AERONET-based models of smoke-dominated aerosol near source regions and transported over oceans, and implications for satellite retrievals of aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

    2014-10-01

    Smoke aerosols from biomass burning are an important component of the global aerosol system. Analysis of Aerosol Robotic Network (AERONET) retrievals of aerosol microphysical/optical parameters at 10 sites reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke observed at coastal/island AERONET sites also mostly lie within the range of variability at the near-source sites. Differences between sites tend to be larger than variability at an individual site, although optical properties for some sites in different regions can be quite similar. Across the sites, typical midvisible SSA ranges from ~ 0.95-0.97 (sites dominated by boreal forest or peat burning, typically with larger fine-mode particle radius and spread) to ~ 0.88-0.9 (sites most influenced by grass, shrub, or crop burning, typically smaller fine-mode particle radius and spread). The tropical forest site Alta Floresta (Brazil) is closer to this second category, although with intermediate SSA ~ 0.92. The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average midvisible SSA ~ 0.85. Sites with stronger absorption also tend to have stronger spectral gradients in SSA, becoming more absorbing at longer wavelengths. Microphysical/optical models are presented in detail so as to facilitate their use in radiative transfer calculations, including extension to UV (ultraviolet) wavelengths, and lidar ratios. One intended application is to serve as candidate optical models for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean often have insufficient absorption (i.e. too high SSA) to represent these biomass burning aerosols. The underestimates in satellite-retrieved AOD in smoke outflow regions, which have important consequences for applications of these satellite data sets, are consistent with

  14. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

    2004-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  15. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

    2003-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  16. Aerosols and their sources at Summit Greenland - First results of continuous size- and time-resolved sampling

    NASA Astrophysics Data System (ADS)

    VanCuren, Richard A.; Cahill, Thomas; Burkhart, John; Barnes, David; Zhao, Yongjing; Perry, Kevin; Cliff, Steven; McConnell, Joe

    2012-06-01

    An ongoing program to continuously collect time- and size-resolved aerosol samples from ambient air at Summit Station, Greenland (72.6 N, 38.5 W) is building a long-term data base to both record individual transport events and provide long-term temporal context for past and future intensive studies at the site. As a "first look" at this data set, analysis of samples collected from summer 2005 to spring 2006 demonstrates the utility of continuous sampling to characterize air masses over the ice pack, document individual aerosol transport events, and develop a long-term record. Seven source-related aerosol types were identified in this analysis: Asian dust, Saharan dust, industrial combustion, marine with combustion tracers, fresh coarse volcanic tephra, and aged volcanic plume with fine tephra and sulfate, and the well-mixed background "Arctic haze". The Saharan dust is a new discovery; the other types are consistent with those reported from previous work using snow pits and intermittent ambient air sampling during intensive study campaigns. Continuous sampling complements the fundamental characterization of Greenland aerosols developed in intensive field programs by providing a year-round record of aerosol size and composition at all temporal scales relevant to ice core analysis, ranging from individual deposition events and seasonal cycles, to a record of inter-annual variability of aerosols from both natural and anthropogenic sources.

  17. Sources and atmospheric transformations of semivolatile organic aerosols

    NASA Astrophysics Data System (ADS)

    Grieshop, Andrew P.

    Fine atmospheric particulate matter (PM2.5) is associated with increased mortality, a fact which led the EPA to promulgate a National Ambient Air Quality Standard (NAAQS) for PM2.5 in 1997. Organic material contributes a substantial portion of the PM2.5 mass; organic aerosols (OA) are either directly emitted (primary OA or POA) or formed via the atmospheric oxidation of volatile precursor compounds as secondary OA (SOA). The relative contributions of POA and SOA to atmospheric OA are uncertain, as are the contributions from various source classes (e.g. motor vehicles, biomass burning). This dissertation first assesses the importance of organic PM within the context of current US air pollution regulations. Most control efforts to date have focused on the inorganic component of PM. Although growing evidence strongly implicates OA, especially which from motor vehicles, in the health effects of PM, uncertain and complex source-receptor relationships for OA discourage its direct control for NAAQS compliance. Analysis of both ambient data and chemical transport modeling results indicate that OA does not play a dominant role in NAAQS violations in most areas of the country under current and likely future regulations. Therefore, new regulatory approaches will likely be required to directly address potential health impacts associated with OA. To help develop the scientific understanding needed to better regulate OA, this dissertation examined the evolution of organic aerosol emitted by combustion systems. The current conceptual model of POA is that it is non-volatile and non-reactive. Both of these assumptions were experimental investigated in this dissertation. Novel dilution measurements were carried out to investigate the gas-particle partitioning of OA at atmospherically-relevant conditions. The results demonstrate that POA from combustion sources is semivolatile. Therefore its gas-particle partitioning depends on temperature and atmospheric concentrations; heating and

  18. Carbonaceous aerosols from different tropical biomass burning sources

    NASA Astrophysics Data System (ADS)

    Cachier, Hélène; Brémond, Marie-Pierre; Buat-Ménard, Patrick

    1989-08-01

    FOLLOWING a repetitive pattern, biomass burning affects the intertropical belt on a continental scale during the dry season1. The importance of these anthropogenic activities with regard to carbonaceous-component emissions into the global atmosphere is now well recognized2-4. It has been suggested that large injections of black carbon aerosols from the Tropics are of potential importance for the radiative and chemical balance of the troposphere5-10. Studies on carbonaceous aerosols have indicated that, on an annual basis, the intensity of the emissions from tropical biomass burning could compare with that of emissions from fossil-fuel burning in industrial countries7,8. Also, results from combustion chamber experiments have determined the important range of the emission factor for both the organic and the black carbon components of the aerosol1-16. Following on from our earlier studies on total atmospheric particulate carbon (Ct) and isotopic composition (δ13C) (ref. 2), we now present new data on the black carbon content (Cb) of atmospheric particles sampled during the biomass-burning season in the wooden savannah of the Ivory Coast. The Cb/Ct ratio is generally lower than expected and highly variable. This variability indicates that there are drastic changes in source apportionment, which from our isotope studies may be ascribed to the variety of vegetation fuel and also to the mode of combustion. Therefore the Cb/Ct ratio can potentially discriminate biomass-burning emissions from different tropical ecosystems.

  19. Calculation of source terms for NUREG-1150

    SciTech Connect

    Breeding, R.J.; Williams, D.C.; Murfin, W.B.; Amos, C.N.; Helton, J.C.

    1987-10-01

    The source terms estimated for NUREG-1150 are generally based on the Source Term Code Package (STCP), but the actual source term calculations used in computing risk are performed by much smaller codes which are specific to each plant. This was done because the method of estimating the uncertainty in risk for NUREG-1150 requires hundreds of source term calculations for each accident sequence. This is clearly impossible with a large, detailed code like the STCP. The small plant-specific codes are based on simple algorithms and utilize adjustable parameters. The values of the parameters appearing in these codes are derived from the available STCP results. To determine the uncertainty in the estimation of the source terms, these parameters were varied as specified by an expert review group. This method was used to account for the uncertainties in the STCP results and the uncertainties in phenomena not considered by the STCP.

  20. Aerosols over Continental Portugal (1978-1993): their sources and an impact on the regional climate

    NASA Astrophysics Data System (ADS)

    Morozova, A. L.; Mironova, I. A.

    2014-12-01

    Understanding of aerosol sources which affect climate is an important problem open in front of scientists as well as policymakers. The role of aerosols in local climate variability depends on a~balance between aerosol absorbing and scattering particles as well as on variability of environmental conditions. In this paper we investigate variability of aerosol content (both absorbing and scattering UV radiation) over Continental Portugal in dependence on aerosol sources (volcanic eruptions, dust events, wildfires and anthropogenic pollution). The effect of the aerosol on the climate is studied analyzing their contribution to variations of temperature, sunshine duration and precipitation over Portuguese regions. The present analysis is based on a developed modern multiple regression technique allowing us to build the statistical correlation models to determine both the main local aerosol sources and aerosol's influence on the climate of the Continental Portugal during 1978-1993 time period. The analysis allows us to conclude that the main sources driving the variations of the aerosol content over studied locations are wildfires, mineral dust intrusions and anthropogenic pollution. The relations between the aerosol content variations and the atmospheric parameters depend on the level of urbanization of the studied region, the type of aerosol and the season. The most significant finding is the decrease of the daily temperature (and diurnal temperature range) related to the decrease of sunshine duration observed during the summer periods of increased content of the absorbing aerosols in the atmosphere.

  1. Regional versus Local Sources of aerosols over Cyprus

    NASA Astrophysics Data System (ADS)

    Kleanthous, Savvas; Nicolaou, Panagiota; Theodosi, Christina; Zarmpas, Pavlos; Christofides, Ioannis; Mihalopoulos, Nikolaos

    2013-04-01

    Long term monitoring of PM concentrations in Cyprus reported the occurrence of a significant number of PM exceedances above the limits set by EU legislation and point out the need for abatement strategies. To address these critical issues, mass and chemical composition of daily PM10 aerosol samples were collected at a suburban (Limassol; LIM RES), a natural background site (EMEP site, Ayia Marina) and an urban center (Nicosia, NIC TRA) from January 2010 to December 2010. By considering the chemical composition measured at EMEP as representative of the regional background, the contribution of local sources at both NIC TRA and LIM RES sites can be also estimated. In total, "local" ions account for 1.7 and 2.4 μg m-3, i.e 33 and 48% of the total ionic mass recorded in NIC TRA and LIM RES. Sea salt attained levels of 2.3 ± 1.2 μg m-3, 1.9 ± 1.3 μg m-3 and 3.5 ± 2.3 μg m-3, contributing up to 10, 7 and 11% of the PM10 mass measured at EMEP, NIC TRA and LIM RES, respectively. The local concentrations of OC and EC were equal to 3.3±1.1 μg m-3 and 3.2±1.3 μg m-3 for NIC TRA and 1.70±0.03 μg m-3 and 1.39±0.42 μg m-3 for LIM RES relative to the values measured at the EMEP site. The high EC concentrations in NIC TRA underline the major role of traffic-related emissions. As expected for the natural background site, OC/EC ratio equals 4.84, a strong indicator of secondary organic aerosol (SOA) formation. Whereas in the urban and suburban sites, the OC/EC ratio is lower ranging from 1.46 to 1.84, denoting significant influence from fossil fuel primary emissions in the studied areas. Considering that dust at EMEP is due to "regional" dust, the dust measured at both traffic related sites is the sum of "regional" and "local dust", the second most probably originating from soil dust and car/road abrasion. The "local dust" at NIC TRA and LIM RES accounted for 28% and 21% of the total PM10 mass, whilst regional dust at EMEP of 45%. The temporal variation of "local dust

  2. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2015-01-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9% and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/z 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ~10 years of meteorological, particle composition, and fire data.

  3. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2014-07-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9 and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/zs 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time (LST) when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ∼10 years of meteorological, particle composition, and fire data.

  4. Long-term impacts of aerosols on vertical development of cloud and precipitation

    SciTech Connect

    Li Z.; Liu Y.; Niu, F.; Fan, J.; Rosenfeld, D.; Ding, Y.

    2011-11-13

    Aerosols alter cloud density and the radiative balance of the atmosphere. This leads to changes in cloud microphysics and atmospheric stability, which can either suppress or foster the development of clouds and precipitation. The net effect is largely unknown, but depends on meteorological conditions and aerosol properties. Here, we examine the long-term impact of aerosols on the vertical development of clouds and rainfall frequencies, using a 10-year dataset of aerosol, cloud and meteorological variables collected in the Southern Great Plains in the United States. We show that cloud-top height and thickness increase with aerosol concentration measured near the ground in mixed-phase clouds-which contain both liquid water and ice-that have a warm, low base. We attribute the effect, which is most significant in summer, to an aerosol-induced invigoration of upward winds. In contrast, we find no change in cloud-top height and precipitation with aerosol concentration in clouds with no ice or cool bases. We further show that precipitation frequency and rain rate are altered by aerosols. Rain increases with aerosol concentration in deep clouds that have a high liquid-water content, but declines in clouds that have a low liquid-water content. Simulations using a cloud-resolving model confirm these observations. Our findings provide unprecedented insights of the long-term net impacts of aerosols on clouds and precipitation.

  5. SOURCE TERMS FOR HLW GLASS CANISTERS

    SciTech Connect

    J.S. Tang

    2000-08-15

    This calculation is prepared by the Monitored Geologic Repository (MGR) Waste Package Design Section. The objective of this calculation is to determine the source terms that include radionuclide inventory, decay heat, and radiation sources due to gamma rays and neutrons for the high-level radioactive waste (HLW) from the, West Valley Demonstration Project (WVDP), Savannah River Site (SRS), Hanford Site (HS), and Idaho National Engineering and Environmental Laboratory (INEEL). This calculation also determines the source terms of the canister containing the SRS HLW glass and immobilized plutonium. The scope of this calculation is limited to source terms for a time period out to one million years. The results of this calculation may be used to carry out performance assessment of the potential repository and to evaluate radiation environments surrounding the waste packages (WPs). This calculation was performed in accordance with the Development Plan ''Source Terms for HLW Glass Canisters'' (Ref. 7.24).

  6. Sub-Antarctic marine aerosol: significant contributions from biogenic sources

    NASA Astrophysics Data System (ADS)

    Schmale, J.; Schneider, J.; Nemitz, E.; Tang, Y. S.; Dragosits, U.; Blackall, T. D.; Trathan, P. N.; Phillips, G. J.; Sutton, M.; Braban, C. F.

    2013-03-01

    Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea salt sulfate 2% nitrate, 7% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea salt signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acids/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 40%), a sea salt OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (C : N ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea salt aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated to sea

  7. Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

    NASA Astrophysics Data System (ADS)

    Schmale, J.; Schneider, J.; Nemitz, E.; Tang, Y. S.; Dragosits, U.; Blackall, T. D.; Trathan, P. N.; Phillips, G. J.; Sutton, M.; Braban, C. F.

    2013-09-01

    Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 41%), a sea spray OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated

  8. Characteristics and sources of carbonaceous aerosols from Shanghai, China

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

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

  9. Relating Aerosol Absorption due to Soot, Organic Carbon, and Dust to Emission Sources Determined from In-situ Chemical Measurements

    SciTech Connect

    Cazorla, Alberto; Bahadur, R.; Suski, Kaitlyn; Cahill, John F.; Chand, Duli; Schmid, Beat; Ramanathan, V.; Prather, Kimberly

    2013-09-17

    Estimating the aerosol contribution to the global or regional radiative forcing can take advantage of the relationship between the spectral aerosol optical properties and the size and chemical composition of aerosol. Long term global optical measurements from observational networks or satellites can be used in such studies, and using in-situ chemical mixing state measurements can help us to constrain the limitations of such an estimation. In this study, the Absorption Ångström Exponent (AAE) and the Scattering Ångström Exponent (SAE) are used to develop a new methodology for deducing chemical speciation based on wavelength dependence of the optical properties. In addition, in-situ optical properties and single particle chemical composition measured during three aircraft field campaigns are combined in order to validate the methodology for the estimation of aerosol composition using spectral optical properties. Results indicate a dominance of mixed types in the classification leading to an underestimation of the primary sources, however secondary sources are better classified. The distinction between carbonaceous aerosols from fossil fuel and biomass burning origins is not clear. On the other hand, the knowledge of the aerosol sources in California from chemical studies help to identify other misclassification such as the dust contribution.

  10. Aerosols over continental Portugal (1978-1993): their sources and an impact on the regional climate

    NASA Astrophysics Data System (ADS)

    Morozova, A. L.; Mironova, I. A.

    2015-06-01

    Understanding of aerosol sources that affect climate is an ongoing problem facing scientists as well as policymakers. The role of aerosols in local climate variability depends on a balance between light absorbing and scattering particles as well as on variability of environmental conditions. In this paper we investigate variability of aerosol content (both absorbing and scattering ultraviolet radiation) over continental Portugal in connection with aerosol sources (volcanic eruptions, dust events, wildfires and anthropogenic pollution). The effect of the aerosol on the climate is studied analyzing their contribution to variations of temperature, pressure, sunshine duration and precipitation over Portuguese regions. The present analysis is based on a developed modern multiple regression technique allowing us to build the statistical correlation models to determine both the main local aerosol sources and aerosol's influence on the climate of continental Portugal during 1978-1993. The analysis allows us to conclude that the main sources driving the variations of the aerosol content over studied locations are wildfires, mineral dust intrusions and anthropogenic pollution. The relations between the aerosol content variations and the atmospheric parameters depend on the level of urbanization of the studied region, the type of aerosol and the season. The most significant finding is the decrease of the daily maximum temperature (and diurnal temperature range) related to the decrease of sunshine duration observed during the summer periods of increased content of the absorbing aerosols in the atmosphere.

  11. Sensitive glow discharge ion source for aerosol and gas analysis

    DOEpatents

    Reilly, Peter T. A.

    2007-08-14

    A high sensitivity glow discharge ion source system for analyzing particles includes an aerodynamic lens having a plurality of constrictions for receiving an aerosol including at least one analyte particle in a carrier gas and focusing the analyte particles into a collimated particle beam. A separator separates the carrier gas from the analyte particle beam, wherein the analyte particle beam or vapors derived from the analyte particle beam are selectively transmitted out of from the separator. A glow discharge ionization source includes a discharge chamber having an entrance orifice for receiving the analyte particle beam or analyte vapors, and a target electrode and discharge electrode therein. An electric field applied between the target electrode and discharge electrode generates an analyte ion stream from the analyte vapors, which is directed out of the discharge chamber through an exit orifice, such as to a mass spectrometer. High analyte sensitivity is obtained by pumping the discharge chamber exclusively through the exit orifice and the entrance orifice.

  12. Assessing sensitivity of source term estimation

    NASA Astrophysics Data System (ADS)

    Long, Kerrie J.; Haupt, Sue Ellen; Young, George S.

    2010-04-01

    Source term estimation algorithms compute unknown atmospheric transport and dispersion modeling variables from concentration observations made by sensors in the field. Insufficient spatial and temporal resolution in the meteorological data as well as inherent uncertainty in the wind field data make source term estimation and the prediction of subsequent transport and dispersion extremely difficult. This work addresses the question: how many sensors are necessary in order to successfully estimate the source term and meteorological variables required for atmospheric transport and dispersion modeling? The source term estimation system presented here uses a robust optimization technique - a genetic algorithm (GA) - to find the combination of source location, source height, source strength, surface wind direction, surface wind speed, and time of release that produces a concentration field that best matches the sensor observations. The approach is validated using the Gaussian puff as the dispersion model in identical twin numerical experiments. The limits of the system are tested by incorporating additive and multiplicative noise into the synthetic data. The minimum requirements for data quantity and quality are determined by an extensive grid sensitivity analysis. Finally, a metric is developed for quantifying the minimum number of sensors necessary to accurately estimate the source term and to obtain the relevant wind information.

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  14. Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

    NASA Astrophysics Data System (ADS)

    Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

    2015-12-01

    The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which

  15. Investigating water soluble organic aerosols: Sources and evolution

    NASA Astrophysics Data System (ADS)

    Hecobian, Arsineh N.

    Many studies are being conducted on the different properties of organic aerosols (OA-s) as it is first emitted into the atmosphere and the consequent changes in these characteristics as OA-s age and secondary organic aerosol (SOA) is produced and in turn aged. This thesis attempts to address some of the significant and emerging issues that deal with the formation and transformation of water-soluble organic aerosols in the atmosphere. First, a proven method for the measurement of gaseous sulfuric acid, negative ion chemical ionization mass spectrometry (CIMS), has been modified for fast and sensitive measurements of particulate phase sulfuric acid (i.e. sulfate). The modifications implemented on this system have also been the subject of preliminary verifications for measurements of aerosol phase oxalic acid (an organic acid). Second, chemical and physical characteristics of a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS experiment are presented here. A statistical summary of the emission (or enhancement) ratios relative to carbon monoxide is presented for various gaseous and aerosol species. Extensive investigations of fire plume evolutions were undertaken during the second part of this field campaign. For four distinct Boreal fires, where plumes were intercepted by the aircraft over a wide range of down-wind distances, emissions of various compounds and the effect of aging on them were investigated in detail. No clear evidence of production of secondary compounds (e.g., WSOC and OA) was observed. High variability in emissions between the different plumes may have obscured any clear evidence of changes in the mass of various species with increasing plume age. Also, the lack if tropospheric oxidizing species (e.g., O3 and OH) may have contributed to the lack of SOA formation. Individual intercepts of smoke plumes in this study were segregated by source regions. The normalized excess mixing

  16. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations of the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  17. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    DOE PAGESBeta

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

  18. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    NASA Astrophysics Data System (ADS)

    Parworth, Caroline; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Tilp, Alison; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ∼30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations of the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  19. Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

    NASA Astrophysics Data System (ADS)

    Elser, Miriam; Bozzetti, Carlo; El-Haddad, Imad; Maasikmets, Marek; Teinemaa, Erik; Richter, Rene; Wolf, Robert; Slowik, Jay G.; Baltensperger, Urs; Prévôt, André S. H.

    2016-06-01

    Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero ≤ 2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background

  20. A Study of Aerosol Effect on Marine Water Clouds with Long-term Satellite Climate Data Records

    NASA Astrophysics Data System (ADS)

    Zhao, X.; Heidinger, A. K.; Walther, A.

    2015-12-01

    Cloud microphysical structures and properties provide a critical link between the energy and hydrological cycles of Earth's climate system. A change of cloud microphysical properties related to anthropogenic activities may result in distressing climate consequence and changes. Since atmospheric aerosol is the major source of cloud condensation nuclei (CNN) that is critical for the formation of cloud microphysical structures and properties, aerosol changes due to anthropogenic emissions will result in the modification of CCN and cloud microphysical properties and eventually cause the changes of Earth's climate. In this study, we will investigate the effect of aerosol on the microphysical properties, including cloud particle effective radius, cloud water path, and cloud optical depth, of marine stratus clouds by using more than 30-years climate data records (CDRs) of aerosols and clouds derived from NOAA operational AVHRR satellite observations. The correlation between satellite derived cloud and aerosol microphysical parameters will be determined and the statistics significance will be examined using the long-term AVHRR satellite CDRs.

  1. Subsurface Shielding Source Term Specification Calculation

    SciTech Connect

    S.Su

    2001-04-12

    The purpose of this calculation is to establish appropriate and defensible waste-package radiation source terms for use in repository subsurface shielding design. This calculation supports the shielding design for the waste emplacement and retrieval system, and subsurface facility system. The objective is to identify the limiting waste package and specify its associated source terms including source strengths and energy spectra. Consistent with the Technical Work Plan for Subsurface Design Section FY 01 Work Activities (CRWMS M&O 2001, p. 15), the scope of work includes the following: (1) Review source terms generated by the Waste Package Department (WPD) for various waste forms and waste package types, and compile them for shielding-specific applications. (2) Determine acceptable waste package specific source terms for use in subsurface shielding design, using a reasonable and defensible methodology that is not unduly conservative. This calculation is associated with the engineering and design activity for the waste emplacement and retrieval system, and subsurface facility system. The technical work plan for this calculation is provided in CRWMS M&O 2001. Development and performance of this calculation conforms to the procedure, AP-3.12Q, Calculations.

  2. Radionuclides reveal age and source of aerosols collected over central North Atlantic

    NASA Astrophysics Data System (ADS)

    Zhang, B.; Urban, N. R.; Perlinger, J. A.; Owen, R. C.; China, S.; Mazzoleni, C.; Mazzoleni, L. R.

    2014-12-01

    Aerosol filter samples were collected daily during summer 2013, at the Pico Mountain Observatory (PMO, 38.47°N, 28.40°W, 2,225 m a.s.l.), Azores Islands. PMO monitors free troposphere air and aerosols transported from neighboring continents; North America has the most frequent influence due to predominantly westerly winds in mid-latitude regions, while aerosols from Europe and Africa are sampled occasionally. The residence time during long-range transport in the atmosphere has a critical impact on aerosol chemical and physical properties, and it can be estimated by measuring activities of radionuclides attached to aerosols. 210Pb (t1/2 = 22.1 years) and 210Po (t1/2 = 138 days) are daughter nuclides in the decay chain of 222Rn, an inert gas species produced throughout the Earth's crust and emitted into the atmosphere. Due to different rates of decay, the activity ratio of 210Po to 210Pb can be used to estimate atmospheric residence times of the carrier aerosols. 210Po activity counting of 58 samples was conducted to investigate aerosol residence times in this study. 210Po activity was measured twice serially for each aerosol sample to predict the initial activity of 210Po on the sampling date and the activity of very slowly decaying 210Pb. Aerosol ages calculated by the activity ratio of 210Po to 210Pb were compared with air tracer ages simulated using the FLEXible PARTicle dispersion model (FLEXPART) and studied together with aerosol particle physical properties. The activity of terrestrial radionuclides per unit of aerosol mass can also reveal source information of the aerosols. FLEXPART backward trajectories will be used to verify correlations between source regions and activity of radionuclides in aerosols. In previous research related to long-range atmospheric transport to PMO, FLEXPART has proven to be reliable in identifying upwind source regions.

  3. Cloud Nucleating Properties of Aerosols During TexAQS - GoMACCS 2006: Influence of Aerosol Sources, Composition, and Size

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.; Onasch, T. B.; Alllan, J. D.; Worsnop, D.

    2006-12-01

    TexAQS - GoMACCS 2006 was conducted from July to September 2006 in the Gulf of Mexico and Houston Ship Channel to investigate sources and processing of gas and particulate phase species and to determine their impact on regional air quality and climate. As part of the experiment, the NOAA R.V. Ronald H. Brown transited from Charleston, S.C. to the study region. The ship was equipped with a full compliment of gas and aerosol instruments. To determine the cloud nucleating properties of aerosols, measurements were made of the aerosol number size distribution, aerosol chemical composition, and cloud condensation nuclei (CCN) concentration at five supersaturations. During the transit and over the course of the experiment, a wide range of aerosol sources and types was encountered. These included urban and industrial emissions from the S.E. U.S. as the ship left Charleston, a mixture of Saharan dust and marine aerosol during the transit around Florida and across the Gulf of Mexico, urban emissions from Houston, and emissions from the petrochemical industries, oil platforms, and marine vessels in the Gulf coast region. Highest activation ratios (ratio of CCN to total particle number concentration at 0.4 percent supersaturation) were measured in anthropogenic air masses when the aerosol was composed primarily of ammonium sulfate salts and in marine air masses with an aerosol composed of sulfate and sea salt. A strong gradient in activation ratio was measured as the ship moved from the Gulf of Mexico to the end of the Houston Ship Channel (values decreasing from about 0.8 to less than 0.1) and the aerosol changed from marine to industrial. The activation ratio under these different regimes in addition to downwind of marine vessels and oil platforms will be discussed in the context of the aerosol size distribution and chemical composition. The discussion of composition will include the organic mass fraction of the aerosol, the degree of oxidation of the organics, and the water

  4. Long-term variations in the South Asian monsoon annual cycle: the role of regional anthropogenic aerosol forcing

    NASA Astrophysics Data System (ADS)

    Bollasina, Massimo; Ming, Yi

    2013-04-01

    Detection and attribution of long-term variations of the South Asian monsoon is of extreme importance. Indeed, even small changes in the onset and duration of the monsoon season or in the spatial distribution of the seasonal mean precipitation may severely impact agriculture, health, water availability, ecosystems, and economy for a substantial fraction of the world's population. In the past decades emissions of aerosols have dramatically increased over South Asia due to rapid urbanization and population growth. As a result, the study of the impact of anthropogenic aerosols on the monsoon has recently emerged as one of the topics of highest priority in the scientific community. This study makes use of a state-of-the-art coupled climate model, the GFDL CM3, to investigate two aspects of the aerosol influence on the 20th-century changes in the monsoon. The model has fully-interactive aerosols and a representation of both direct and indirect effects. Aerosols are responsible for the advancement of the monsoon onset over India, leading, in agreement with observations, to enhanced precipitation in June over most parts of the subcontinent. Our experiments show that the earlier onset is preceded in early spring by a strong aerosol forcing over the Bay of Bengal and Indonesia and associated atmospheric circulation anomalies. The latter triggers thermodynamical changes over the northwestern part of the Subcontinent in May and June, including enhanced surface heating, which in turn drive the movement of the monsoon to the west. We also performed historical experiments with time-evolving radiative forcings aimed at isolating the contribution of regional versus remote anthropogenic aerosol emissions on the observed 20th century widespread drying of the Indian monsoon. Indian-only aerosol sources are found to play a predominant role in generating suppressed rainfall over the subcontinent, especially during early summer. Remote aerosols contribute, although in a minor way, to

  5. Blowing Snow - A Major Source of Aerosol in the Polar Regions?

    NASA Astrophysics Data System (ADS)

    Kalnajs, L.; DeCarlo, P. F.; Giordano, M.; Davis, S. M.; Deshler, T.; Johnson, A.; Goetz, J. D.; Mukherjee, A. D.; Slater, A. G.

    2015-12-01

    Sea salt aerosol is the dominant aerosol component in unpolluted Polar Regions, particularly in the sea ice zone. In the lower latitude liquid ocean, wave action and bubble bursting is thought to be the main mechanism for sea salt aerosol production. However there is growing evidence that in the Polar Regions, particularly near sea ice, that the sublimation of wind lofted salty snow may be a dominant source of sea salt aerosol. An extensive set of aerosol sizing and compositional measurements was made at sea ice location near Ross Island, Antarctica during two field measurement campaigns - a summer campaign in 2014 and late winter campaign in 2015. Sizing measurements from both open and closed path aerosol instruments, and compositional measurements from an Aerosol Mass Spectrometer suggest that there is a significant enhancement in both super and sub micron aerosol associated with high wind events and blowing snow in the boundary layer. While the composition of this aerosol indicates that it is primarily of marine origin, the ratios of the major sea salt ions suggest that processing in the snow pack significantly modifies the aerosol. This alternate sea salt aerosol production mechanism could have significant impact on the modeling of tropospheric halogen chemistry and on the interpretation of sea salt-based proxies in the ice core record.

  6. The Stratospheric Aerosol and Gas Experiment III - International Space Station: Extending Long-Term Ozone and Aerosol Observations (Invited)

    NASA Astrophysics Data System (ADS)

    Eckman, R.; Zawodny, J. M.; Cisewski, M.; Gasbarre, J.; Flittner, D. E.; Hill, C.; Roell, M.; Moore, J. R.; Hernandez, G.; McCormick, M. P.

    2013-12-01

    The Stratospheric Aerosol and Gas Experiment III - International Space Station (SAGE III on ISS) will extend the global measurements of vertical profiles of ozone, aerosols, water vapor, nitrogen dioxide, and other trace gases begun with SAGE I in 1979, enabling the detection of long-term trends. SAGE III on ISS is the fourth in a series of instruments developed for monitoring these constituents in the stratosphere and troposphere. The SAGE III instrument is a moderate resolution spectrometer covering wavelengths from 290 nm to 1550 nm, using the heritage occultation technique, utilizing both the sun and the moon. Launch to ISS is planned for early 2015 aboard a Falcon 9 spacecraft. SAGE III will investigate the spatial and temporal variability of the measured species in order to determine their role in climatological processes, biogeochemical cycles, the hydrologic cycle, and atmospheric chemistry. It will characterize tropospheric, as well as stratospheric aerosols and upper tropospheric and stratospheric clouds, and investigate their effects on the Earth's environment including radiative, microphysical, and chemical interactions. The multi-decadal SAGE ozone and aerosol data sets have undergone intense scrutiny and are the international standard for accuracy and stability. SAGE data have been used to monitor the effectiveness of the Montreal Protocol. Amongst its key objectives will be to assess the state of the recovery in the distribution of ozone, to reestablish the aerosol measurements needed by both climate and ozone models, and to gain further insight into key processes contributing to ozone and aerosol variability. The ISS is ideal for Earth observing experiments; its mid-inclination orbit allows for a large range in latitude sampling and nearly continuous communications with payloads. In this presentation, we describe the SAGE III on ISS mission, its implementation, current status, and concentrate on its key science objectives.

  7. Concentrations and sources of metals in the Antarctic Peninsula aerosol

    SciTech Connect

    Dick, A.L. )

    1991-07-01

    Aerosol samples were collected at a remote site near the east coast of the Antarctic Peninsula during the austral summer of 1984/85. Filter samples were analyzed for Al (as a crustal reference element), marine cations (Na, K, and Ca), heavy metals (Cd, Cu, Pb, and Zn), and sulfate using atomic absorption spectrometry, isotope dilution mass spectrometry, neutron activation analysis, and ion chromatography. Ultraclean sample collection and analysis procedures used to avoid sample contamination are described in detail here. Mean concentrations of heavy metals were found to be: Cd, 0.06 pg m{sup {minus}3}; Cu, 1.0 pg m{sup {minus}3}; Pb, 4.7 pg m{sup {minus}3}; and Zn, 6.1 pg m{sup {minus}3}. These are the lowest concentrations yet determined in the troposphere, but for Pb and Zn they still indicate a significant enrichment over expected crustal concentrations. For these elements, estimated marine and volcanic contributions cannot account for this excess and suggest pollution as the dominant source even at this remote location. For Cd and Cu a dominant anthropogenic source cannot be ruled out, although current estimated of crustal, marine, a volcanic emissions could account for levels determined.

  8. Effects of aerosol sources and chemical compositions on cloud drop sizes and glaciation temperatures

    NASA Astrophysics Data System (ADS)

    Zipori, Assaf; Rosenfeld, Daniel; Tirosh, Ofir; Teutsch, Nadya; Erel, Yigal

    2015-09-01

    The effect of aerosols on cloud properties, such as its droplet sizes and its glaciation temperatures, depends on their compositions and concentrations. In order to examine these effects, we collected rain samples in northern Israel during five winters (2008-2011 and 2013) and determined their chemical composition, which was later used to identify the aerosols' sources. By combining the chemical data with satellite-retrieved cloud properties, we linked the aerosol types, sources, and concentrations with the cloud glaciation temperatures (Tg). The presence of dust increased Tg from -26°C to -12°C already at relatively low dust concentrations. This result is in agreement with the conventional wisdom that desert dust serves as good ice nuclei (INs). With higher dust concentrations, Tg saturated at -12°C, even though cloud droplet sizes decreased as a result of the cloud condensation nucleating (CCN) activity of the dust. Marine air masses also encouraged freezing, but in this case, freezing was enhanced by the larger cloud droplet sizes in the air masses (caused by low CCN concentrations) and not by IN concentrations or by aerosol type. An increased fraction of anthropogenic aerosols in marine air masses caused a decrease in Tg, indicating that these aerosols served as poor IN. Anthropogenic aerosols reduced cloud droplet sizes, which further decreased Tg. Our results could be useful in climate models for aerosol-cloud interactions, as we investigated the effects of aerosols of different sources on cloud properties. Such parameterization can simplify these models substantially.

  9. Multi-year investigations of aerosols from an island station, Port Blair, in the Bay of Bengal: climatology and source impacts

    NASA Astrophysics Data System (ADS)

    Naseema Beegum, S.; Krishna Moorthy, K.; Gogoi, Mukunda M.; Babu, S. Suresh; Pandey, S. K.

    2012-08-01

    Long-term measurements of spectral aerosol optical depth (AOD) using multi-wavelength solar radiometer (MWR) for a period of seven years (from 2002 to 2008) from the island location, Port Blair (11.63° N, 92.7° E, PBR) in the Bay of Bengal (BoB), along with the concurrent measurements of the size distribution of near-surface aerosols, have been analyzed to delineate the climatological features of aerosols over eastern BoB. In order to identity the contribution of different aerosol types from distinct sources, concentration weighted trajectory (CWT) analysis has been employed. Climatologically, AODs increase from January to reach peak value of ~0.4 (at 500 nm) in March, followed by a weak decrease towards May. Over this general pattern, significant modulations of intra-seasonal time scales, caused by the changes in the relative strength of distinctively different sources, are noticed. The derivative (α') of the Angstrom wavelength exponent α in the wavelength domain, along with CWT analysis, are used to delineate the different important aerosol types that influence this remote island. Corresponding changes in the aerosol size distributions are inferred from the numerical inversion of the spectral AODs as well from (surface) measurements. The analyses revealed that advection plays a major role in modifying the aerosol properties over the remote island location, the potential sources contributing to the accumulation mode (coarse mode) aerosols over eastern BoB being the East Asia and South China regions (Indian mainland and the oceanic regions).

  10. AEROSOL SOURCE CHARACTERIZATION STUDY IN MIAMI, FLORIDA. TRACE ELEMENT ANALYSIS

    EPA Science Inventory

    Aerosol in Miami, Florida was sampled in June 1975 to better characterize the aerosol in an urban environment devoid of heavy industry. The three sampling sites selected were an area with light industrial activity, one with heavy commercial activity, and a sparsely populated resi...

  11. “A significant source of isoprene aerosol controlled by acidity”

    EPA Science Inventory

    “A significant source of isoprene aerosol controlled by acidity” by Pye et al.Abstract: Isoprene is a significant contributor to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, CMAQ provides explicit p...

  12. Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

    EPA Science Inventory

    ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

  13. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-01-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the Southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8±8.4 μg m-3 and 13.5±8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva)~200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  14. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-07-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m-3 and 13.5 ± 8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  15. BWR Source Term Generation and Evaluation

    SciTech Connect

    J.C. Ryman

    2003-07-31

    This calculation is a revision of a previous calculation (Ref. 7.5) that bears the same title and has the document identifier BBAC00000-01717-0210-00006 REV 01. The purpose of this revision is to remove TBV (to-be-verified) -41 10 associated with the output files of the previous version (Ref. 7.30). The purpose of this and the previous calculation is to generate source terms for a representative boiling water reactor (BWR) spent nuclear fuel (SNF) assembly for the first one million years after the SNF is discharged from the reactors. This calculation includes an examination of several ways to represent BWR assemblies and operating conditions in SAS2H in order to quantify the effects these representations may have on source terms. These source terms provide information characterizing the neutron and gamma spectra in particles per second, the decay heat in watts, and radionuclide inventories in curies. Source terms are generated for a range of burnups and enrichments (see Table 2) that are representative of the waste stream and stainless steel (SS) clad assemblies. During this revision, it was determined that the burnups used for the computer runs of the previous revision were actually about 1.7% less than the stated, or nominal, burnups. See Section 6.6 for a discussion of how to account for this effect before using any source terms from this calculation. The source term due to the activation of corrosion products deposited on the surfaces of the assembly from the coolant is also calculated. The results of this calculation support many areas of the Monitored Geologic Repository (MGR), which include thermal evaluation, radiation dose determination, radiological safety analyses, surface and subsurface facility designs, and total system performance assessment. This includes MGR items classified as Quality Level 1, for example, the Uncanistered Spent Nuclear Fuel Disposal Container (Ref. 7.27, page 7). Therefore, this calculation is subject to the requirements of the

  16. Aerosol structure and vertical distribution in a multi-source dust region.

    PubMed

    Zhang, Jie; Zhang, Qiang; Tang, Congguo; Han, Yongxiang

    2012-01-01

    The vertical distribution of aerosols was directly observed under various atmospheric conditions in the free troposphere using surface micro-pulse lidar (MPL4) at the Zhangye Station (39.08 degrees N, 100.27 degrees E) in western China in the spring of 2008. The study shows that the aerosol distribution over Zhangye can be vertically classified into upper, middle and lower layers with altitudes of 4.5 to 9 km, 2.5 to 4.5 km, and less than 2.5 km, respectively. The aerosol in the upper layer originated from the external sources at higher altitude regions, from far desert regions upwind of Zhangye or transported from higher atmospheric layers by free convection, and the altitude of this aerosol layer decreased with time; the aerosols in the middle and lower layers originated from both external and local sources. The aerosol extinction coefficients in the upper and lower layers decreased with altitude, whereas the coefficient in the middle layer changed only slightly, which suggests that aerosol mixing occurs in the middle layer. The distribution of aerosols with altitude has three features: a single peak that forms under stable atmospheric conditions, an exponential decrease with altitude that occurs under unstable atmospheric conditions, and slight change in the mixed layer. Due to the impact of the top of the atmospheric boundary layer, the diurnal variation in the aerosol extinction coefficient has a single peak, which is higher in the afternoon and lower in the morning. PMID:23513689

  17. Sources markers in aerosols, oceanic particles and sediments

    NASA Astrophysics Data System (ADS)

    Saliot, A.

    2009-02-01

    This review presents some diagnostic criteria used for identifying and quantifying terrestrial organic matter inputs to the ocean. Coupled to the isotopic composition of total organic carbon, the analysis of stable biomarkers permits to trace higher plant contributions in aerosols, dusts, sedimenting particles and dissolved phase in the water column and ultimately in recent and ancient sediments and soils. Some applications are presented, based on the analysis of n-alkyl compounds by a combination of gas chromatography and mass spectrometry (n-alkanes, n-alkanols, n-alkanoic acids and wax esters). Another approach has been developed using the analysis of macromolecular compounds present in higher plants. Abundances of the phenolic compounds from lignin, benzene carboxylic acids obtained during cupric oxide oxidation, Curie pyrolysis are used to characterise terrestrial organic matter sources and inputs. Finally due to the importance of biomass burning in continent-ocean transfers, biomarkers are presented in the polycyclic aromatic hydrocarbon class and for monosaccharide derivatives from the breakdown of cellulose.

  18. In situ Measurements of Absorbing Aerosols from Urban Sources, in Maritime Environments and during Biomass Combustion

    NASA Astrophysics Data System (ADS)

    Mazzoleni, C.; Manvendra, D.; Chylek, P.; Arnott, P.

    2006-12-01

    Absorbing aerosols have important but still ill quantified effects on climate, visibility, cloud processes, and air quality. The compilation of aerosol scattering and absorption databases from reliable measurements is essential to reduce uncertainties in these inter-linked research areas. The atmospheric radiative balance for example, is modeled using the aerosol single scattering albedo (ratio of scattering to scattering plus absorption, SSA) as a fundamental input parameter in climate models. Sulfate aerosols with SSA values close to 1 scatter solar radiation resulting in a negative radiative forcing. However aerosol SSA values less than 1 are common when combustion processes are contributing to the aerosol sources. Absorbing aerosols directly heat the atmosphere and reduce the solar radiation at the surface. Currently, the net global anthropogenic aerosol direct radiative forcing is estimated to be around -0.5W m-2 with uncertainty of about 80% largely due to lack of understanding of SSA of sulfate-organic-soot aerosols. We present a rapidly expanding data set of direct in situ aerosol absorption and scattering measurements performed since June 2005 by photoacoustic instrument (at 781 and 870 nm), with integrated a total scattering sensor, during numerous field campaigns. Data have been collected over a wide range of aerosol sources, local environments and anthropogenic activities. Airborne measurements were performed in marine stratus off shore of the California coast and in cumulus clouds and clear air in the Houston, TX area; ground-based measurements have been performed in many locations in Mexico City; while laboratory measurements have been collected during a controlled combustion experiment of many different biomass fuels. The large dynamic range of aerosol types and conditions from these different field campaigns will be integrated to help quantify the SSA values, their variability, and their implications on the radiative forcing of climate.

  19. Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy.

    PubMed

    Decesari, Stefano; Mircea, Mihaiela; Cavalli, Fabrizia; Fuzzi, Sandro; Moretti, Fabio; Tagliavini, Emilio; Facchini, Maria Cristina

    2007-04-01

    The functional group compositions of atmospheric aerosol water-soluble organic compoundswere obtained employing proton nuclear magnetic resonance (1H NMR) spectroscopy in a series of recent experiments in several areas of the world characterized by different aerosol sources and pollution levels. Here, we discuss the possibility of using 1H NMR functional group distributions to identifythe sources of aerosol in the different areas. Despite the limited variability of functional group compositions of atmospheric aerosol samples, characteristic 1H NMR fingerprints were derived for three major aerosol sources: biomass burning, secondary formation from anthropogenic and biogenic VOCs, and emission from the ocean. The functional group patterns obtained in areas characterized by one of the above dominant source processes were then compared to identify the dominant sources for samples coming from mixed sources. This analysis shows that H NMR spectroscopy can profitably be used as a valuable tool for aerosol source identification. In addition, compared to other existing methodologies, it is able to relate the source fingerprints to integral chemical properties of the organic mixtures, which determine their reactivity and their physicochemical properties and ultimately the fate of the organic particles in the atmosphere. PMID:17438803

  20. Characterization of marine boundary layer aerosol from North Atlantic and European sources: Physical and chemical properties and climate forcing parameters

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike

    This thesis focuses on aerosol properties measured in Southwestern Portugal during the second Aerosol Characterization Experiment. Fundamental aerosol physical properties such as particle size distribution and hygroscopic properties are related to possible sources and aerosol transformation processes. From these fundamental properties we derive aerosol properties that are important for aerosol forcing of climate. First, a new method for calculating CCN spectra is proposed in this work and tested using sensitivity studies and comparisons to direct measurements. The measured and calculated CCN spectra differ on average by 30%, which at small supersaturations is similar to the measurement uncertainties. Second, aerosol number to volume ratios (R) are calculated and the fact that values of R are relatively constrained is explained based on observed correlations between size distribution parameters. Third, a simple parameterization of the humidity dependence of the submicron aerosol scattering coefficient has been derived, depending only on a volume weighted average diameter growth factor and the volume mean diameter of the dry size distribution. One set of empirical parameters can be used to parameterize all aerosol types characterized during the ACE-2 measurement period. Aerosol physical properties and climate forcing parameters in the North-East Atlantic Ocean were clearly affected by pollution outbreaks from Europe. The submicron particle volume increased by a factor of 5 in polluted conditions, the light scattering coefficient of dry particles increased on average by a factor of up to 10, CCN concentrations at supersaturations of 0.2% increased by a factor of 3--5. The aerosol fundamental properties vary often strongly with air mass history, but also show short-term variability that often has a characteristic diurnal scale. The number concentration of fine particles below 50nm and the particle hygroscopic growth factors are mostly dominated by diurnal processes

  1. The contribution of anthropogenic sources to the aerosols over East China Sea

    NASA Astrophysics Data System (ADS)

    Wang, Fujiang; Chen, Ying; Meng, Xi; Fu, Jiangping; Wang, Bo

    2016-02-01

    Total suspended particulate (TSP) samples were collected at a pristine island (Huaniao) in northern East China Sea (ECS) between Mar. 2011 and Jan. 2013 and analyzed for the concentrations of major ions and trace elements. Aerosol sources and the distribution of source regions are identified using positive matrix factorization (PMF) and potential source contribution function (PSCF) methods. It is found that aerosols over Huaniao Island are contributed by six main factors including primary industrial emissions (11.3%), secondary aerosol (22%), oxalate-associated aerosol (15.7%), sea salt (36.7%), ship emission (6.3%) and mineral dust (8.1%). Anthropogenic source contribution to the resolved aerosol mass reached the highest (76.6%) and lowest (18%) values in January 2013 and August 2012 respectively, strongly influenced by the prevailing winds of East Asian monsoon. The main source regions of secondary aerosol are southeastern Hebei and Shandong, which is consistent with the most intensive distribution of coal-fired power plants and the largest emission of precursors in this area. Oxalate-associated aerosol is produced primarily along the coastal line. Primary industrial emissions mainly originate from southwestern Shandong and Yangtze River Delta.

  2. Carbon isotope based aerosol source apportionment in Eastern European city Vilnius

    NASA Astrophysics Data System (ADS)

    Garbaras, Andrius; Sapolaite, Justina; Garbariene, Inga; Ezerinskis, Zilvinas; Pocevicius, Matas; Krikscikas, Laurynas; Jacevicius, Sarunas; Plukis, Arturas; Remeikis, Vidmantas

    2016-04-01

    We present carbonaceous aerosol source apportionment results in Eastern European city Vilnius (capital of Lithuania) using stable carbon isotope ratio (δ13C) and radiocarbon (14C) methods. The aerosol sampling campaigns were performed in 2014-2016 winter seasons in Vilnius. PM1 particles were collected on quartz fiber filters using high volume sampler, while PM10 and size segregated aerosol particles were collected using low volume and MOUDI 128 cascade impactor respectively. δ13C values were measured with EA-IRMS system while radiocarbon analysis was performed using Single Stage Accelerator Mass Spectrometer (SSAMS). For the AMS analysis, filters (or aluminium foils from cascade impactor) were graphitized using Automated Graphitization Equipment. It was estimated that dominant carbonaceous aerosol source in Vilnius was of biogenic/biomass origin (60-90 %). Fossil fuel sources accounted for up to 23 % of total carbon fraction. Combining stable carbon and radiocarbon isotope analysis we were able to quantify the amount of coal derived aerosol particles. The contribution of coal burning emissions were up to 14 %. We will present the applicability of dual carbon (13C and 14C) isotope ratio method for the aerosol source apportionment in different regions of Europe, also the perspectives of using MOUDI cascade impactors to make source apportionment in size segregated aerosol particles.

  3. Hazardous constituent source term. Revision 2

    SciTech Connect

    Not Available

    1994-11-17

    The Department of Energy (DOE) has several facilities that either generate and/or store transuranic (TRU)-waste from weapons program research and production. Much of this waste also contains hazardous waste constituents as regulated under Subtitle C of the Resource Conservation and Recovery Act (RCRA). Toxicity characteristic metals in the waste principally include lead, occurring in leaded rubber gloves and shielding. Other RCRA metals may occur as contaminants in pyrochemical salt, soil, debris, and sludge and solidified liquids, as well as in equipment resulting from decontamination and decommissioning activities. Volatile organic compounds (VOCS) contaminate many waste forms as a residue adsorbed on surfaces or occur in sludge and solidified liquids. Due to the presence of these hazardous constituents, applicable disposal regulations include land disposal restrictions established by Hazardous and Solid Waste Amendments (HSWA). The DOE plans to dispose of TRU-mixed waste from the weapons program in the Waste Isolation Pilot Plant (WIPP) by demonstrating no-migration of hazardous constituents. This paper documents the current technical basis for methodologies proposed to develop a post-closure RCRA hazardous constituent source term. For the purposes of demonstrating no-migration, the hazardous constituent source term is defined as the quantities of hazardous constituents that are available for transport after repository closure. Development of the source term is only one of several activities that will be involved in the no-migration demonstration. The demonstration will also include uncertainty and sensitivity analyses of contaminant transport.

  4. Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass at Bakersfield

    EPA Science Inventory

    Secondary organic aerosols (SOA), known to form in the atmosphere from oxidation of volatile organic compounds (VOCs) emitted by anthropogenic and biogenic sources, are a poorly understood but substantial component of atmospheric particles. In this study, we examined the chemic...

  5. Sources and evolution of cloud-active aerosol in California's Sierra Nevada Mountains

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Corrigan, C.; Noblitt, S.; Creamean, J.; Collins, D. B.; Cahill, J. F.; Prather, K. A.; Collett, J. L.; Henry, C.

    2011-12-01

    To assess the sources of cloud-active aerosol and their influence on the hydrological cycle in California, the CalWater Experiment took place in winter 2011 in the foothills of the Sierra Nevada Mountains. During this experiment, we coupled the capabilities of demonstrated miniaturized instrumentation - cloud condensation nuclei (CCN), water condensation nuclei (WCN) and microchip capillary electrophoresis (MCE) - to provide direct chemical measurements of cloud active aerosols. Ion concentrations of CCN droplets attribute the anthropogenic, marine and secondary organic contributions to cloud-active aerosols. Detailed spectra from an Aerosol-Time-of-Flight Mass Spectrometer provide additional information on the sources of aerosol. Storm fronts and changes in atmospheric boundary layer brought aerosol and anions associated with Central Valley pollution to the field site with CCN concentrations reaching several thousand cm-3. Hygroscopicity parameters indicate aging of the organic fraction during aerosol transport from the Central Valley to the mountains. Otherwise, CCN concentrations were low when high pressure systems prevented boundary layer development and intrusion of the Central Valley pollution to the site. MCE results show that nitrates and sulfates comprise most of the fraction of the aerosol anion mass (PM1). During the passage of storm fronts, which transported pollution from the Central Valley upslope, nitrate concentrations peaked at several μ g m-3. Low supersaturation CCN concentrations coincide with increases in aerosol nitrate, which suggests that nitrate has a role in cloud formation of giant CCN and, furthermore, in precipitation processes in the Sierra Nevada. CCN spectra show large variations depending on the aerosol sources and sometimes exhibit bi-modal distributions with minima at 0.3% Sc -- similar to the so-called 'Hoppel minima' associated to number size distributions. During these bi-modal events, sulfate also increases supporting the

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

    NASA Technical Reports Server (NTRS)

    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

  7. Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

    PubMed

    Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

    2014-09-15

    The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic

  8. Skin as a potential source of infectious foot and mouth disease aerosols

    PubMed Central

    Dillon, Michael B.

    2011-01-01

    This review examines whether exfoliated, virus-infected animal skin cells could be an important source of infectious foot and mouth disease virus (FMDV) aerosols. Infectious material rafting on skin cell aerosols is an established means of transmitting other diseases. The evidence for a similar mechanism for FMDV is: (i) FMDV is trophic for animal skin and FMDV epidermis titres are high, even in macroscopically normal skin; (ii) estimates for FMDV skin cell aerosol emissions appear consistent with measured aerosol emission rates and are orders of magnitude larger than the minimum infectious dose; (iii) the timing of infectious FMDV aerosol emissions is consistent with the timing of high FMDV skin concentrations; (iv) measured FMDV aerosol sizes are consistent with skin cell aerosols; and (v) FMDV stability in natural aerosols is consistent with that expected for skin cell aerosols. While these findings support the hypothesis, this review is insufficient, in and of itself, to prove the hypothesis and specific follow-on experiments are proposed. If this hypothesis is validated, (i) new FMDV detection, management and decontamination approaches could be developed and (ii) the relevance of skin cells to the spread of viral disease may need to be reassessed as skin cells may protect viruses against otherwise adverse environmental conditions. PMID:21450741

  9. Aerosol and CCN over the Southern Ocean: Sources, Sinks and Processes

    NASA Astrophysics Data System (ADS)

    Clarke, A. D.; Freitag, S.; Howell, S. G.; Snider, J. R.; Kazil, J.; Feingold, G.; McNaughton, C. S.; Brekhovskikh, V.; Kapustin, V.; Campos, T. L.; Shank, L.

    2013-12-01

    Aerosol able to activate as cloud condensation nuclei (CCN) in marine stratus play an important role in cloud properties and processes. The 2008 VOCALS experiment (http://www.eol.ucar.edu/projects/vocals/) explored the aerosol cloud system over the South East Pacific (SEP). There, marine boundary layer (MBL) air from the Southern Ocean is directed north parallel to the South American coast and exposed to continental emissions. During this transport the initial clean MBL aerosol is modified in response to production, processing, entrainment, mixing, and removal. Here we discuss how the aerosol, the CCN and the clouds over the SEP are coupled by these processes. VOCALS data along 20S indicated cleanest air offshore and west of about 78W. However, some of the cleanest air (lowest CO concentrations) over the SEP were present in pockets of open cells (POC's). This suggests POC's are favored in places where remnants of Southern Ocean MBL air experienced the least mixing with higher CO sources during transport, either coastal or via entrainment of free troposphere air. Entrainment from the free troposphere (FT) was found to be an important source of marine boundary layer (MBL) aerosol in both near-shore and off-shore regions while direct advection of continental aerosol tended to influence aerosol and CCN closer to the coast. Entrainment from the FT included diverse sources from South America as well as long range transport from the western Pacific. Entrainment of FT aerosol can resupply the MBL with CCN and this process appears greatly enhanced when patchy 'rivers' of pollution lie directly above the inversion. This process was evident both offshore and near the coast. Production of CCN from sea spray aerosol (SSA) were found to increase with wind speed but atmospheric concentrations did not generally increase in the higher wind offshore regions because these regions had greater drizzle removal that compensated for increased production. Generally SSA larger than 60 nm

  10. Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

    NASA Technical Reports Server (NTRS)

    Pueschel , R. F.; Gore, Waren J. Y. (Technical Monitor)

    1997-01-01

    Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

  11. Apportionment of urban aerosol sources in Chongqing (China) using synergistic on-line techniques

    NASA Astrophysics Data System (ADS)

    Chen, Yang; Yang, Fumo

    2016-04-01

    The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Chongqing (southwestern China) have been determined. Aerosol chemical composition analyses were performed using multiple on-line techniques, such as single particle aerosol mass spectrometer (SPAMS) for single particle chemical composition, on-line elemental carbon-organic carbon analyzer (on-line OC-EC), on-line X-ray fluorescence (XRF) for elements, and in-situ Gas and Aerosol Compositions monitor (IGAC) for water-soluble ions in PM2.5. All the datasets from these techniques have been adjusted to a 1-h time resolution for receptor model input. Positive matrix factorization (PMF) has been used for resolving aerosol sources. At least six sources, including domestic coal burning, biomass burning, dust, traffic, industrial and secondary/aged factors have been resolved and interpreted. The synergistic on-line techniques were helpful for identifying aerosol sources more clearly than when only employing the results from the individual techniques. This results are useful for better understanding of aerosol sources and atmospheric processes.

  12. SOURCE APPORTIONMENT OF PHOENIX PM2.5 AEROSOL WITH THE UNMIX RECEPTOR MODEL

    EPA Science Inventory

    The multivariate receptor model Unmix has been used to analyze a 3-yr PM2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall percentage source contribution estimates (SCE) for five source categories: ga...

  13. A large sulfate aerosol source during the winter haze in China missing from current models

    NASA Astrophysics Data System (ADS)

    Wang, Y.; Zhang, Q.; Jiang, J.; Zhou, W.; Wang, B.

    2013-12-01

    Regional haze with PM2.5 levels exceeding ten folds of the WHO standard has become the largest air quality concerns in China. In Jan 2013, an episode with daily PM2.5 exceeding 500 ug/m3 occurred for multiple days over North China in Jan 2013, threatening the health of a population of more than 150 million. In situ measurements reveal that sulfate has the largest increase during this winter episode in terms of both absolute mass concentrations and fractions in PM2.5. The enhancement factor during the haze is 9.0 for sulfate, much larger than that of OC (2.9) and EC (2.6). This Jan episode offers an interesting opportunity to test current understanding of aerosol formation mechanisms in winter for this region. We find that while the GEOS-Chem nested-grid chemical transport model (CTM) has some success in simulating PM2.5 in Jan 2013, it significantly underestimates the enhancement of sulfate during the sever haze period, suggesting a missing chemical formation mechanism of sulfate during the winter haze in the model. Based on survey of previous lab studies and observational constraints, we propose that the conversion of SO2 to sulfate via heterogeneous reactions on pre-existing wet and deliquesced aerosols is a significant source of sulfate under appropriate relative humidity conditions during the haze. Adding this mechanism in the model proves to be the most effective in reconciling model results with the observed sulfate aerosol concentrations.

  14. The Denver Aerosol Sources and Health (DASH) Study: Overview and Early Findings

    PubMed Central

    Vedal, S.; Hannigan, M.P.; Dutton, S.J.; Miller, S. L.; Milford, J.B.; Rabinovitch, N.; Kim, S.-Y.; Sheppard, L.

    2012-01-01

    Improved understanding of the sources of air pollution that are most harmful could aid in developing more effective measures for protecting human health. The Denver Aerosol Sources and Health (DASH) study was designed to identify the sources of ambient fine particulate matter (PM2.5) that are most responsible for the adverse health effects of short-term exposure to PM 2.5. Daily 24-hour PM2.5 sampling began in July 2002 at a residential monitoring site in Denver, Colorado, using both Teflon and quartz filter samplers. Sampling is planned to continue through 2008. Chemical speciation is being carried out for mass, inorganic ionic compounds (sulfate, nitrate and ammonium), and carbonaceous components, including elemental carbon, organic carbon, temperature-resolved organic carbon fractions and a large array of organic compounds. In addition, water soluble metals were measured daily for 12 months in 2003. A receptor-based source apportionment approach utilizing positive matrix factorization (PMF) will be used to identify PM 2.5 source contributions for each 24-hour period. Based on a preliminary assessment using synthetic data, the proposed source apportionment should be able to identify many important sources on a daily basis, including secondary ammonium nitrate and ammonium sulfate, diesel vehicle exhaust, road dust, wood combustion and vegetative debris. Meat cooking, gasoline vehicle exhaust and natural gas combustion were more challenging for PMF to accurately identify due to high detection limits for certain organic molecular marker compounds. Measurements of these compounds are being improved and supplemented with additional organic molecular marker compounds. The health study will investigate associations between daily source contributions and an array of health endpoints, including daily mortality and hospitalizations and measures of asthma control in asthmatic children. Findings from the DASH study, in addition to being of interest to policymakers, by

  15. The Denver Aerosol Sources and Health (DASH) study: Overview and early findings

    NASA Astrophysics Data System (ADS)

    Vedal, S.; Hannigan, M. P.; Dutton, S. J.; Miller, S. L.; Milford, J. B.; Rabinovitch, N.; Kim, S.-Y.; Sheppard, L.

    Improved understanding of the sources of air pollution that are most harmful could aid in developing more effective measures for protecting human health. The Denver Aerosol Sources and Health (DASH) study was designed to identify the sources of ambient fine particulate matter (PM 2.5) that are most responsible for the adverse health effects of short-term exposure to PM 2.5. Daily 24-h PM 2.5 sampling began in July 2002 at a residential monitoring site in Denver, Colorado, using both Teflon and quartz filter samplers. Sampling is planned to continue through 2008. Chemical speciation is being carried out for mass, inorganic ionic compounds (sulfate, nitrate and ammonium), and carbonaceous components, including elemental carbon, organic carbon, temperature-resolved organic carbon fractions and a large array of organic compounds. In addition, water-soluble metals were measured daily for 12 months in 2003. A receptor-based source apportionment approach utilizing positive matrix factorization (PMF) will be used to identify PM 2.5 source contributions for each 24-h period. Based on a preliminary assessment using synthetic data, the proposed source apportionment should be able to identify many important sources on a daily basis, including secondary ammonium nitrate and ammonium sulfate, diesel vehicle exhaust, road dust, wood combustion and vegetative debris. Meat cooking, gasoline vehicle exhaust and natural gas combustion were more challenging for PMF to accurately identify due to high detection limits for certain organic molecular marker compounds. Measurements of these compounds are being improved and supplemented with additional organic molecular marker compounds. The health study will investigate associations between daily source contributions and an array of health endpoints, including daily mortality and hospitalizations and measures of asthma control in asthmatic children. Findings from the DASH study, in addition to being of interest to policymakers, by

  16. Potential emission flux to aerosol pollutants over Bengal Gangetic plain through combined trajectory clustering and aerosol source fields analysis

    NASA Astrophysics Data System (ADS)

    Kumar, D. Bharath; Verma, S.

    2016-09-01

    A hybrid source-receptor analysis was carried out to evaluate the potential emission flux to winter monsoon (WinMon) aerosols over Bengal Gangetic plain urban (Kolkata, Kol) and semi-urban atmospheres (Kharagpur, Kgp). This was done through application of fuzzy c-mean clustering to back-trajectory data combined with emission flux and residence time weighted aerosols analysis. WinMon mean aerosol optical depth (AOD) and angstrom exponent (AE) at Kol (AOD: 0.77; AE: 1.17) were respectively slightly higher than and nearly equal to that at Kgp (AOD: 0.71; AE: 1.18). Out of six source region clusters over Indian subcontinent and two over Indian oceanic region, the cluster mean AOD was the highest when associated with the mean path of air mass originating from the Bay of Bengal and the Arabian sea clusters at Kol and that from the Indo-Gangetic plain (IGP) cluster at Kgp. Spatial distribution of weighted AOD fields showed the highest potential source of aerosols over the IGP, primarily over upper IGP (e.g. Punjab, Haryana), lower IGP (e.g. Uttarpradesh) and eastern region (e.g. west Bengal, Bihar, northeast India) clusters. The emission flux contribution potential (EFCP) of fossil fuel (FF) emissions at surface (SL) of Kol/Kgp, elevated layer (EL) of Kol, and of biomass burning (BB) emissions at SL of Kol were primarily from upper, lower, upper/lower IGP clusters respectively. The EFCP of FF/BB emissions at Kgp-EL/SL, and that of BB at EL of Kol/Kgp were mainly from eastern region and Africa (AFR) clusters respectively. Though the AFR cluster was constituted of significantly high emission flux source potential of dust emissions, the EFCP of dust from northwest India (NWI) was comparable to that from AFR at Kol SL/EL.

  17. Long term measurements of the estimated hygroscopic enhancement of aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Hervo, Maxime; Sellegri, Karine; Pichon, Jean Marc; Roger, Jean Claude; Laj, Paolo

    2015-04-01

    Water vapour has a major impact on aerosol optical properties, thus on the Radiative Forcing for aerosol-radiation interaction (RFari). However there is few studies measuring this impact over a large period. Optical properties of aerosols were measured at the GAW Puy de Dôme station (1465m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the dry optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the planetary boundary layer height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type and the season. At 90% humidity, the scattering factor enhancement (fsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH= 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type. To our knowledge, these results are one of the first presenting the impact of water vapour on the aerosol optical properties for a long period, and the first for a site at the border between the planetary boundary layer

  18. Long-term aerosol study on continental scale through EARLINET vertical profiles

    NASA Astrophysics Data System (ADS)

    Mona, Lucia; Pappalardo, Gelsomina; Linne, Holger; Wandinger, Ulla

    2015-04-01

    Lidar techniques offer the opportunity for investigating the aerosol vertical profiles, which is an important information for climatological, meteorological and air quality issues. EARLINET (European Aerosol Research Lidar Network) has been providing aerosol optical properties vertical profiles over Europe since May 2000. Long-term aerosol observations performed within EARLINET allows a climatological study of aerosol properties over Europe. All EARLINET stations perform almost simultaneously measurements three times per week following a scheduling established in 2000. Besides these climatological measurements, additional measurements are performed in order to monitor special events (as volcanic eruptions and desert dust intrusion), for satellite data evaluation and integrated studies and during intensive measurements campaigns. Aerosol optical properties vertical profiles are freely available at www.earlinet.org and through ACRIS data center http://www.actris.net/. This data are currently published on the CERA database with an associated doi number. Based mainly on Raman technique, EARLINET stations typically provide direct measurement of extinction profiles, and therefore of the aerosol optical depth (AOD), a key parameter for understanding the aerosol role on radiation budget. The free troposphere contribution to AOD and altitude of lofted layers are provided thanks to the vertical profiling capability of lidar technique. The representativeness of EARLINET regular scheduling for climatological studies is investigating through the comparison with AERONET and MODIS measurements. We find that the regular measurements schedule is typically sufficient for climatological studies. In addition lidar punctual measurements are representative for a larger area (1°x1°) in a climatological sense. Long term analysis of EARLINET profiles shows that the AOD in generally decreasing over Europe in agreement with both passive-sensors and in situ measurements. Mean vertical

  19. CCN frequency distributions and aerosol chemical composition from long-term observations at European ACTRIS supersites

    NASA Astrophysics Data System (ADS)

    Decesari, Stefano; Rinaldi, Matteo; Schmale, Julia Yvonne; Gysel, Martin; Fröhlich, Roman; Poulain, Laurent; Henning, Silvia; Stratmann, Frank; Facchini, Maria Cristina

    2016-04-01

    Cloud droplet number concentration is regulated by the availability of aerosol acting as cloud condensation nuclei (CCN). Predicting the air concentrations of CCN involves knowledge of all physical and chemical processes that contribute to shape the particle size distribution and determine aerosol hygroscopicity. The relevance of specific atmospheric processes (e.g., nucleation, coagulation, condensation of secondary organic and inorganic aerosol, etc.) is time- and site-dependent, therefore the availability of long-term, time-resolved aerosol observations at locations representative of diverse environments is strategic for the validation of state-of-the-art chemical transport models suited to predict CCN concentrations. We focused on long-term (year-long) datasets of CCN and of aerosol composition data including black carbon, and inorganic as well as organic compounds from the Aerosol Chemical Speciation Monitor (ACSM) at selected ACTRIS supersites (http://www.actris.eu/). We discuss here the joint frequency distribution of CCN levels and of aerosol chemical components concentrations for two stations: an alpine site (Jungfraujoch, CH) and a central European rural site (Melpitz, DE). The CCN frequency distributions at Jungfraujoch are broad and generally correlated with the distributions of the concentrations of aerosol chemical components (e.g., high CCN concentrations are most frequently found for high organic matter or black carbon concentrations, and vice versa), which can be explained as an effect of the strong seasonality in the aerosol characteristics at the mountain site. The CCN frequency distributions in Melpitz show a much weaker overlap with the distributions of BC concentrations or other chemical compounds. However, especially at high CCN concentration levels, a statistical correlation with organic matter (OM) concentration can be observed. For instance, the number of CCN (with particle diameter between 20 and 250 nm) at a supersaturation of 0.7% is

  20. Long-term Satellite Observations of Asian Dust Storm: Source, Pathway, and Interannual Variability

    NASA Technical Reports Server (NTRS)

    Hsu, N. Christina

    2008-01-01

    between Deep Blue retrievals of aerosol optical thickness and those directly from AERONET sunphotometers over desert and semi-desert regions. New Deep Blue products will allow scientists to determine quantitatively the aerosol properties near sources using high spatial resolution measurements from SeaWiFS and MODIS-like instruments. Long-term satellite measurements (1998 - 2007) from SeaWiFS will be utilized to investigate the interannual variability of source, pathway, and dust loading associated with the Asian dust storm outbreaks. In addition, monthly averaged aerosol optical thickness during the springtime from SeaWiFS will also be compared with the MODIS Deep Blue products.

  1. Sources and Transport of Aerosol above the Boundary Layer over the Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Corrigan, Craig; Ritchie, John; Pont, Veronique; Claeys, Marine; Sciare, Jean; Mallet, Marc; Dulac, François; Mihalopoulos, Nikos

    2015-04-01

    The Mediterranean Region has been identified as sensitive to changes in the hydrological cycle, which could affect the water resources for millions of people by the turn of the century. However, prior to recent observations, most climate models have not accounted for the impacts of aerosol in this region. Past airborne studies have shown that aerosol sources from Europe and Africa are often transported throughout the lower troposphere; yet, because of their complex vertical distribution, it is a challenge to capture the variability and quantify the contribution of these sources to the radiative budget and precipitation processes. The PAEROS ChArMEx Mountain Experiment (PACMEx) complemented the regional activities by collecting aerosol data from atop a mountain on the island of Corsica, France in order to assess boundary layer / free troposphere atmospheric processes. In June/July 2013, PACMEx instruments were deployed at 2000 m.asl near the center of Corsica, France to complement ground-based aerosol observations at 550 m.asl on the northern peninsula, as well as airborne measurements. Comparisons between the peninsula site and the mountain site show similar general trends in aerosol properties; yet, differences in aerosol properties reveal the myriad transport mechanisms over the Mediterranean Basin. Using aerosol physicochemical data coupled with back trajectory analysis, different sources have been identified including Saharan dust transport, residual dust mixed with sea salt, anthropogenic emissions from Western Europe, and a period of biomass burning from Eastern Europe. Each period exhibits distinct signatures in the aerosol related to transport processes above and below the boundary layer. In addition, the total aerosol concentrations at the mountain site revealed a strong diurnal cycling the between the atmospheric boundary layer and the free troposphere, which is typical of mountain-top observations. PACMEx was funded by the National Science Foundation

  2. Potential source identification for aerosol concentrations over a site in Northwestern India

    NASA Astrophysics Data System (ADS)

    Payra, Swagata; Kumar, Pramod; Verma, Sunita; Prakash, Divya; Soni, Manish

    2016-03-01

    The collocated measurements of aerosols size distribution (ASD) and aerosol optical thickness (AOT) are analyzed simultaneously using Grimm aerosol spectrometer and MICROTOP II Sunphotometer over Jaipur, capital of Rajasthan in India. The contrast temperature characteristics during winter and summer seasons of year 2011 are investigated in the present study. The total aerosol number concentration (TANC, 0.3-20 μm) during winter season was observed higher than in summer time and it was dominated by fine aerosol number concentration (FANC < 2 μm). Particles smaller than 0.8 μm (at aerodynamic size) constitute ~ 99% of all particles in winter and ~ 90% of particles in summer season. However, particles greater than 2 μm contribute ~ 3% and ~ 0.2% in summer and winter seasons respectively. The aerosols optical thickness shows nearly similar AOT values during summer and winter but corresponding low Angstrom Exponent (AE) values during summer than winter, respectively. In this work, Potential Source Contribution Function (PSCF) analysis is applied to identify locations of sources that influenced concentrations of aerosols over study area in two different seasons. PSCF analysis shows that the dust particles from Thar Desert contribute significantly to the coarse aerosol number concentration (CANC). Higher values of the PSCF in north from Jaipur showed the industrial areas in northern India to be the likely sources of fine particles. The variation in size distribution of aerosols during two seasons is clearly reflected in the log normal size distribution curves. The log normal size distribution curves reveals that the particle size less than 0.8 μm is the key contributor in winter for higher ANC.

  3. Sources of volcanic aerosols: Petrologic and volcanological constraints

    NASA Technical Reports Server (NTRS)

    Sigurdsson, Haraldur

    1991-01-01

    Global climatic effects brought about by volcanism are related to the impact of volcanic gases and their derivative aerosols on the atmosphere, rather than the effects of volcanic ash. Evidence from both historic eruptions and polar ice cores indicate that volcanic sulfur gases are the dominant aerosol-forming component, resulting in produciton of a sulfuric acid-rich stratosphere aerosol that can have profound effects on the earth radiation budget over periods of a few years. Due to highly variable sulfur content of different magma types, the climatic effects do not relate simply to total erupted mass. There is a close relationship between volcanic sulfur yield to the atmospheric and hemispheric surface temperature decrease following an eruption, with up to 1 C surface temperature decrease indicated following a major volcanic event such as the 1815 Tambora eruption. While the erupted mass of HCl and HF is equal to or greater than that of sulfur gases in some volcanic events, the halogens do not form known aerosols nor are they abundant in ice core acidity layers. The early removal of halogens from eruption columns occurs by rain flushing and adsorption onto tephra particles, but the fate of halogens in the atmosphere following very large explosive eruptions is unknown. The CO2 flux to the atmosphere from volcanic eruptions is volumetrically one of the most important of the gas species, but owing to the huge size of the atmospheric reservoir of this gas, the volcanic contribution is likely to have negligible effects.

  4. Source term evaluation for combustion modeling

    NASA Technical Reports Server (NTRS)

    Sussman, Myles A.

    1993-01-01

    A modification is developed for application to the source terms used in combustion modeling. The modification accounts for the error of the finite difference scheme in regions where chain-branching chemical reactions produce exponential growth of species densities. The modification is first applied to a one-dimensional scalar model problem. It is then generalized to multiple chemical species, and used in quasi-one-dimensional computations of shock-induced combustion in a channel. Grid refinement studies demonstrate the improved accuracy of the method using this modification. The algorithm is applied in two spatial dimensions and used in simulations of steady and unsteady shock-induced combustion. Comparisons with ballistic range experiments give confidence in the numerical technique and the 9-species hydrogen-air chemistry model.

  5. Concentrations and sources of organic carbon aerosols in the free troposphere over North America

    NASA Astrophysics Data System (ADS)

    Heald, Colette L.; Jacob, Daniel J.; Turquety, SolèNe; Hudman, Rynda C.; Weber, Rodney J.; Sullivan, Amy P.; Peltier, Richard E.; Atlas, Eliot L.; de Gouw, Joost A.; Warneke, Carsten; Holloway, John S.; Neuman, J. Andrew; Flocke, Frank M.; Seinfeld, John H.

    2006-12-01

    Aircraft measurements of water-soluble organic carbon (WSOC) aerosol over NE North America during summer 2004 (ITCT-2K4) are simulated with a global chemical transport model (GEOS-Chem) to test our understanding of the sources of organic carbon (OC) aerosol in the free troposphere (FT). Elevated concentrations were observed in plumes from boreal fires in Alaska and Canada. WSOC aerosol concentrations outside of these plumes average 0.9 ± 0.9 μg C m-3 in the FT (2-6 km). The corresponding model value is 0.7 ± 0.6 μg C m-3, including 42% from biomass burning, 36% from biogenic secondary organic aerosol (SOA), and 22% from anthropogenic emissions. Previous OC aerosol observations over the NW Pacific in spring 2001 (ACE-Asia) averaged 3.3 ± 2.8 μg C m-3 in the FT, compared to a model value of 0.3 ± 0.3 μg C m-3. WSOC aerosol concentrations in the boundary layer (BL) during ITCT-2K4 are consistent with OC aerosol observed at the IMPROVE surface network. The model is low in the boundary layer by 30%, which we attribute to secondary formation at a rate comparable to primary anthropogenic emission. Observed WSOC aerosol concentrations decrease by a factor of 2 from the BL to the FT, as compared to a factor of 10 decrease for sulfate, indicating that most of the WSOC aerosol in the FT originates in situ. Despite reproducing mean observed WSOC concentrations in the FT to within 25%, the model cannot account for the variance in the observations (R = 0.21). Covariance analysis of FT WSOC aerosol with other measured chemical variables suggests an aqueous-phase mechanism for SOA generation involving biogenic precursors.

  6. Exploring Climatology and Long-Term Variations of Aerosols from NASA Reanalysis MERRA-2 with Giovanni

    NASA Technical Reports Server (NTRS)

    Shen, Suhung; Ostrenga, Dana; Vollmer, Bruce; Li, Zhanqing

    2016-01-01

    Dust plays important roles in energy cycle and climate variations. The dust deposition is the major source of iron in the open ocean, which is an essential micronutrient for phytoplankton growth and therefore may influence the ocean uptake of atmospheric CO2. Mineral dust can also act as fertilizer for forests over long time periods. Over 35 years of simulated global aerosol products from NASA atmospheric reanalysis, second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) are available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). The MERRA-2 covers the period 1980-present, continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated by using MERRA-2 aerosol model, which interact directly with the radiation parameterization, and radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Dust deposition data along with other major aerosol compositions (e.g. black carbon, sea salt, and sulfate, etc.) are simulated as dry and wet deposition, respectively. The hourly and monthly data are available at spatial resolution of 0.5ox0.625o (latitude x longitude). Quick data exploration of climatology and interannual variations of MERRA-2 aerosol can be done through the online visualization and analysis tool, Giovanni. This presentation, using dust deposition as an example, demonstrates a number of MERRA-2 data services at GES DISC. Global distributions of dust depositions, and their seasonal and inter-annual variations are investigated from MERRA-2 monthly aerosol products.

  7. A Missing Wintertime Source of Aerosols over the Arctic Inferred from Satellite and In Situ Observations

    NASA Astrophysics Data System (ADS)

    Jaegle, L.; Di Pierro, M.

    2013-12-01

    We use observations of aerosol extinction from the CALIOP instrument on the CALIPSO satellite to map the aerosol distribution over the Arctic as a function of season and altitude between 2006 and 2010. The resulting aerosol distribution is compared to a simulation from the GEOS-Chem chemical transport model. CALIOP observations in the lower troposphere over the High Arctic (>70°N) display a strong winter maximum of 15 Mm-1. The GEOS-Chem model calculates extinction values that are a factor of 2-3 too low for this widespread wintertime haze. In contrast, the model captures the low Arctic and free tropospheric CALIOP extinctions quite well. Comparisons to in situ nephelometer observations at Barrow in Alaska and Alert in Canada confirm this surface High Arctic underestimate. Furthermore, while GEOS-Chem reproduces ground-based observations of sulfate aerosol concentrations obtained at both sites, it significantly underestimates wintertime concentrations of fine mode sea salt aerosols. We hypothesize that the gap between observed and modeled aerosol extinction is due to a missing source of sea salt over the High Arctic during winter. The seasonality and spatial distribution of this missing source is consistent with a blowing snow source over Arctic sea ice. We examine whether the blowing snow parameterization of Yang et al. (2008) can help reconcile model and observations.

  8. Collaborative research. Study of aerosol sources and processing at the GVAX Pantnagar Supersite

    SciTech Connect

    Worsnop, Doug; Volkamer, Rainer

    2012-08-13

    The Two Column Aerosol Project (TCAP) investigated uncertainties in the aerosol direct effect in the northern hemisphere mid-latitudes. The University of Colorado 2D-MAX-DOAS and LED-CE-DOAS instruments were collocated with DOE’s Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) and Mobile Aerosol Observing System (MAOS) during the TCAP-1 campaign at Cape Cod, MA (1 July to 13 August 2012). We have performed atmospheric radiation closure studies to evaluate the use of a novel parameter, i.e., the Raman Scattering Probability (RSP). We have performed first measurements of RSP almucantar scans, and measure RSP in spectra of scattered solar photons at 350nm and 430nm. Radiative Transfer Modelling of RSP demonstrate that the RSP measurement is maximally sensitive to infer even extremely low aerosol optical depth (AOD < 0.01) reliably by DOAS at low solar relative azimuth angles. We further assess the role of elevated aerosol layers on near surface observations of oxygen collision complexes, O 2-O2. Elevated aerosol layers modify the near surface absorption of O2-O2 and RSP. The combination of RSP and O2-O2 holds largely unexplored potential to better constrain elevated aerosol layers and measure column aerosol optical properties such as aerosol effective radius, extinction, aerosol phase functions and refractive indices. The TCAP deployment also provides a time series of reactive trace gas vertical profiles, i.e., nitrogen dioxide (NO2) and glyoxal (C2H2O2), which are measured simultaneously with the aerosol optical properties by DOAS. NO2 is an important precursor for ozone (O3) that modifies oxidative capacity. Glyoxal modifies oxidative capacity and is a source for brown carbon by forming secondary organic aerosol (SOA) via multiphase reactions in aerosol and cloud water. We have performed field measurements of these gases

  9. TRIGA MARK-II source term

    NASA Astrophysics Data System (ADS)

    Usang, M. D.; Hamzah, N. S.; J. B., Abi M.; M. Z., M. Rawi; Abu, M. P.

    2014-02-01

    ORIGEN 2.2 are employed to obtain data regarding γ source term and the radio-activity of irradiated TRIGA fuel. The fuel composition are specified in grams for use as input data. Three types of fuel are irradiated in the reactor, each differs from the other in terms of the amount of Uranium compared to the total weight. Each fuel are irradiated for 365 days with 50 days time step. We obtain results on the total radioactivity of the fuel, the composition of activated materials, composition of fission products and the photon spectrum of the burned fuel. We investigate the differences of results using BWR and PWR library for ORIGEN. Finally, we compare the composition of major nuclides after 1 year irradiation of both ORIGEN library with results from WIMS. We found only minor disagreements between the yields of PWR and BWR libraries. In comparison with WIMS, the errors are a little bit more pronounced. To overcome this errors, the irradiation power used in ORIGEN could be increased a little, so that the differences in the yield of ORIGEN and WIMS could be reduced. A more permanent solution is to use a different code altogether to simulate burnup such as DRAGON and ORIGEN-S. The result of this study are essential for the design of radiation shielding from the fuel.

  10. TRIGA MARK-II source term

    SciTech Connect

    Usang, M. D. Hamzah, N. S. Abi, M. J. B. Rawi, M. Z. M. Rawi Abu, M. P.

    2014-02-12

    ORIGEN 2.2 are employed to obtain data regarding γ source term and the radio-activity of irradiated TRIGA fuel. The fuel composition are specified in grams for use as input data. Three types of fuel are irradiated in the reactor, each differs from the other in terms of the amount of Uranium compared to the total weight. Each fuel are irradiated for 365 days with 50 days time step. We obtain results on the total radioactivity of the fuel, the composition of activated materials, composition of fission products and the photon spectrum of the burned fuel. We investigate the differences of results using BWR and PWR library for ORIGEN. Finally, we compare the composition of major nuclides after 1 year irradiation of both ORIGEN library with results from WIMS. We found only minor disagreements between the yields of PWR and BWR libraries. In comparison with WIMS, the errors are a little bit more pronounced. To overcome this errors, the irradiation power used in ORIGEN could be increased a little, so that the differences in the yield of ORIGEN and WIMS could be reduced. A more permanent solution is to use a different code altogether to simulate burnup such as DRAGON and ORIGEN-S. The result of this study are essential for the design of radiation shielding from the fuel.

  11. A Study of Aerosol Optical and Chemical Properties from the Perspectives of Source Region, Local, and Synoptic Meteorology During Summer 2013 at a Southeast US Regionally Representative Site

    NASA Astrophysics Data System (ADS)

    Krintz, I. A.; Link, M. F.; Madison, B.; Morrow, H. A.; Sherman, J. P.; Zhou, Y.

    2014-12-01

    An intensive summer 2013 aerosol field campaign was conducted at the Appalachian Atmospheric Interdisciplinary Research facility at Appalachian State University (AppalAIR), coinciding with the SOAS campaign in the SE U.S. Measurements included lower tropospheric and column-averaged aerosol properties as part of the NOAA-ESRL and NASA AERONET, lidar-derived vertical profiles of aerosols and clouds, surface and vertical meteorology, and aerosol and organic precursor chemical composition. Clustered 120-hour HYSPLIT back-trajectories were used to determine the influence of source region on aerosol properties and composition. A synoptic-scale weather classification scheme (Sheridan 2000) was applied to bin the aerosol properties by synoptic weather type. Co-located near-surface T, P, and RH measurements and vertical profiles from 75 radiosonde launches were used to determine the influence of local meteorology on the aerosol properties. The anomalously cool, wet summer dampened and delayed the summer peak in aerosol scattering and absorption, relative to previous summers and limited the number of sunphotometer retrievals of column-averaged aerosol properties. Nevertheless, aerosol loading, composition, and several key optical properties such as absorption Angstrom exponent displayed distinct dependence on source region and meteorology. As an example, both light scattering and isoprene-derived SOA concentrations (Link et al, 2014) were highest for more pollution-influenced NE air masses, for which lower hemispheric backscatter fractions and absorption Angstrom exponents were observed. Aerosol loading was generally lower for SW and SE air masses, with the exception of extra-moist tropical weather types, which coincided with high aerosol optical depth and larger, hygroscopic, primarily scattering particles. Aerosol loading increased with local temperature and pressure and some other properties also displayed temperature dependence but the range of temperatures observed

  12. Long term fine aerosol analysis by XRF and PIXE techniques in the city of Rijeka, Croatia

    NASA Astrophysics Data System (ADS)

    Ivošević, Tatjana; Orlić, Ivica; Radović, Iva Bogdanović

    2015-11-01

    The results of a long term, multi elemental XRF and PIXE analysis of fine aerosol pollution in the city of Rijeka, Croatia, are reported for the first time. The samples were collected during a seven months period (6th Aug 2013-28th Feb 2014) on thin stretched Teflon filters and analyzed by energy dispersive X-ray fluorescence (EDXRF) at the Laboratory for Elemental Micro-Analysis (LEMA), University of Rijeka and by Particle Induced X-ray Emission (PIXE) using 1.6 MeV protons at the Laboratory for Ion Beam Interactions (LIBI), Ruđer Bošković Institute, Zagreb. The newly developed micro-XRF system at LEMA provided results for 19 elements in the range from Si to Pb. The PIXE at the LIBI provided information for the same elements as well for the light elements such as Na, Mg and Al. Black carbon was determined with the Laser Integrated Plate Method (LIPM). The results were statistically evaluated by means of the positive matrix factorization (PMF). The seven major pollution sources were identified together with their relative contributions, these are: secondary sulfates, road traffic, smoke, road dust, sea spray, ship emissions and soil dust.

  13. MODELING PHOTOCHEMISTRY AND AEROSOL FORMATION IN POINT SOURCE PLUMES WITH THE CMAQ PLUME-IN-GRID

    EPA Science Inventory

    Emissions of nitrogen oxides and sulfur oxides from the tall stacks of major point sources are important precursors of a variety of photochemical oxidants and secondary aerosol species. Plumes released from point sources exhibit rather limited dimensions and their growth is gradu...

  14. CARBON CONTAINING COMPONENT OF THE LOS ANGELES AEROSOL: SOURCE APPORTIONMENT AND CONTRIBUTIONS TO THE VISIBILITY BUDGET

    EPA Science Inventory

    Source resolution of the organic component of the fine fraction of the ambient aerosol (d(sub p) < 3.5 micrometers) has been carried out by combining source information from the organic component with thermal analysis and local emission inventories. The primary and secondary carb...

  15. Rapid Detection and Identification of Biogenic Aerosol Releases and Sources

    NASA Astrophysics Data System (ADS)

    Wagner, J.; Macher, J.; Ghosal, S.; Ahmed, K.; Hemati, K.; Wall, S.; Kumagai, K.

    2011-12-01

    Biogenic aerosols can be important contributors to aerosol chemistry, cloud droplet and ice nucleation, absorption and scattering of radiation, human health and comfort, and plant, animal, and microbial ecology. Many types of bioaerosols, e.g., fungal spores, are released into the atmosphere in response to specific climatological and meteorological conditions. The rapid identification of bioaerosol releases is thus important for better characterization of the above phenomena, as well as enabling public officials to respond quickly and appropriately to releases of infectious agents or biological toxins. One approach to rapid and accurate bioaerosol detection is to employ sequential, automated samples that can be fed directly into an image acquisition and data analysis device. Raman spectroscopy-based identification of bioaerosols, automated analysis of microscopy images, and automated detection of near-monodisperse peaks in aerosol size-distribution data were investigated as complementary approaches to traditional, manual methods for the identification and counting of fungal and actinomycete spores. Manual light microscopy is a widely used analytical technique that is compatible with a number of air sample formats and requires minimal sample preparation. However, a major drawback is its dependence on a human analyst's ability to distinguish particles and accurately count, size, and identify them. Therefore, automated methods, such as those evaluated in this study, have the potential to provide cost-effective and rapid alternatives if demonstrated to be accurate and reliable. An exploratory examination of individual spores for several macro- and microfungi (those with and without large fruiting bodies) by Raman microspectroscopy found unique spectral features that were used to identify fungi to the genus level. Automated analyses of digital spore images accurately recognized and counted single fungal spores and clusters. An automated procedure to discriminate near

  16. Characterizing an extractive electrospray ionization (EESI) source for the online mass spectrometry analysis of organic aerosols.

    PubMed

    Gallimore, Peter J; Kalberer, Markus

    2013-07-01

    Organic compounds comprise a major fraction of tropospheric aerosol and understanding their chemical complexity is a key factor for determining their climate and health effects. We present and characterize here a new online technique for measuring the detailed chemical composition of organic aerosols, namely extractive electrospray ionization mass spectrometry (EESI-MS). Aerosol particles composed of soluble organic compounds were extracted into and ionized by a solvent electrospray, producing molecular ions from the aerosol with minimal fragmentation. We demonstrate here that the technique has a time resolution of seconds and is capable of making stable measurements over several hours. The ion signal in the MS was linearly correlated with the mass of aerosol delivered to the EESI source over the range tested (3-600 μg/m(3)) and was independent of particle size and liquid water content, suggesting that the entire particle bulk is extracted for analysis. Tandem MS measurements enabled detection of known analytes in the sub-μg/m(3) range. Proof-of-principle measurements of the ozonolysis of oleic acid aerosol (20 μg/m(3)) revealed the formation of a variety of oxidation products in good agreement with previous offline studies. This demonstrates the technique's potential for studying the product-resolved kinetics of aerosol-phase chemistry at a molecular level with high sensitivity and time resolution. PMID:23710930

  17. Source apportionment of carbonaceous aerosols over South and East Asia using dual carbon isotopes

    NASA Astrophysics Data System (ADS)

    Gustafsson, O.; Kirillova, E. N.; Andersson, A.-; Kruså, M.; Sheesley, R. J.; Tiwari, S.-; Lee, M.; Chen, B.; Du, K.

    2012-12-01

    Emissions of black carbon (BC) and other components of carbonaceous aerosols affect both climate and health in South and East Asia, yet substantial uncertainties exist regarding their sources. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain both to direct mitigation and as their different properties make their effects on climate forcing and respiratory health different. This study approached the sourcing challenge by applying microscale radiocarbon measurements to aerosol particles collected in both source regions and at regional receptor observatories of both S Asia (New Delhi and the Maldives Climate Observatory) and of E Asia (Beijing, Shanghai, South China Coastal Observatory and the Korea Climate Observatory - Gosan, KCO-G, Jeju Island). The radiocarbon approach is ideally suited to this task as fossil sources are void of 14C whereas biomass combustion products hold a contemporary 14C signal. For S Asia, the 14C-based observations suggest that biomass combustion contributes half to two-thirds of the BC loading. In contrast, for E Asia, fossil fuel combustion account for four-fifths of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all fifteen BC emission inventory models. There are also poor constraints on the sources of water-soluble organic carbon (WSOC), a large hydrophilic component of carbonaceous aerosols that enhances the propensity of aerosols to form clouds. In a 15-mo continuous campaign in S Asia, radiocarbon-based source apportionment of WSOC shows the dominance of biogenic/biomass combustion sources but also a substantial anthropogenic fossil-fuel contribution (about 20%). WSOC in E Asia reaching KCO-G were 50% from fossil sources. Aerosols reaching the Maldives after long-range over-ocean transport were enriched by 3-4‰ in δ13C-WSOC. This is

  18. The "Parade Blue": effects of short-term emission control on aerosol chemistry.

    PubMed

    Li, Haiyan; Zhang, Qiang; Duan, Fengkui; Zheng, Bo; He, Kebin

    2016-07-18

    The strict control on emissions implemented in Beijing, China, during the 2015 China Victory Day Parade (V-day Parade) to commemorate the 70(th) Anniversary of Victory in World War II, provided a good opportunity to investigate the relationship between emission sources and aerosol chemistry in a heavily polluted megacity. From August 11 to September 3, 2015, an Aerosol Chemical Speciation Monitor was deployed in urban Beijing, together with other collocated instruments, for the real-time measurement of submicron aerosol characteristics. The average PM1 mass concentration was 11.3 (±6.7) μg m(-3) during the V-day Parade, 63.5% lower than that before the V-day Parade. Differently to the relatively smaller decrease of organics (53%), secondary inorganic aerosols (sulfate, nitrate and ammonium) showed significant reductions of 65-78% during the V-day Parade. According to the positive matrix factorization results, primary organic aerosol (POA) from traffic and cooking emissions decreased by 41.5% during the parade, whereas secondary organic aerosol (SOA) presented a much greater reduction (59%). The net effectiveness of emission control measures was investigated further under comparable weather conditions before and during the parade. By excluding the effects of meteorological parameters, the total PM1 mass was reduced by 52-57% because of the emission controls. Although the mass concentrations of aerosol species were reduced substantially, the PM1 bulk composition was similar before and during the control period as a consequence of synergetic control of various precursors. The emission restrictions also suppressed the secondary formation processes of sulfate and nitrate, indicated by the substantially reduced SOR and NOR (molar ratios of sulfate or nitrate to the sums of the sulfate and SO2 or nitrate and NO2) during the event. The study also explored the influence of emission controls on the evolution of organic aerosol using the mass ratios of SOA/POA and oxygen

  19. Size distribution, mixing state and source apportionments of black carbon aerosols in London during winter time

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-06-01

    Black carbon aerosols (BC) at a London urban site were characterized in both winter and summer time 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorization (PMF) factors of organic aerosol mass spectra measured by a high resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However the size distribution of Dc (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different Dc distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), or easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm, and 169 ± 29 nm respectively. The corresponding bulk relative coating thickness of BC (coated particle size / BC core - Dp / Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  20. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-09-01

    Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However, the size distribution of sf (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different sf distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core - Dp/Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  1. Lignin-derived phenols in Houston aerosols: implications for natural background sources.

    PubMed

    Shakya, Kabindra M; Louchouarn, Patrick; Griffin, Robert J

    2011-10-01

    Solvent-extractable monomeric methoxyphenols in aerosol samples conventionally have been used to indicate the influence of biomass combustion. In addition, the presence of lignin oxidation products (LOP), derived from the CuO oxidation of vascular plant organic matter, can help trace the source and inputs of primary biological particles in aerosols. Ambient aerosols (coarse and fine) collected in Houston during summer 2010 were analyzed by gas chromatography-mass spectrometry to characterize monomeric and polymeric sources of LOPs. This is the first time polymeric forms of the LOPs have been characterized in ambient aerosols. The absence or small concentrations of solvent-extractable monomeric LOPs and levoglucosan isomers point to the limited influence of biomass burning during the sampling period. The trace levels of anhydrosugar concentrations most likely result from long-range transport. This observation is supported by the absence of co-occurring lignin monomers that undergo photochemical degradation during transport. The larger concentration (142 ng m(-3)) of lignin polymers in coarse aerosols shows the relative importance of primary biological aerosol particles, even in the urban atmosphere. The LOP parameters suggest a predominant influence from woody tissue of angiosperms, with minor influence from soft tissues, gymnosperms, and soil organic matter. PMID:21877739

  2. Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: impact of anthropogenic sources.

    PubMed

    Ram, Kirpa; Sarin, M M

    2015-01-15

    In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20-70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO4(2-), and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale. PMID:25199599

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

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-06-01

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

  4. Long-term Analysis of Aerosol Optical Thickness from Satellite Retrievals over selected large agglomerations

    NASA Astrophysics Data System (ADS)

    Vountas, Marco; von Hoyningen-Huene, Wolfgang; Yoon, Jongmin; Burrows, John P.

    Aside from adverse health effect urban aerosols have potential effects on the climate system. In this study Aerosol Optical Thickness (AOT) retrievals over land are performed to study the medium to long-term trends of aerosols in large agglomerations (aka megacities). This task is challenging because of the high variability of the surface reflectance. The Bremen AErosol Retrieval (BAER) algorithm has retrieved AOT successfully over land with different satellite data in other studies. Here, the annual-and long-term trend of AOT over several regions have been analyzed using BAER based on SeaWiFS (Sea-viewing Wide Field-of-view Sensor) L1b data over a period of 11 years. Among the regions analyzed were several European regions, as well as Sao Paolo, Brazil, and Perl River Delta in south China. Practically all regions investigated showed a week negative trend in AOT (validated by AERONET), except over Perl River Delta where a comparatively strong positive trend of up to 0.007/yr could be observed.

  5. Long-term impacts of aerosols on the vertical development of clouds and precipitation

    SciTech Connect

    Li, Zhanqing; Niu, F.; Fan, Jiwen; Liu, Yangang; Rosenfeld, Daniel; Ding, Yanni

    2011-12-01

    Aerosol has complex effects on clouds and precipitation that may augment or offset each other contingent upon a variety of variables. As a result, its long-term impact on climate is largely unknown. Using 10 years of the US Atmospheric Radiation Measurement (ARM) measurements, strong aerosol effects of climatologically significance are detected. With increasing total aerosol number concentration (condensation nucleus, CN) measured near the ground, both cloud top height and precipitation change systematically for mix-phase clouds of warm-base (cloud base <1km) and cold-top (above the freezing level), but not for pure liquid and ice clouds. Cloud thickness can increase systematically with the CN concentration by up to a factor of 2. The response of precipitation to CN depends on cloud liquid water path (LWP). As CN increases, rain occurs more frequently for high LWP but less frequently for low LWP. Such strong signals of aerosol long-term impact on cloud and precipitation have not been reported and have significant implications for climate change studies, especially concerning regional and global climate change induced by pollution.

  6. From OLS to VIIRS, an overview of nighttime satellite aerosol retrievals using artificial light sources

    NASA Astrophysics Data System (ADS)

    Zhang, J.; Miller, S. D.; Reid, J. S.; Hyer, E. J.; McHardy, T. M.

    2015-12-01

    Compared to abundant daytime satellite-based observations of atmospheric aerosol, observations at night are relatively scarce. In particular, conventional satellite passive imaging radiometers, which offer expansive swaths of spatial coverage compared to non-scanning lidar systems, lack sensitivity to most aerosol types via the available thermal infrared bands available at night. In this talk, we make the fundamental case for the importance of nighttime aerosol information in forecast models, and the need to mitigate the existing nocturnal gap. We review early attempts at estimating nighttime aerosol optical properties using the modulation of stable artificial surface lights. Initial algorithm development using DMSP Operational Linescan System (OLS) has graduated to refined techniques based on the Suomi-NPP Visible Infrared Imaging Radiometer Suite (VIIRS) Day/Night Band (DNB). We present examples of these retrievals for selected cases and compare the results to available surface-based point-source validation data.

  7. Heavy Ion Formation in Titan's Ionosphere: Magnetospheric Introduction of Free Oxygen and Source of Titan's Aerosols?

    NASA Technical Reports Server (NTRS)

    Sittler, E. C., Jr.; Hartle, R. E.; Cooper, J. F.; Johnson, R. E.; Coates, A.; dePater, imke; Strom, Daphne; Simoes, F.; Steele, A.; Robb, F.

    2007-01-01

    With the recent discovery of heavy ions, positive and negative, by the Cassini Plasma Spectrometer (CAPS) instrument in Titan's ionosphere, it reveals new possibilities for aerosol formation at Titan and the introduction of free oxygen to the aerosol chemistry from Saturn's magnetosphere with Enceladus as the primary oxygen source. One can estimate whether the heavy ions in the ionosphere are of sufficient number to account for all the aerosols, under what conditions are favorable for heavy ion formation and how they are introduced as seed particles deeper in Titan's atmosphere where the aerosols form and eventually find themselves on Titan's surface where unknown chemical processes can take place. Finally, what are the possibilities with regard to their chemistry on the surface with some free oxygen present in their seed particles?

  8. Fine mode aerosol composition at three long-term atmospheric monitoring sites in the Amazon Basin

    SciTech Connect

    Artaxo, P.; Gerab, F.; Yamasoe, M.A.; Martins, J.V.

    1994-11-01

    The Amazon Basin tropical rain forest is a key region to study processes that are changing the composition of the global atmosphere, including the large amount of fine mode aerosol particles emitted during biomass burning that might influence the global atmosphere. Three background monitoring stations, Alta Floresta, Cuiaba, and Serra do Navio, are operating continuously measuring aerosol composition. Fine (particle diameter less than 2.0 microns) and coarse (particle diameter greater than 2.0 microns and less than 10 microns) mode aerosol particles were collected using stacked filter units. Particle-induced X-ray emission was used to measure concentrations of up to 20 elements in the fine mode: Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, Zr, and Pb. Soot carbon and gravimetric mass analysis were also performed. Absolute Principal Factor Analysis (APFA) has derived absolute elemental source profiles. APFA showed four aerosol particle components: soil dust (Al, Ca, Ti, Mn, Fe), biomass burning (soot, fine mode mass concentration, K, Cl), natural primary biogenic particles with gas-to-particle component (K, S, Ca, Mn, Zn), and marine aerosol (Cl). Biogenic and biomass burning aerosol particles dominate the fine mode mass concentration, with the presence of K, P, S, Cl, Zn, Br, and fine mode mass concentration (FPM). At the Alta Floresta and Cuiaba sites, during the dry season, a strong component of biomass burning is observed. Inhalable particulate matter (particle diameter less than 10 microns) mass concentration up to 700 micrograms/cu m was measured. Fine particle mass concentration alone can go as high as 400 micrograms/cu m for large regions.

  9. 10 CFR 50.67 - Accident source term.

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... 10 Energy 1 2011-01-01 2011-01-01 false Accident source term. 50.67 Section 50.67 Energy NUCLEAR... Conditions of Licenses and Construction Permits § 50.67 Accident source term. (a) Applicability. The... to January 10, 1997, who seek to revise the current accident source term used in their design...

  10. 10 CFR 50.67 - Accident source term.

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... 10 Energy 1 2010-01-01 2010-01-01 false Accident source term. 50.67 Section 50.67 Energy NUCLEAR... Conditions of Licenses and Construction Permits § 50.67 Accident source term. (a) Applicability. The... to January 10, 1997, who seek to revise the current accident source term used in their design...

  11. Evaluation of coarse and fine particulate sources using a portable aerosol monitor in a desert community.

    PubMed

    Phalen, Robert N; Coleman, Ted

    2012-08-01

    The purpose of this study was to use a portable aerosol monitor as a preliminary screening tool to identify local sources of coarse (PM(10-2.5)) and fine (PM(2.5)) particulate matter within the Coachella Valley, a low-elevation desert community. The portable aerosol monitor proved to be useful in identifying particle sources unique to the region, namely, sand dunes with sparse ground cover (vegetation), a river wash, and diesel truck and freight train traffic. The general limitations relate to discrepancies in the fraction of PM(10-2.5) when compared to regional air quality data and a lack of accurate mass-based data. PMID:22617941

  12. Single particle characterization, source apportionment, and aging effects of ambient aerosols in Southern California

    NASA Astrophysics Data System (ADS)

    Shields, Laura Grace

    Composed of a mixture of chemical species and phases and existing in a variety of shapes and sizes, atmospheric aerosols are complex and can have serious influence on human health, the environment, and climate. In order to better understand the impact of aerosols on local to global scales, detailed measurements on the physical and chemical properties of ambient particles are essential. In addition, knowing the origin or the source of the aerosols is important for policymakers to implement targeted regulations and effective control strategies to reduce air pollution in their region. One of the most ground breaking techniques in aerosol instrumentation is single particle mass spectrometry (SPMS), which can provide online chemical composition and size information on the individual particle level. The primary focus of this work is to further improve the ability of one specific SPMS technique, aerosol time-of-flight mass spectrometry (ATOFMS), for the use of identifying the specific origin of ambient aerosols, which is known as source apportionment. The ATOFMS source apportionment method utilizes a library of distinct source mass spectral signatures to match the chemical information of the single ambient particles. The unique signatures are obtained in controlled source characterization studies, such as with the exhaust emissions of heavy duty diesel vehicles (HDDV) operating on a dynamometer. The apportionment of ambient aerosols is complicated by the chemical and physical processes an individual particle can undergo as it spends time in the atmosphere, which is referred to as "aging" of the aerosol. Therefore, the performance of the source signature library technique was investigated on the ambient dataset of the highly aged environment of Riverside, California. Additionally, two specific subsets of the Riverside dataset (ultrafine particles and particles containing trace metals), which are known to cause adverse health effects, were probed in greater detail. Finally

  13. Studying organic aerosols during bonfire night in Manchester: ME-2 source apportionment

    NASA Astrophysics Data System (ADS)

    Reyes Villegas, Ernesto; Allan, James

    2016-04-01

    Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality (Zhao et al. 2014) such as bonfires and fireworks. In general, during these episodes, high particulate matter concentrations drop within 24 hrs; however, it is the fine fraction that dominates the emissions, known to have a potentially negative impact on air quality, thus the impact of bonfires/fireworks on air quality must be considered. Aerosols and gases were measured using a variety of instruments at The University of Manchester, sampling atmospheric emissions on Bonfire night, 5 November, one week before and one week later, in 2013 and 2014. The Multilinear Engine (ME-2) factorization tool was used through the recently developed source finder interface (SoFi, Canonaco et al. 2013) to identify sources of organic aerosols (OA) sampled with an Aerosol Mass Spectrometer (AMS). ME-2 identified five sources: solid fuel OA (SFOA), hydrocarbon like OA (HOA), cooking OA (COA), semi-volatile (SVOOA) and low volatility (LVOOA) during both years. In 2014, air pollutant concentrations were particularly high, with the highest SFOA concentrations being 20 μgm-3 at 20:30 hrs. when fireworks from different parks in Manchester were launched. Black carbon (BC) concentrations started increasing before the fireworks, around 18:00 hrs; these concentrations are representative of bonfire emissions. However, traffic emissions may be contributing to BC here; further work will be done to differentiate traffic emissions from solid fuel emissions. By analysing daily aerosol concentrations according to DEFRA's Daily Air Quality Index, it is possible to observe that in 2014, PM2.5 concentrations were considered to be high (65 μgm-3) while in 2013, PM2.5 concentrations were considered low (12 μgm-3); in the case of BBOA, concentrations ranged from 2.9 μgm-3 in 2014 to 0.65 μgm-3 in 2013. The discrepancy between these studies is mainly a result of different meteorological

  14. Insights into Submicron Aerosol Composition and Sources from the WINTER Aircraft Campaign Over the Eastern US.

    NASA Astrophysics Data System (ADS)

    Schroder, J. C.; Campuzano Jost, P.; Day, D. A.; Fibiger, D. L.; McDuffie, E. E.; Blake, N. J.; Hills, A. J.; Hornbrook, R. S.; Apel, E. C.; Weinheimer, A. J.; Campos, T. L.; Brown, S. S.; Jimenez, J. L.

    2015-12-01

    The WINTER aircraft campaign was a recent field experiment to probe the sources and evolution of gas pollutants and aerosols in Northeast US urban and industrial plumes during the winter. A highly customized Aerodyne aerosol mass spectrometer (AMS) was flown on the NCAR C-130 to characterize submicron aerosol composition and evolution. Thirteen research flights were conducted covering a wide range of conditions, including rural, urban, and marine environments during day and night. Organic aerosol (OA) was a large component of the submicron aerosol in the boundary layer. The fraction of OA (fOA) was smaller (35-40%) than in recent US summer campaigns (~60-70%). Biomass burning was observed to be an important source of OA in the boundary layer, which is consistent with recent wintertime studies that show a substantial contribution of residential wood burning to the OA loadings. OA oxygenation (O/C ratio) shows a broad distribution with a substantial fraction of smaller O/C ratios when compared to previous summertime campaigns. Since measurements were rarely made very close to primary sources (i.e. directly above urban areas), this is consistent with oxidative chemistry being slower during winter. SOA formation and aging in the NYC plume was observed during several flights and compared with summertime results from LA (CalNex) and Mexico City (MILAGRO). Additionally, an oxidation flow reactor (OFR) capable of oxidizing ambient air up to several equivalent days of oxidation was deployed for the first time in an aircraft platform. The aerosol outflow of the OFR was sampled with the AMS to provide real-time snapshots of the potential for aerosol formation and aging. For example, a case study of a flight through the Ohio River valley showed evidence of oxidation of SO2 to sulfate. The measured sulfate enhancements were in good agreement with our OFR chemical model. OFR results for SOA will be discussed.

  15. Global Retrieval of Aerosol Properties from Sources to Sinks By MODIS

    NASA Technical Reports Server (NTRS)

    Hsu, N. Christina

    2005-01-01

    Mineral dust and smoke aerosols play an important role in both climate forcing and oceanic productivity throughout the entire year. Due to the relatively short lifetime (a few hours to about a week), the distributions of these airborne particles vary extensively in both space and time. Consequently, satellite observations are needed over both source and sink regions for continuous temporal and spatial sampling of dust and smoke properties. However, despite their importance, the high spatial resolution satellite measurements of these aerosols near their sources have been lacking, In this paper, we will demonstrate the capability of a new satellite algorithm to retrieve aerosol optical thickness and single scattering albedo over bright-reflecting surfaces such as urban areas and deserts. Such retrievals have been difficult to perform using previously available algorithms that use wavelengths from the mid-visible to the near IR because they have trouble separating the aerosol signal from the contribution due to the bright surface reflectance. The new algorithm, called Deep Blue, utilizes blue-wavelength measurements from instruments such as MODIS and SeaWiFS to infer the properties of aerosols, since the surface reflectance over land in the blue part of the spectrum is much lower than for longer wavelength channels. We have validated the satellite retrieved aerosol optical thickness with data from AERONET sunphotometers over land, including desert and semi-desert regions. The comparisons show reasonable agreements between these two. Our results show that the dust plumes lifted from the deserts near India/Pakistan border, and over Afghanistan, and the Arabian Peninsula are often observed by MODIS to be transported along the Indo-Gangetic Basin and mixed with the fine mode pollution particles generated by anthropogenic activities in this region, particularly during the pre-monsoon season (April-May). These new satellite products will allow scientists to determine

  16. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-06-01

    An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed along with a Scanning Mobility Particle Sizer (SMPS) and a Multi Angle Absorption Photometers (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1) in Lanzhou, northwest China, during 12 July-7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution mass spectra of organic aerosols (OA) identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns both with peak at ~07:00-11:00 (BJT: UTC +8) corresponding to the morning rush hours, while cooking OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00-15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00-13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity with that of

  17. Nonradioactive Environmental Emissions Chemical Source Term for the Double Shell Tank (DST) Vapor Space During Waste Retrieval Operations

    SciTech Connect

    MAY, T.H.

    2000-04-21

    A nonradioactive chemical vapor space source term for tanks on the Phase 1 and the extended Phase 1 delivery, storage, and disposal mission was determined. Operations modeled included mixer pump operation and DST waste transfers. Concentrations of ammonia, specific volatile organic compounds, and quantitative volumes of aerosols were estimated.

  18. Sources, seasonality, and trends of Southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

    NASA Astrophysics Data System (ADS)

    Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

    2015-07-01

    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the Southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 km × 25 km resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the Southeast US. GEOS-Chem simulation of sulfate requires a missing oxidant, taken here to be stabilized Criegee intermediates, but which could alternatively reflect an unaccounted for heterogeneous process. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 20 % in the cloud convective layer at 1.5-3 km, and 20 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-])) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by organic aerosol. This would explain the long-term decline of ammonium aerosol in the Southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the Southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the Southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 21 %. The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from

  19. Challenges to producing a long-term stratospheric aerosol climatology for chemistry and climate

    NASA Astrophysics Data System (ADS)

    Thomason, Larry; Vernier, Jean-Paul; Bourassa, Adam; Rieger, Landon; Luo, Beiping; Peter, Thomas; Arfeuille, Florian

    2016-04-01

    Stratospheric aerosol data sets are key inputs for climate models (GCMs, CCMs) particularly for understanding the role of volcanoes on climate and as a surrogate for understanding the potential of human-derived stratospheric aerosol as mitigation for global warming. In addition to supporting activities of individual climate models, the data sets also act as a historical input to the activities of SPARC's Chemistry-Climate Model Initiative (CCMI) and the World Climate Research Programme's Coupled Model Intercomparison Project (CMIP). One such data set was produced in 2004 as a part of the SPARC Assessment of Stratospheric Aerosol Properties (ASAP), extending from 1979 and 2004. It was primarily constructed from the Stratospheric Aerosol and Gas Experiment series of instruments but supplemented by data from other space-based sources and a number of ground-based and airborne instruments. Updates to this data set have expanded the timeframe to span from 1850 through 2014 through the inclusion of data from additional sources, such as photometer data and ice core analyses. Fundamentally, there are limitations to the reliability of the optical properties of aerosol inferred from even the most complete single instrument data sets. At the same time, the heterogeneous nature of the underlying data to this historical data set produces considerable challenges to the production of a climate data set which is both homogeneous and reliable throughout its timespan. In this presentation, we will discuss the impact of this heterogeneity showing specific examples such as the SAGE II to OSIRIS/CALIPSO transition in 2005. Potential solutions to these issues will also be discussed.

  20. A Long-term Record of Saharan Dust Aerosol Properties from TOMS Observations: Optical Depth and Single Scattering Albedo

    NASA Technical Reports Server (NTRS)

    Torres, Omar; Bhartia, P. K.; Herman, J. R.; Einaudi, Franco (Technical Monitor)

    2000-01-01

    The interaction between the strong Rayleigh scattering in the near UV spectral region (330-380 nm) and the processes of aerosol absorption and scattering, produce a clear spectral signal in the upwelling radiance at the top of the atmosphere. This interaction is the basis of the TOMS (Total Ozone Mapping Spectrometer) aerosol retrieval technique that can be used for their characterization and to differentiate non-absorbing sulfates from strongly UV-absorbing aerosols such as mineral dust. For absorbing aerosols, the characterization is in terms of the optical depth and single scattering albedo with assumptions about the aerosol plume height. The results for non-absorbing aerosols are not dependent on plume height. Although iron compounds represent only between 5% to 8% of desert dust aerosol mass, hematite (Fe2O3) accounts for most of the near UV absorption. Because of the large ultraviolet absorption characteristic of hematite, the near UV method of aerosol sensing is especially suited for the detection and characterization of desert dust aerosols. Using the combined record of near UV measurements by the Nimbus7 (1978-1992) and Earth Probe (1996-present) TOMS instruments, a global longterm climatology of near UV optical depth and single scattering albedo has been produced. The multi-year long record of mineral aerosol properties over the area of influence of the Saharan desert, will be discussed.

  1. Chemical composition of aerosols over Bay of Bengal during pre-monsoon: Dominance of anthropogenic sources

    NASA Astrophysics Data System (ADS)

    Nair, Prabha R.; George, Susan K.; Aryasree, S.; Jacob, Salu

    2014-03-01

    Total suspended particulates were collected from the marine boundary layer of Bay of Bengal (BoB) as part of the Integrated Campaign for Aerosols gases & Radiation Budget (ICARB) conducted under the Geosphere Biosphere Programme of Indian Space Research Organisation during pre-monsoon period. These samples were analyzed to quantify various chemical species and to bring out a comprehensive and quantitative picture of the chemical composition of aerosols in the marine environment of Bay of Bengal. Almost all the species showed highest mass concentration over north/head BoB. On the other hand, their mass fractions were high over mid/south BoB which has implications on the radiative forcing in this region. The source characteristics of various species were identified using specific chemical components as tracers. Presence of significant amount of non-sea-salt aerosols (~7-8 times of sea-salt) and several trace species like Ni, Pb, Zn, etc were observed in this marine environment indicating significant continental/anthropogenic influence. An approximate estimate of the contributions of anthropogenic and natural aerosols to the total aerosol mass loading showed prominence of anthropogenic component over mid and south BoB also. Based on this study first-cut aerosol chemical models were evolved for BoB region.

  2. Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

    NASA Astrophysics Data System (ADS)

    Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

    2012-11-01

    Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish

  3. Potential source regions and processes of aerosol in the summer Arctic

    NASA Astrophysics Data System (ADS)

    Heintzenberg, J.; Leck, C.; Tunved, P.

    2015-06-01

    Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected.

  4. Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method

    NASA Astrophysics Data System (ADS)

    Zencak, Zdenek; Elmquist, Marie; Gustafsson, Örjan

    To make progress towards linking the atmosphere and biogeosphere parts of the black carbon (BC) cycle, a chemothermal oxidation method (CTO-375), commonly applied for isolating BC from complex geomatrices such as soils, sediments and aquatic particles, was applied to investigate the BC also in atmospheric particles. Concentrations and 14C-based source apportionment of CTO-375 based BC was established for a reference aerosol (NIST RM-8785) and for wintertime aerosols collected in Stockholm and in a Swedish background area. The results were compared with thermal-optical (OC/EC) measurements. For NIST RM-8785, a good agreement was found between the BC CTO-375 concentration and the reported elemental carbon (EC) concentration measured by the "Speciation Trends Network—National Institute of Occupational Safety and Health" method (EC NIOSH) with BC CTO-375 of 0.054±0.002 g g -1 and EC NIOSH of 0.067±0.008 g g -1. In contrast, there was an average factor of ca. 20 difference between BC CTO-375 and EC NIOSH for the ambient Scandinavian wintertime aerosols, presumably reflecting a combination of BC CTO-375 isolating only the recalcitrant soot-BC portion of the BC continuum and the EC NIOSH metric inadvertently including some intrinsically non-pyrogenic organic matter. Isolation of BC CTO-375 with subsequent off-line radiocarbon analysis yielded fraction modern values (fM) for total organic carbon (TOC) of 0.93 (aerosols from a Swedish background area), and 0.58 (aerosols collected in Stockholm); whereas the fM for BC CTO-375 isolates were 1.08 (aerosols from a Swedish background area), and 0.87 (aerosols collected in Stockholm). This radiocarbon-based source apportionment suggests that contribution from biomass combustion to cold-season atmospheric BC CTO-375 in Stockholm was 70% and in the background area 88%.

  5. Aerosol source apportionment from 1 year measurements at the CESAR tower at Cabauw, NL

    NASA Astrophysics Data System (ADS)

    Schlag, P.; Kiendler-Scharr, A.; Blom, M. J.; Canonaco, F.; Henzing, J. S.; Moerman, M. M.; Prévôt, A. S. H.; Holzinger, R.

    2015-12-01

    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, NL. The campaign lasted nearly one year from July 2012 to June 2013 as part of the ACTRIS project. Including black carbon data 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 %). 12 exceedances of the World Health Organization (WHO) PM2.5 daily mean limit (25 μg m-3) were 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 (SOA, 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 ageing 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.

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

    NASA Astrophysics Data System (ADS)

    Schlag, Patrick; Kiendler-Scharr, Astrid; Blom, Marcus Johannes; Canonaco, Francesco; Sebastiaan Henzing, Jeroen; Moerman, Marcel; Prévôt, André Stephan Henry; Holzinger, Rupert

    2016-07-01

    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.

  7. Primary and secondary aerosols in Beijing in winter: sources, variations and processes

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

    2016-07-01

    Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

  8. Nuclear microprobe analysis and source apportionment of individual atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Rabello, Marta L. C.; Watt, Frank; Grime, Geoff; Swietlicki, Erik

    1993-04-01

    In atmospheric aerosol research, 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.

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

    PubMed

    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

  10. Pollution transport efficiency toward the Arctic: Sensitivity to aerosol scavenging and source regions

    NASA Astrophysics Data System (ADS)

    Bourgeois, Quentin; Bey, Isabelle

    2011-04-01

    The processes driving current changes in Arctic atmospheric composition and climate are still uncertain. In particular the relative contributions of major source regions from the midlatitudes remain a matter of debate in the literature. The objectives of this study are to better quantify the relative contributions of different processes governing the transport of pollution from the midlatitudes to the Arctic and the relative contributions of different geopolitical source regions. We use a suite of observational data sets (including the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaigns and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument) to constrain a global aerosol simulation from the ECHAM5-HAMMOZ model. Preliminary comparison of model results with vertical profiles of sulfate and black carbon (BC) collected during the ARCTAS campaigns and with aerosol extinction time series retrieved from CALIOP indicates that the model underestimates export of aerosols from the planetary boundary layer to the free troposphere in the midlatitudes and long-range transport of aerosols from the midlatitudes toward the Arctic. In contrast, observed CO profiles are relatively well simulated, which points to a possible problem with wet scavenging. Decreasing the prescribed aerosol scavenging coefficients within the range of experimental data available in the literature significantly improves the agreement with observations. Sulfate and BC burdens in the Arctic increase by a factor 5-6. Annual global lifetimes of sulfate and BC increase from 3.1 to 4.6 days and from 4.4 to 5.9 days, respectively. Using the improved simulation, we find that 59% of sulfate in the Arctic troposphere comes from the oxidation of SO2 emitted in Siberia (19%), Europe (18%), Asia (13%), and North America (9%). Anthropogenic and biomass burning BC emitted in Siberia, Asia, Europe, and North America contributes 29, 27, 25, and

  11. Long-term source monitoring with BATSE

    NASA Technical Reports Server (NTRS)

    Wilson, R. B.; Harmon, B. A.; Finger, M. H.; Fishman, G. J.; Meegan, C. A.; Paciesas, W. S.

    1992-01-01

    The uncollimated Burst and Transient Source Experiment (BATSE) large area detectors (LADs) are well suited to nearly continuous monitoring of the stronger hard x-ray sources, and time series analysis for pulsars. An overview of the analysis techniques presently being applied to the data are discussed, including representative observations of the Crab Nebula, Crab pulsar, and summaries of the sources detected to data. Results of a search for variability in the Crab Pulsar pulse profile are presented.

  12. EPIDEMIOLOGICAL STUDIES ON EXTRA PULMONARY EFFECTS OF FRESH AND AGED URBAN AEROSOLS FROM DIFFERENT SOURCES

    EPA Science Inventory

    The studies will give evidence on health effects of key characteristics of the urban aerosol such as oxidative stress and on the role of sources in urban areas. In addition, they will assess the potential role of ambient air pollution concentrations on smaller time-scales than...

  13. The Vertical Structure, Sources, and Evolution of Aerosols in the Mediterranean Region

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Bourrianne, Thierry; Léon, Jean-François; Pont, Véronique; Mallet, Marc; Lambert, Dominique; Augustin, Patrick; Dulac, François; Junkermann, Wolfgang

    2013-04-01

    The VESSAER campaign (VErtical Structure and Sources of AERosols in the Mediterranean Region) was designed to characterize the different sources of aerosol in the Mediterranean Basin and assess the regional impact of aerosol on cloud microphysical and radiative properties. VESSAER was conducted on an ultra-light aircraft in summer 2012. Research activities included ground-based observations in the central and northern regions of Corsica, as well as aerosol lidar and sunphotometer measurements near the eastern coast. The main scientific goals were to investigate local versus long-range sources of aerosol and cloud condensation nuclei (CCN) and their vertical stratification in the lower troposphere, study evolution and ageing due to atmospheric processes, and determine aerosol direct radiative impacts over a larger spatial scale. The background aerosol concentrations (D > 0.01 um) within the boundary layer in Corsica were nearly 2000 cm^-3 and increased to ca. 104 cm^-3 during pollution events when back-trajectories originated from coastal areas in France and Italy and the Po Valley. Nearly all of these particles were CCN-active at 0.38% supersaturation, indicating a relatively hygroscopic aerosol. Vertical profiles of aerosol hygroscopicity revealed that ageing (with respect to CCN-activity) of European emissions occurred exclusively in the boundary layer. Within two days, the European emissions had become hygroscopic, probably a result of cloud processing. In contrast, aerosol hygroscopicity did not change as a function of transport time in elevated aerosol layers, suggesting that photochemical ageing of less hygroscopic material is relatively slow compared to ageing processes in the boundary layer. The vertical profiles clearly showed the long-range transport of dust from the Saharan Desert and pollution from the European continent, which were the two major sources of aerosol during the campaign. Two of the research flights coincided with CALIPSO overpasses, when

  14. Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Slowik, J. G.; Richter, R.; Reche, C.; Alastuey, A.; Querol, X.; Seco, R.; Peñuelas, J.; Jiménez, J. L.; Crippa, M.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.

    2011-10-01

    PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O/C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O/C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the organic mass fragments at m/z 55, 57, and 44 is developed here and

  15. Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Slowik, J. G.; Richter, R.; Reche, C.; Alastuey, A.; Querol, X.; Seco, R.; Peñuelas, J.; Jiménez, J. L.; Crippa, M.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.

    2012-02-01

    PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional air quality and atmospheric parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O:C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O:C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the markers m/z 55, 57, and 44 is

  16. Use of multi-element tracers to source apportion mercury in south Florida aerosols

    NASA Astrophysics Data System (ADS)

    Graney, Joseph R.; Dvonch, J. Timothy; Keeler, Gerald J.

    The relative importance of local sources of mercury (Hg) in aerosols from urban areas in south Florida in relation to regional or global sources transported to the Everglades was investigated using a multi-element tracer approach. The sources of metals and Hg within aerosols were determined by integrating the collection of aerosols at seven locations with meteorology, source sampling, and statistical analysis. Sources include sea spray, soil dust from local carbonate bedrock and long range Saharan dust transport, regional scale transport of sulfate aerosols, and local point sources including oil-fired power plants, medical and waste incineration, and cement kilns. Using a principal components analysis-multiple linear regression (PCA-MLR) approach, 80% of the Hg in particulate form at the Thompson Park Everglades receptor site (THP) could be attributed to local sources. The key to the success of the source attribution at THP was collection of samples on a 12-h sampling basis in order to account for diurnal changes in meteorological conditions in south Florida associated with land-sea breeze development. Fifty-six±7% of the particulate Hg at THP was associated with elevated Zn concentrations which source sampling and surface meteorology indicate as emissions from municipal waste incineration located southeast of THP. Another 14±5% of the particulate Hg was associated with elevated Cu and Pb concentrations from sources SSE of THP. Eleven±1% of the particulate Hg originated from medical waste incineration sources and was associated with elevated levels of Cl and rapid SE to NW transport. Elevated concentrations of Si, Al, Fe, Mn, and K occurred on the same days at all sites, following passage of tropical storms over south Florida. PCA grouped these elements within a factor that is likely Saharan dust in origin, only 12±2% of the particulate Hg at THP could be attributed to this non-local source. Because the majority of the particulate Hg at THP can be attributed to

  17. Aerosol typing - key information from aerosol studies

    NASA Astrophysics Data System (ADS)

    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

  18. Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

    NASA Astrophysics Data System (ADS)

    Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

    2015-09-01

    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5-3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-]) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8-28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines

  19. Composition and sources of organic tracers in aerosol particles of industrial central India

    NASA Astrophysics Data System (ADS)

    Giri, Basant; Patel, Khageshwar S.; Jaiswal, Nitin K.; Sharma, Saroj; Ambade, Balram; Wang, Wentao; Simonich, Staci L. Massey; Simoneit, Bernd R. T.

    2013-02-01

    Organic aerosols are important atmospheric components, and their formation and sources represent important aspects of urban air quality and health effects. Asia, including India, is the largest global source of aerosol particles due to regional natural advection (e.g. desert and soil dust) and anthropogenic activities (e.g. emissions from traffic, industry and burning of coal, biomass and agricultural waste) that generate vast amounts of particulate matter (PM) significantly contributing to climate change. This article reports on the distributions, concentrations, and sources of organic compounds (i.e., alkanes, carboxylic acids, carbonyl compounds, alcohols, plasticizers, PAHs, biomarkers) of PM in the ambient atmosphere of an extensively industrialized area of central India (Raipur, Chhattisgarh, a coal mega-burning region). The dominant components are emissions from fossil fuel utilization, burning of biomass and plastics, and fugitive sources. Speciation and variations of potential new tracer compounds identified are also described.

  20. Relative Contributions of Fossil and Contemporary Carbon sources to PM 2.5 Aerosols at Nine IMPROVE Network Sites

    SciTech Connect

    Bench, G; Fallon, S; Schichtel, B; Malm, W; McDade, C

    2006-06-26

    Particulate matter aerosols contribute to haze diminishing vistas and scenery at National Parks and Wilderness Areas within the United States. To increase understanding of the sources of carbonaceous aerosols at these settings, the total carbon loading and {sup 14}C/C ratio of PM 2.5 aerosols at nine IMPROVE (Interagency Monitoring for Protection Of Visual Environments) network sites were measured. Aerosols were collected weekly in the summer and winter at one rural site, two urban sites, five sites located in National Parks and one site located in a Wildlife Preserve. The carbon measurements together with the absence of {sup 14}C in fossil carbon materials and the known {sup 14}C/C levels in contemporary carbon materials were used to derive contemporary and fossil carbon contents of the particulate matter. Contemporary and fossil carbon aerosol loadings varied across the sites and suggest different percentages of carbon source inputs. The urban sites had the highest fossil carbon loadings that comprised around 50% of the total carbon aerosol loading. The Wildlife Preserve and National Park sites together with the rural site had much lower fossil carbon loading components. At these sites, variations in the total carbon aerosol loading were dominated by non-fossil carbon sources. This suggests that reduction of anthroprogenic sources of fossil carbon aerosols may result in little decrease in carbonaceous aerosol loading at many National Parks and rural areas.

  1. Source strength of fungal spore aerosolization from moldy building material

    NASA Astrophysics Data System (ADS)

    Górny, Rafał L.; Reponen, Tiina; Grinshpun, Sergey A.; Willeke, Klaus

    The release of Aspergillus versicolor, Cladosporium cladosporioides, and Penicillium melinii spores from agar and ceiling tile surfaces was tested under different controlled environmental conditions using a newly designed and constructed aerosolization chamber. This study revealed that all the investigated parameters, such as fungal species, air velocity above the surface, texture of the surface, and vibration of contaminated material, affected the fungal spore release. It was found that typical indoor air currents can release up to 200 spores cm -2 from surfaces with fungal spores during 30-min experiments. The release of fungal spores from smooth agar surfaces was found to be inadequate for accurately predicting the emission from rough ceiling tile surfaces because the air turbulence increases the spore release from a rough surface. A vibration at a frequency of 1 Hz at a power level of 14 W resulted in a significant increase in the spore release rate. The release appears to depend on the morphology of the fungal colonies grown on ceiling tile surfaces including the thickness of conidiophores, the length of spore chains, and the shape of spores. The spores were found to be released continuously during each 30-min experiment. However, the release rate was usually highest during the first few minutes of exposure to air currents and mechanical vibration. About 71-88% of the spores released during a 30-min interval became airborne during the first 10 min.

  2. Unspeciated Organic Emissions From Combustion Sources And Their Influence On The Secondary Organic Aerosol Budget In The United States

    NASA Astrophysics Data System (ADS)

    Jathar, S.; Gordon, T.; Hennigan, C. J.; Pye, H. O.; Donahue, N. M.; Adams, P. J.; Robinson, A. L.

    2012-12-01

    Combustion sources are a major source of organic emissions and therefore a potentially important source for secondary organic aerosol (SOA) formation in the atmosphere. Although speciated organic emissions from combustion sources are considered in models to form SOA, a large fraction of the organics are unspeciated. In this work, we analyze data from numerous smog chamber experiments, which photo-oxidized dilute emissions from different combustion sources (on-road gasoline vehicles, aircraft, on-road diesel vehicles, wood burning and open biomass burning), to determine the contribution that unspeciated emissions make to SOA formation. An SOA model based on speciated organics is able to explain, on average, 8-31% of the SOA measured in the experiments. We hypothesize that the remainder results from the gas-phase oxidation of unspeciated emissions, which account on average for 25-75% of the non-methane organic gas (NMOG) emissions. Using the SOA data, we develop, for the first time, source-specific parameterizations to model SOA from unspeciated emissions; all sources seem to have median SOA yields similar to large n-alkanes (C12+). To assess the influence of unspeciated emissions on SOA formation regionally, we use the parameterization to predict SOA production in the United States. Using emissions data collected during the smog chamber experiments and data available in literature, we build a gross inventory for unspeciated emissions in the United States. We discover that unspeciated organics might be included in the current generation of SOA models but misallocated in terms of its SOA potential. The top six combustion sources (on- and off-road gasoline, on- and off-road diesel, open biomass and wood burning) emit 2.61 Tg yr-1 of unspeciated emissions (20% of US anthropogenic VOC emissions from combustion sources) and are estimated to form a minimum of 0.68 Tg yr-1 of SOA; the estimate is a third of the biogenic SOA produced in the US. We predict that accounting for

  3. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

    2012-02-01

    Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25-0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate

  4. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

    2011-10-01

    Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra in the m/z range 12-250 showing Pearson's r values >0.94 for the correlations between the different SOA types after 5 h of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxidized OA (SV-OOA) observed in the ambient aerosol. The atomic O : C ratios were found to be in the range of 0.25-0.55 with no major increase during the first 5 h of aging. On average, the diesel SOA showed the lowest O : C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions based on their carbon number revealed that the SOA source with the highest O : C ratio had the largest fraction of small ions. Fragment ions containing up to 3 carbon atoms accounted for 66%, 68%, 72% and 76% of the organic spectrum of the SOA produced by the diesel car, wood burner, α-pinene and

  5. Vertical Structure and Sources of Aerosols in the Mediterranean Region (VESSAER)

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Junkermann, W.; Leon, J.; Pont, V.; Mallet, M.; Augustin, P.; Dulac, F.

    2012-12-01

    The Mediterranean region has been identified as one of the most prominent global "Hot-Spots" in future climate change projections [Giorgi and Lionello, 2008] and is particularly characterized by its vulnerability to changes in the water cycle. To this end, the VESSAER campaign (VErtical Structure and Sources of AERosols in the Mediterranean Region) was designed to characterize the different sources of aerosol in the Mediterranean Basin and assess their regional impact on cloud microphysical and radiative properties. VESSAER was conducted on the ENDURO-KIT ultra-light aircraft [W. Junkermann, 2001] in late June-early July 2012. Activities include ground observations as well as aerosol lidar and sunphotometer measurements in conjunction with the airborne measurements. The VESSAER campaign complements existing ChArMEx (http://charmex.lsce.ipsl.fr/ ; PI: F. Dulac) and HyMeX (http://www.hymex.org/ ; PI: V. Ducroc and P. Drobinski) activities, which are the target of many European research institutes in 2012 and 2013. The main scientific goals during VESSAER are to investigate local versus long-range sources of aerosol and cloud condensation nuclei (CCN) and their vertical stratification in the lower troposphere, use aerosol hygroscopicity to study their evolution due to atmospheric processes, and couple in-situ airborne measurements with ground-based remote sensing to determine aerosol direct radiative impacts over a larger spatial scale. The background aerosol concentrations within the boundary layer (BL) in Corsica are nearly 2000 cm-3 (Dp > 10 nm); 50 cm-3 (Dp > 300 nm). We were surprised to find that nearly all of these particles are CCN-active at 0.3% supersaturation and presume that ageing and/or cloud processing play a role in rendering the aerosol in the Mediterranean Basin more hygroscopic. The vertical profiles during VESSAER clearly show the long-range transport of dust from the Saharan Desert and pollution from the European continent -- which were the two

  6. NEW TECHNOLOGY FOR THE CONTROL OF AEROSOLS FROM STATIONARY SOURCES

    EPA Science Inventory

    The paper discusses an EPA program to develop new technologies for controlling particulate matter from stationary sources, including both electrostatically augmented fabric filtration (ESFF) and electrostatic precipitators (ESPs). The first generation ESFF system, using an electr...

  7. HETEROGENEOUS SOOT NANOSTRUCTURE IN ATMOSPHERIC AND COMBUSTION SOURCE AEROSOLS

    EPA Science Inventory

    Microscopic images of soot emissions from wildfire and a wide range of anthropogenic combustion sources show that the nanostructures of individual particles in these emissions are predominantly heterogeneous, decidedly influenced by the fuel composition and by the particular comb...

  8. Global Distribution and Sources of Volatile and Nonvolatile Aerosol In the Remote Troposphere

    NASA Technical Reports Server (NTRS)

    Singh, Hanwant B.; Avery, M.; Viezee, W.; Che, Y.; Tabazadeh, A.; Hamill, P.; Pueschel, R.; Hannan, J. R.; Anderson, B.; Fuelberg, H. E.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    Airborne measurements of aerosol (Condensation Nuclei, CN) and selected trace gases made in the areas of the North Atlantic Ocean during SONEX (October/November 1997), and the south tropical Pacific Ocean during PEM-Tropics A (September/October 1996) and PEM-Tropics B (March/April 1999) have been analyzed. Emphasis is on the interpretations of variations in the number densities of the fine (>17 nm) and ultrafine (>8 nm) CN in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (10(exp 4)-10(exp 5)/cu cm) are present in the clean upper troposphere with highest values over the tropical1subtropical region. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosol particles behave in a manner similar to tracers of combustion (CO) and photochemical pollution (PAN), implying a source from continental pollution of industrial or biomass burning origin. In the upper troposphere, we find that volatile and nonvolatile partials number densities are inversely correlated. An aerosol microphysical model is used to suggest that coagulation of fine volatile particles with fewer larger nonvolatile particles provides one possible mechanism for this relationship. It appears that nonvolatile particles, of principally anthropogenic origin,provide a highly efficient removal process for the fine volatile aerosol.

  9. Atmospheric aerosol compositions and sources at two national background sites in northern and southern China

    NASA Astrophysics Data System (ADS)

    Zhu, Qiao; He, Ling-Yan; Huang, Xiao-Feng; Cao, Li-Ming; Gong, Zhao-Heng; Wang, Chuan; Zhuang, Xin; Hu, Min

    2016-08-01

    Although China's severe air pollution has become a focus in the field of atmospheric chemistry and the mechanisms of urban air pollution there have been researched extensively, few field sampling campaigns have been conducted at remote background sites in China, where air pollution characteristics on a larger scale are highlighted. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), together with an Aethalometer, was deployed at two of China's national background sites in northern (Lake Hongze site; 33.23° N, 118.33° E; altitude 21 m) and southern (Mount Wuzhi site; 18.84° N, 109.49° E; altitude 958 m) China in the spring seasons in 2011 and 2015, respectively, in order to characterize submicron aerosol composition and sources. The campaign-average PM1 concentration was 36.8 ± 19.8 µg m-3 at the northern China background (NCB) site, which was far higher than that at the southern China background (SCB) site (10.9 ± 7.8 µg m-3). Organic aerosol (OA) (27.2 %), nitrate (26.7 %), and sulfate (22.0 %) contributed the most to the PM1 mass at NCB, while OA (43.5 %) and sulfate (30.5 %) were the most abundant components of the PM1 mass at SCB, where nitrate only constituted a small fraction (4.7 %) and might have contained a significant amount of organic nitrates (5-11 %). The aerosol size distributions and organic aerosol elemental compositions all indicated very aged aerosol particles at both sites. The OA at SCB was more oxidized with a higher average oxygen to carbon (O / C) ratio (0.98) than that at NCB (0.67). Positive matrix factorization (PMF) analysis was used to classify OA into three components, including a hydrocarbon-like component (HOA, attributed to fossil fuel combustion) and two oxygenated components (OOA1 and OOA2, attributed to secondary organic aerosols from different source areas) at NCB. PMF analysis at SCB identified a semi-volatile oxygenated component (SV-OOA) and a low-volatility oxygenated

  10. Sources of anions in aerosols in northeast Greenland during late winter

    NASA Astrophysics Data System (ADS)

    Fenger, M.; Sørensen, L. L.; Kristensen, K.; Jensen, B.; Nquyen, Q. T.; Nøjgaard, J. K.; Massling, A.; Skov, H.; Glasius, M.

    2012-06-01

    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 the 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 analyze the 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 is a source of very coarse chloride particles in the Arctic.

  11. Sources of anions in aerosols in northeast Greenland during late winter

    NASA Astrophysics Data System (ADS)

    Fenger, M.; Sørensen, L. L.; Kristensen, K.; Jensen, B.; Nguyen, Q. T.; Nøjgaard, J. K.; Massling, A.; Skov, H.; Becker, T.; Glasius, M.

    2013-02-01

    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.

  12. Comparing Organic Aerosol Composition from Marine Biogenic Sources to Seawater and to Physical Sea Spray Models

    NASA Astrophysics Data System (ADS)

    Russell, L. M.; Frossard, A. A.; Sanchez, K.; Massoli, P.; Elliott, S.; Burrows, S. M.; Bates, T. S.; Quinn, P.

    2015-12-01

    In much of the marine atmosphere, organic components in aerosol particles have many sources other than sea spray that contribute organic constituents. For this reason, physical sea spray models provide an important technique for studying the organic composition of particles from marine biogenic sources. The organic composition of particles produced by two different physical sea spray models were measured in three open ocean seawater types: (i) Coastal California in the northeastern Pacific, which is influenced by wind-driven, large-scale upwelling leading to productive or eutrophic (nutrient-rich) seawater and high chl-a concentrations, (ii) George's Bank in the northwestern Atlantic, which is also influenced by nutrient upwelling and eutrophic seawater with phytoplankton productivity and high chl-a concentrations, and (iii) the Sargasso Sea in the subtropical western Atlantic, which is oligotrophic and nutrient-limited, reflected in low phytoplankton productivity and low chl-a concentrations. Fourier transform infrared spectroscopy provides information about the functional group composition that represents the marine organic fraction more completely than is possible with techniques that measure non-refractory mass (vaporizable at 650°C). After separating biogenic marine particles from those from other sources, the measured compositions of atmospheric marine aerosol particles from three ocean regions is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. The organic composition of atmospheric primary marine (ocean-derived) aerosol particles is nearly identical to model generated primary marine aerosol particles from bubbled seawater. Variability in productive and non-productive seawater may be caused by the presence of surfactants that can stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components without substantial changes in overall group composition

  13. Sources of primary and secondary organic aerosol and their diurnal variations.

    PubMed

    Zheng, Mei; Zhao, Xiuying; Cheng, Yuan; Yan, Caiqing; Shi, Wenyan; Zhang, Xiaolu; Weber, Rodney J; Schauer, James J; Wang, Xinming; Edgerton, Eric S

    2014-01-15

    PM(2.5), as one of the criteria pollutants regulated in the U.S. and other countries due to its adverse health impacts, contains more than hundreds of organic pollutants with different sources and formation mechanisms. Daytime and nighttime PM2.5 samples from the August Mini-Intensive Gas and Aerosol Campaign (AMIGAS) in the southeastern U.S. were collected during summer 2008 at one urban site and one rural site, and were analyzed for organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC), and various individual organic compounds including some important tracers for carbonaceous aerosol sources by gas chromatography-mass spectrometry. Most samples exhibited higher daytime OC concentration, while higher nighttime OC was found in a few events at the urban site. Sources, formation mechanisms and composition of organic aerosol are complicated and results of this study showed that it exhibited distinct diurnal variations. With detailed organic tracer information, sources contributing to particulate OC were identified: higher nighttime OC concentration occurring in several occasions was mainly contributed by the increasing primary emissions at night, especially diesel exhaust and biomass burning; whereas sources responsible for higher daytime OC concentration included secondary organic aerosol (SOA) formation (e.g., cis-pinonic acid and non-biomass burning WSOC) together with traffic emissions especially gasoline engine exhaust. Primary tracers from combustion related sources such as EC, polycyclic aromatic hydrocarbons, and hopanes and steranes were significantly higher at the urban site with an urban to rural ratio between 5 and 8. However, this urban-rural difference for secondary components was less significant, indicating a relatively homogeneous distribution of SOA spatially. We found cholesterol concentrations, a typical tracer for meat cooking, were consistently higher at the rural site especially during the daytime, suggesting the likely

  14. Chemical characterisation of atmospheric aerosols during a 2007 summer field campaign at Brasschaat, Belgium: sources and source processes of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Gómez-González, Y.; Wang, W.; Vermeylen, R.; Chi, X.; Neirynck, J.; Janssens, I. A.; Maenhaut, W.; Claeys, M.

    2012-01-01

    Measurements of organic marker compounds and inorganic species were performed on PM2.5 aerosols from a Belgian forest site that is severely impacted by urban pollution ("De Inslag", Brasschaat, Belgium) during a 2007 summer period within the framework of the "Formation mechanisms, marker compounds, and source apportionment for biogenic atmospheric aerosols (BIOSOL)" project. The measured organic species included (i) low-molecular weight (MW) dicarboxylic acids (LMW DCAs), (ii) methanesulfonate (MSA), (iii) terpenoic acids originating from the oxidation of α-pinene, β-pinene, d-limonene and Δ3-carene, and (iv) organosulfates related to secondary organic aerosol from the oxidation of isoprene and α-pinene. The organic tracers explained, on average, 5.3 % of the organic carbon (OC), of which 0.7 % was due to MSA, 3.4 % to LMW DCAs, 0.6 % to organosulfates, and 0.6 % to terpenoic acids. The highest atmospheric concentrations of most species were observed during the first five days of the campaign, which were characterised by maximum day-time temperatures >22 °C. Most of the terpenoic acids and the organosulfates peaked during day-time, consistent with their local photochemical origin. High concentrations of 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA) and low concentrations of cis-pinonic acid were noted during the first five days of the campaign, indicative of an aged biogenic aerosol. Several correlations between organic species were very high (r>0.85), high (0.70.7) and showed an Arrhenius-type relationship, consistent with their formation through OH radical chemistry.

  15. Long-term observations of aerosol size distributions in semi-clean and polluted savannah in South Africa

    NASA Astrophysics Data System (ADS)

    Vakkari, V.; Beukes, J. P.; Laakso, H.; Mabaso, D.; Pienaar, J. J.; Kulmala, M.; Laakso, L.

    2012-09-01

    originates from regional wild fires, while at Marikana domestic heating in the informal settlements is the main source. Air mass history analysis for Botsalano identified four regional scale source areas in Southern Africa and enabled the differentiation between fresh and aged rural background aerosol originating from the clean sector, i.e., western sector with very few large anthropogenic sources. Comparison to size distributions published for other comparable environments in Northern Hemisphere shows Southern African savannah to have a unique combination of sources and meteorological parameters. The observed strong link between combustion and seasonal variation is comparable only to the Amazon basin; however the lack of long-term observations in the Amazonas does not allow a quantitative comparison. All the data presented in the figures, as well as the time series of monthly mean and median size distributions are included in numeric form as a Supplement to provide a reference point for the aerosol modelling community.

  16. Long-term observations of aerosol size distributions in semi-clean and polluted savannah in South Africa

    NASA Astrophysics Data System (ADS)

    Vakkari, V.; Beukes, J. P.; Laakso, H.; Mabaso, D.; Pienaar, J. J.; Kulmala, M.; Laakso, L.

    2013-02-01

    concentration originates from regional wild fires, while at Marikana domestic heating in the informal settlements is the main source. Air mass history analysis for Botsalano identified four regional scale source areas in southern Africa and enabled the differentiation between fresh and aged rural background aerosol originating from the clean sector, i.e., western sector with very few large anthropogenic sources. Comparison to size distributions published for other comparable environments in Northern Hemisphere shows southern African savannah to have a unique combination of sources and meteorological parameters. The observed strong link between combustion and seasonal variation is comparable only to the Amazon basin; however, the lack of long-term observations in the Amazonas does not allow a quantitative comparison. All the data presented in the figures, as well as the time series of monthly mean and median size distributions are included in numeric form as a Supplement to provide a reference point for the aerosol modelling community.

  17. Phase 1 immobilized low-activity waste operational source term

    SciTech Connect

    Burbank, D.A.

    1998-03-06

    This report presents an engineering analysis of the Phase 1 privatization feeds to establish an operational source term for storage and disposal of immobilized low-activity waste packages at the Hanford Site. The source term information is needed to establish a preliminary estimate of the numbers of remote-handled and contact-handled waste packages. A discussion of the uncertainties and their impact on the source term and waste package distribution is also presented. It should be noted that this study is concerned with operational impacts only. Source terms used for accident scenarios would differ due to alpha and beta radiation which were not significant in this study.

  18. Impact of interannual variations in aerosol particle sources on orographic precipitation over California's Central Sierra Nevada

    NASA Astrophysics Data System (ADS)

    Creamean, J. M.; Ault, A. P.; White, A. B.; Neiman, P. J.; Ralph, F. M.; Minnis, P.; Prather, K. A.

    2015-01-01

    Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater field campaign (2009-2011), the variability and associated impacts of different aerosol sources on precipitation were investigated in the California Sierra Nevada using an aerosol time-of-flight mass spectrometer for precipitation chemistry, S-band profiling radar for precipitation classification, remote sensing measurements of cloud properties, and surface meteorological measurements. The composition of insoluble residues in precipitation samples collected at a surface site contained mostly local biomass burning and long-range transported dust and biological particles (2009), local sources of biomass burning and pollution (2010), and long-range transport from distant sources (2011). Although differences in the sources were observed from year-to-year, the most consistent source of dust and biological residues were associated with storms consisting of deep convective cloud systems with significant quantities of precipitation initiated in the ice phase. Further, biological residues were dominant (up to 40%) during storms with relatively warm cloud temperatures (up to -15 °C), supporting the important role bioparticles can play as ice nucleating particles. On the other hand, lower percentages of residues from local biomass burning and pollution were observed over the three winter seasons (on average 31 and 9%, respectively). When precipitation quantities were relatively low, these residues most likely served as CCN, forming smaller more numerous cloud droplets at the base of shallow cloud systems, and resulting in less efficient riming processes. The correlation between the source of aerosols within clouds and precipitation type and quantity will be further probed in models to understand the

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

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-12-01

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

  20. Contributions of local sources, long-range and mountain wind transport for aerosols over an eastern Himalayan high-altitude station in India

    NASA Astrophysics Data System (ADS)

    Chatterjee, Abhijit; Sarkar, Chirantan; Singh, Ajay; Ghosh, Sanjay; Raha, Sibaji; Das, Sanat

    A long-term study (2010-2013) on aerosols mass concentrations (PM2.5), number concentrations of size segregated aerosols and mass concentration of total suspended black carbon aerosols has been made over Darjeeling (27.01 N, 88.15 E), a high altitude (2200 m asl) station at eastern Himalaya in India. Seasonal and diurnal variation of all types of aerosols, their chemical composition and source apportionment revealed that aerosols over this part of Himalaya are mainly of two types; locally generated and long-range transported aerosols. The diurnal variation of aerosols including black carbon showed distinct feature of up-slope mountain wind transport mainly during premonsoon (Mar-May) which brings aerosol particles from low land regions. This present study focuses on the estimation of the individual contributions from local emissions (LE), long-range transport (LRT) and mountain wind transport (MWT) towards the total aerosol loading over Darjeeling. Several strike events (called by local political party) were observed at Darjeeling over the entire period of study (2008-2013) when all the local activities (schools, colleges, offices, vehicular, industrial etc) were stopped fully. Most of the strike events occurred during premonsoon. We have observed three types of events during premonsoon over the entire study period; 1) strike events with the contribution of LRT+MWT with zero local emissions (LE=0), 2) normal days with the contribution of LE+LRT+MWT, 3) normal days with the contribution of LE+MWT with zero long-range contribution (LRT=0). On normal days, the diurnal variation of aerosols during premonsoon showed sharp morning and evening peaks associated to local anthropogenic activities with the effect of up-slope mountain wind during afternoon. During strike events, the morning and evening peaks were absent but a broad peak was observed during afternoon associated to up-slope mountain wind. The increase in aerosol concentrations during afternoon on strike days

  1. Tropospheric entrainment as a source of ground level aerosols within the polar Antarctic cell

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Schofield, R.; Keywood, M.; Wilson, S. R.; Klekociuk, A. R.; Paton-Walsh, C.

    2013-12-01

    region which, being a sea-ice/ocean region, is a significant precursor source compared to the continent. After tropospheric formation, populations descending at the poles are transported northward and reach the surface at the edge of the continent. Current measurements of Antarctic aerosol suggest very low loading which may be explained by these circulation patterns and as such, may underestimate the total loading in this region as well as the contribution of aerosol production in this region to global loading. As climate change intensifies and the ozone hole recovers, the polar Antarctic front may shift latitudes, potentially changing Antarctic aerosol loading, resulting in changes to tropospheric and stratospheric chemistry and reducing transport to other global regions.

  2. Long-term Observation of Aerosol Optical Properties at the SORPES station in Nanjing, China

    NASA Astrophysics Data System (ADS)

    Shen, Yicheng; Ding, Aijun; Virkkula, Aki; Wang, Jiaping; Chi, Xuguang; Qi, Ximeng; Liu, Qiang; Zheng, Longfei; Xie, Yuning

    2016-04-01

    Atmospheric aerosols influence the earth's radiation budget by scattering and absorbing solar radiation and contribute substantial uncertainty in the estimation of climate forcing. Thorough and comprehensive measurements on different parameters including absorption and scattering coefficient, wavelength dependence and angular dependence along with their daily and seasonal variation help to understand the influence of aerosol on radiation. 2-years continuous measurement of aerosol optical properties has been conducted from June 2013 to May 2015 at the Station for Observing Regional Process of Earth System (SORPES) station, which is a regional background station located in downwind direction of Yangtze River Delta (YRD) urban agglomeration in China. A 7-wavelenths aethalometer and a 3-wavelenths nephelometer were used to measure absorption and scattering coefficient, and also other parameters like single scattering albedo (SSA), absorption angstrom Exponent (AAE), scattering angstrom exponent (SAE) and back-scattering refraction. In addtion, simultaneous measurements on chemical composition and particle size distribution were performed so as to investigate the dependencies of aerosol optical properties on chemical composition and size distribution. To get further insight on the influencing factors, Lagrangian particle dispersion modeling (LPDM) was employed for source identification in this study. The averages of absorption coefficient, scattering coefficient and SSA are 26.0±18.7 Mm-1, 426±327 Mm-1 , 0.936±0.3 at 520nm respectively for whole period. SAE between 450 and 635nm is 1.299±0.34 and have strong negative correlation with particle Surface Mean Diameter (SMD). AAE between 370 and 950nm is 1.043±0.15 for whole period but growth to more than 1.6 in all identified Biomass Burning (BB) events.

  3. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China

    PubMed Central

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-01-01

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ34Ssulfate and δ18Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ34S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ34Ssulfate and δ18Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere. PMID:27435991

  4. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China.

    PubMed

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-01-01

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ(34)Ssulfate and δ(18)Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ(34)S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ(34)Ssulfate and δ(18)Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere. PMID:27435991

  5. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China

    NASA Astrophysics Data System (ADS)

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-07-01

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ34Ssulfate and δ18Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ34S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ34Ssulfate and δ18Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere.

  6. Analysis of Three-Dimensional Aerosol Deposition in Pharmacologically Relevant Terms: Beyond Black or White ROIs

    PubMed Central

    Greenblatt, Elliot Eliyahu; Winkler, Tilo; Harris, Robert Scott; Kelly, Vanessa Jane; Kone, Mamary

    2015-01-01

    Abstract Background: This article presents a novel methodological approach to evaluate images of aerosol deposition taken with PET-CT cameras. Traditionally, Black-or-White (BW) Regions of Interest (ROIs) are created to cover Anatomical Regions (ARs) segmented from the high-resolution CT. Such ROIs do not usually consider blurring effects due to limited spatial resolution or breathing motion, and do not consider uncertainty in the AR position within the PET image. The new methodology presented here (Grayscale) addresses these issues, allows estimates of aerosol deposition within ARs, and expresses the deposition in terms of Tissue Dosing (in the lung periphery) and Inner Surface Concentration (in the larger airways). Methods: Imaging data included a PET deposition image acquired during breathing and two CT scans acquired during breath holds at different lung volumes. The lungs were segmented into anatomically consistent ARs to allow unbiased comparisons across subjects and across lobes. The Grayscale method involves defining Voxel Influence Matrices (VIMs) to consider how average activity within each AR influences the measured activity within each voxel. The BW and Grayscale methods were used to analyze aerosol deposition in 14 bronchoconstricted asthmatics. Results: Grayscale resulted in a closer description of the PET image than BW (p<0.0001) and exposed a seven-fold underestimation in measures of specific deposition. The Average Tissue Dosing was 2.11×10−6 Total Lung Dose/mg. The average Inner Surface Concentration was 45×10−6 Total Lung Dose/mm2, with the left lower lobe having a lower ISC than lobes of the right lung (p<0.05). There was a strong lobar heterogeneity in these measures (COV=0.3). Conclusion: The Grayscale approach is an improvement over the BW approach and provides a closer description of the PET image. It can be used to characterize heterogeneous concentrations throughout the lung and may be important in translational research and in the

  7. Source Tracking Aerosols Released from Land-Applied Class B Biosolids during High-Wind Events▿

    PubMed Central

    Baertsch, Carolina; Paez-Rubio, Tania; Viau, Emily; Peccia, Jordan

    2007-01-01

    DNA-based microbial source tracking (MST) methods were developed and used to specifically and sensitively track the unintended aerosolization of land-applied, anaerobically digested sewage sludge (biosolids) during high-wind events. Culture and phylogenetic analyses of bulk biosolids provided a basis for the development of three different MST methods. They included (i) culture- and 16S rRNA gene-based identification of Clostridium bifermentans, (ii) direct PCR amplification and sequencing of the 16S rRNA gene for an uncultured bacterium of the class Chloroflexi that is commonly present in anaerobically digested biosolids, and (iii) direct PCR amplification of a 16S rRNA gene of the phylum Euryarchaeota coupled with terminal restriction fragment length polymorphism to distinguish terminal fragments that are unique to biosolid-specific microorganisms. Each method was first validated with a broad group of bulk biosolids and soil samples to confirm the target's exclusive presence in biosolids and absence in soils. Positive responses were observed in 100% of bulk biosolid samples and in less than 11% of the bulk soils tested. Next, a sampling campaign was conducted in which all three methods were applied to aerosol samples taken upwind and downwind of fields that had recently been land applied with biosolids. When average wind speeds were greater than 5 m/s, source tracking results confirmed the presence of biosolids in 56% of the downwind samples versus 3% of the upwind samples. During these high-wind events, the biosolid concentration in downwind aerosols was between 0.1 and 2 μg/m3. The application of DNA-based source tracking to aerosol samples has confirmed that wind is a possible mechanism for the aerosolization and off-site transport of land-applied biosolids. PMID:17513591

  8. Source tracking aerosols released from land-applied class B biosolids during high-wind events.

    PubMed

    Baertsch, Carolina; Paez-Rubio, Tania; Viau, Emily; Peccia, Jordan

    2007-07-01

    DNA-based microbial source tracking (MST) methods were developed and used to specifically and sensitively track the unintended aerosolization of land-applied, anaerobically digested sewage sludge (biosolids) during high-wind events. Culture and phylogenetic analyses of bulk biosolids provided a basis for the development of three different MST methods. They included (i) culture- and 16S rRNA gene-based identification of Clostridium bifermentans, (ii) direct PCR amplification and sequencing of the 16S rRNA gene for an uncultured bacterium of the class Chloroflexi that is commonly present in anaerobically digested biosolids, and (iii) direct PCR amplification of a 16S rRNA gene of the phylum Euryarchaeota coupled with terminal restriction fragment length polymorphism to distinguish terminal fragments that are unique to biosolid-specific microorganisms. Each method was first validated with a broad group of bulk biosolids and soil samples to confirm the target's exclusive presence in biosolids and absence in soils. Positive responses were observed in 100% of bulk biosolid samples and in less than 11% of the bulk soils tested. Next, a sampling campaign was conducted in which all three methods were applied to aerosol samples taken upwind and downwind of fields that had recently been land applied with biosolids. When average wind speeds were greater than 5 m/s, source tracking results confirmed the presence of biosolids in 56% of the downwind samples versus 3% of the upwind samples. During these high-wind events, the biosolid concentration in downwind aerosols was between 0.1 and 2 microg/m3. The application of DNA-based source tracking to aerosol samples has confirmed that wind is a possible mechanism for the aerosolization and off-site transport of land-applied biosolids. PMID:17513591

  9. Long-Term Evolution of the Aerosol Debris Cloud Produced by the 2009 Impact on Jupiter

    NASA Technical Reports Server (NTRS)

    Sanchez-Lavega, A.; Orton, G. S.; Hueso, R.; Perez-Hoyos, S.; Fletcher, L. N.; Garcia-Melendo, E.; Gomez-Forrellad, J. M.; de Pater, I.; Wong, M.; Hammel. H. B.; Yanamandra-Fisher, P.; Simon-Miller, A.; Barrado-Izagirre, N.; Marchis, F.; Mousis, O.; Oritz, J. L.; Garcia-Rojas, J.; Cecconi, M.; Clarke, J. T.; Noll, K.; Pedraz, S.; Wesley, A.; Kalas, P.; McConnell, N.; Golisch, W.

    2011-01-01

    We present a study of the long-term evolution of the cloud of aerosols produced in the atmosphere of Jupiter by the impact of an object on 19 July 2009. The work is based on images obtained during 5 months from the impact to 31 December 2009 taken in visible continuum wavelengths and from 20 July 2009 to 28 May 2010 taken in near-infrared deep hydrogen-methane absorption bands at 2.1-2.3 micron. The impact cloud expanded zonally from approximately 5000 km (July 19) to 225,000 km (29 October, about 180 deg in longitude), remaining meridionally localized within a latitude band from 53.5 deg S to 61.5 deg S planetographic latitude. During the first two months after its formation the site showed heterogeneous structure with 500-1000 km sized embedded spots. Later the reflectivity of the debris field became more homogeneous due to clump mergers. The cloud was mainly dispersed in longitude by the dominant zonal winds and their meridional shear, during the initial stages, localized motions may have been induced by thermal perturbation caused by the impact's energy deposition. The tracking of individual spots within the impact cloud shows that the westward jet at 56.5 deg S latitude increases its eastward velocity with altitude above the tropopause by 5- 10 m/s. The corresponding vertical wind shear is low, about 1 m/s per scale height in agreement with previous thermal wind estimations. We found evidence for discrete localized meridional motions with speeds of 1-2 m/s. Two numerical models are used to simulate the observed cloud dispersion. One is a pure advection of the aerosols by the winds and their shears. The other uses the EPIC code, a nonlinear calculation of the evolution of the potential vorticity field generated by a heat pulse that simulates the impact. Both models reproduce the observed global structure of the cloud and the dominant zonal dispersion of the aerosols, but not the details of the cloud morphology. The reflectivity of the impact cloud decreased

  10. New developments in the representation of Saharan dust sources in the aerosol-climate model ECHAM6-HAM2

    NASA Astrophysics Data System (ADS)

    Heinold, Bernd; Tegen, Ina; Schepanski, Kerstin; Banks, Jamie R.

    2016-02-01

    In the aerosol-climate model ECHAM6-HAM2, dust source activation (DSA) observations from Meteosat Second Generation (MSG) satellite are proposed to replace the original source area parameterization over the Sahara Desert. The new setup is tested in nudged simulations for the period 2007 to 2008. The evaluation is based on comparisons to dust emission events inferred from MSG dust index imagery, Aerosol Robotic Network (AERONET) sun photometer observations, and satellite retrievals of aerosol optical thickness (AOT).The model results agree well with AERONET measurements especially in terms of seasonal variability, and a good spatial correlation was found between model results and MSG-SEVIRI (Spinning-Enhanced Visible and InfraRed Imager) dust AOT as well as Multi-angle Imaging SpectroRadiometer (MISR) AOT. ECHAM6-HAM2 computes a more realistic geographical distribution and up to 20 % higher annual Saharan dust emissions, using the MSG-based source map. The representation of dust AOT is partly improved in the southern Sahara and Sahel. In addition, the spatial variability is increased towards a better agreement with observations depending on the season. Thus, using the MSG DSA map can help to circumvent the issue of uncertain soil input parameters.An important issue remains the need to improve the model representation of moist convection and stable nighttime conditions. Compared to sub-daily DSA information from MSG-SEVIRI and results from a regional model, ECHAM6-HAM2 notably underestimates the important fraction of morning dust events by the breakdown of the nocturnal low-level jet, while a major contribution is from afternoon-to-evening emissions.

  11. 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

    NASA Astrophysics Data System (ADS)

    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

  12. Organic aerosols

    SciTech Connect

    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.

  13. Differences in the OC/EC Ratios that Characterize Ambient and Source Aerosols due to Thermal-Optical Analysis

    EPA Science Inventory

    Thermal-optical analysis (TOA) is typically used to measure the OC/EC (organic carbon/elemental carbon) and EC/TC (elemental carbon/total carbon) ratios in source and atmospheric aerosols. The present study utilizes a dual-optical carbon aerosol analyzer to examine the effects of...

  14. Regional source identification of atmospheric aerosols in Beijing based on sulfur isotopic compositions

    NASA Astrophysics Data System (ADS)

    Lianfang, Wei; Pingqing, Fu; Xiaokun, Han; Qingjun, Guo; Yele, Sun; Zifa, Wang

    2016-04-01

    65 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months representing the four seasons between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate aerosols were analyzed systematically. The "fingerprint" characteristics of the stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 and potential source contribution function (PSCF), were employed for identifying potential regional sources. Results obviously exhibited the distinctive seasonality for various aerosol speciation associated with PM2.5 in Beijing with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species. Elevated chloride associated with higher concentration of organics were found in autumn and winter, due to enhanced coal combustion emissions. The δ34S values of Beijing aerosol samples ranged from 2.94‰ to 10.2‰ with an average value of 6.18±1.87‰ indicating that the major sulfur source is direct fossil fuel burning-related emissions. Owning to a temperature-dependent fractionation and elevated biogenic sources of isotopically light sulfur in summer, the δ34S values had significant seasonal variations with a winter maximum ( 8.6‰)and a summer minimum ( 5.0‰). The results of trajectory clustering and the PSCF method demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios ( 4.83‰) were associated with air masses from the south, southeast or east, whereas lower sulfate concentrations with higher δ34S values ( 6.69‰) when the air masses were mainly from north or northwest. These results suggested two main different kinds of regional coal combustion sources contributed to the pollution in Beijing.

  15. Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation over California's Central Sierra Nevada

    NASA Astrophysics Data System (ADS)

    Creamean, J.; Ault, A. P.; White, A. B.; Neiman, P. J.; Minnis, P.; Prather, K. A.

    2014-12-01

    Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada Mountains. In 2009, the precipitation collected on the ground was influenced by both local biomass burning and long-range transported dust and biological particles, while in 2010, by mostly local sources of biomass burning and pollution, and in 2011 by mostly long-range transport of dust and biological particles from distant sources. Although vast differences in the sources of residues were observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15°C), suggesting biological components were more efficient IN than mineral dust. On the other hand, when precipitation quantities were lower, local biomass burning and pollution residues were observed (on average 31% and 9%, respectively), suggesting these residues potentially served as CCN at the base of shallow cloud systems and that lower level polluted clouds of storm systems produced less precipitation than non-polluted (i.e., marine) clouds. The direct connection of the sources of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource

  16. Five primary sources of organic aerosols in the urban atmosphere of Belgrade (Serbia).

    PubMed

    Zangrando, Roberta; Barbaro, Elena; Kirchgeorg, Torben; Vecchiato, Marco; Scalabrin, Elisa; Radaelli, Marta; Đorđević, Dragana; Barbante, Carlo; Gambaro, Andrea

    2016-11-15

    Biomass burning and primary biological aerosol particles (PBAPs) represent important primary sources of organic compounds in the atmosphere. These particles and compounds are able to affect climate and human health. In the present work, using HPLC-orbitrapMS, we determined the atmospheric concentrations of molecular markers such as anhydrosugars and phenolic compounds that are specific for biomass burning, as well as the concentrations of sugars, alcohol sugars and d- and l-amino acids (D-AAs and L-AAs) for studying PBAPs in Belgrade (Serbia) aerosols collected in September-December 2008. In these samples, high levels of all these biomarkers were observed in October. Relative percentages of vanillic (V), syringic compounds (S) and p-coumaric acid (PA), as well as levoglucosan/mannosan (L/M) ratios, helped us discriminate between open fire events and wood combustion for domestic heating during the winter. L-AAs and D-AAs (1% of the total) were observed in Belgrade aerosols mainly in September-October. During open fire events, mean D-AA/L-AA (D/L) ratio values of aspartic acid, threonine, phenylalanine, alanine were significantly higher than mean D/L values of samples unaffected by open fire. High levels of AAs were observed for open biomass burning events. Thanks to four different statistical approaches, we demonstrated that Belgrade aerosols are affected by five sources: a natural source, a source related to fungi spores and degraded material and three other sources linked to biomass burning: biomass combustion in open fields, the combustion of grass and agricultural waste and the combustion of biomass in stoves and industrial plants. The approach employed in this work, involving the determination of specific organic tracers and statistical analysis, proved useful to discriminate among different types of biomass burning events. PMID:27450960

  17. Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation Over California's Central Sierra Nevada

    NASA Technical Reports Server (NTRS)

    Creamean, J. M.; Ault, A. P.; White, A. B.; Neiman, P. J.; Ralph, F. M.; Minnis, Patrick; Prather, K. A.

    2014-01-01

    Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada. In 2009, the precipitation collected on the ground was influenced by both local biomass burning (up to 79% of the insoluble residues found in precipitation) and long-range transported dust and biological particles (up to 80% combined), while in 2010, by mostly local sources of biomass burning and pollution (30-79% combined), and in 2011 by mostly long-range transport from distant sources (up to 100% dust and biological). Although vast differences in the source of residues was observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15 C), suggesting these particles were more efficient IN compared to mineral dust. On the other hand, lower percentages of residues from local biomass burning and pollution were observed (on average 31% and 9%, respectively), yet these residues potentially served as CCN at the base of shallow cloud systems when precipitation quantities were low. The direct connection of the source of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource management.

  18. Molecular marker characterization and source appointment of particulate matter and its organic aerosols.

    PubMed

    Choi, Jong-Kyu; Ban, Soo-Jin; Kim, Yong-Pyo; Kim, Yong-Hee; Yi, Seung-Muk; Zoh, Kyung-Duk

    2015-09-01

    This study was carried out to identify possible sources and to estimate their contribution to total suspended particle (TSP) organic aerosol (OA) contents. A total of 120 TSP and PM2.5 samples were collected simultaneously every third day over a one-year period in urban area of Incheon, Korea. High concentration in particulate matters (PM) and its components (NO3(-), water soluble organic compounds (WSOCs), and n-alkanoic acids) were observed during the winter season. Among the organics, n-alkanes, n-alkanoic acids, levoglucosan, and phthalates were major components. Positive matrix factorization (PMF) analysis identified seven sources of organic aerosols including combustion 1 (low molecular weight (LMW)-polycyclic aromatic hydrocarbons (PAHs)), combustion 2 (high molecular weight (HMW)-PAHs), biomass burning, vegetative detritus (n-alkane), secondary organic aerosol 1 (SOA1), secondary organic aerosol 2 (SOA2), and motor vehicles. Vegetative detritus increased during the summer season through an increase in biogenic/photochemical activity, while most of the organic sources were prominent in the winter season due to the increases in air pollutant emissions and atmospheric stability. The correlation factors were high among the main components of the organic carbon (OC) in the TSP and PM2.5. The results showed that TSP OAs had very similar characteristics to the PM2.5 OAs. SOA, combustion (PAHs), and motor vehicle were found to be important sources of carbonaceous PM in this region. Our results imply that molecular markers (MMs)-PMF model can provide useful information on the source and characteristics of PM. PMID:26022138

  19. Global combustion sources of organic aerosols: model comparison with 84 AMS factor-analysis data sets

    NASA Astrophysics Data System (ADS)

    Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

    2016-07-01

    Emissions of organic compounds from biomass, biofuel, and fossil fuel combustion strongly influence the global atmospheric aerosol load. Some of the organics are directly released as primary organic aerosol (POA). Most are emitted in the gas phase and undergo chemical transformations (i.e., oxidation by hydroxyl radical) and form secondary organic aerosol (SOA). In this work we use the global chemistry climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) with a computationally efficient module for the description of organic aerosol (OA) composition and evolution in the atmosphere (ORACLE). The tropospheric burden of open biomass and anthropogenic (fossil and biofuel) combustion particles is estimated to be 0.59 and 0.63 Tg, respectively, accounting for about 30 and 32 % of the total tropospheric OA load. About 30 % of the open biomass burning and 10 % of the anthropogenic combustion aerosols originate from direct particle emissions, whereas the rest is formed in the atmosphere. A comprehensive data set of aerosol mass spectrometer (AMS) measurements along with factor-analysis results from 84 field campaigns across the Northern Hemisphere are used to evaluate the model results. Both the AMS observations and the model results suggest that over urban areas both POA (25-40 %) and SOA (60-75 %) contribute substantially to the overall OA mass, whereas further downwind and in rural areas the POA concentrations decrease substantially and SOA dominates (80-85 %). EMAC does a reasonable job in reproducing POA and SOA levels during most of the year. However, it tends to underpredict POA and SOA concentrations during winter indicating that the model misses wintertime sources of OA (e.g., residential biofuel use) and SOA formation pathways (e.g., multiphase oxidation).

  20. Dust Aerosols at the Source Region During ACE-ASIA: A Surface/Satellite Perspective

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee; Lau, William K. M. (Technical Monitor)

    2001-01-01

    ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

  1. Global modeling study of potentially bioavailable iron input from shipboard aerosol sources to the ocean

    NASA Astrophysics Data System (ADS)

    Ito, Akinori

    2013-01-01

    Iron (Fe) is an essential element for phytoplankton. The majority of iron is transported from arid and semiarid regions to the open ocean, but it is mainly in an insoluble form. Since most aquatic organisms can take up iron only in the dissolved form, aerosol iron solubility is a key factor that can influence the air-sea CO2 fluxes and thus climate. Field observations have shown relatively high iron solubility in aerosols influenced by combustion sources, but specific emissions sources and their contributions to deposition fluxes largely remain uncertain. Here a global chemical transport model was used to investigate the effect of aerosol emissions from ship plumes on iron solubility in particles from the combustion and dust sources. The model results reveal that the oil combustion from shipping mainly contributes to high iron solubility (>10%) at low iron loading (1-110 ng m-3) observed over the high-latitude North Atlantic Ocean, rather than the other combustion sources from continental industrialized regions. Due to continuing growth in global shipping and no regulations regarding particles emissions over the open ocean, the input of potentially bioavailable iron from ship plumes is likely to increase during the next century. The model results suggest that deposition of soluble iron from ships in 2100 contributes 30-60% of the soluble iron deposition over the high-latitude North Atlantic and North Pacific.

  2. Source contributions of sulfate aerosol over East Asia estimated by CMAQ-DDM.

    PubMed

    Itahashi, Syuichi; Uno, Itsushi; Kim, Soontae

    2012-06-19

    We applied the decoupled direct method (DDM), a sensitivity analysis technique for computing sensitivities accurately and efficiently, to determine the source-receptor relationships of anthropogenic SO(2) emissions to sulfate aerosol over East Asia. We assessed source contributions from East Asia being transported to Oki Island downwind from China and Korea during two air pollution episodes that occurred in July 2005. The contribution from China, particularly that from central eastern China (CEC), was found to dominate the sulfate aerosols. To study these contributions in more detail, CEC was divided into three regions, and the contributions from each region were examined. Source contributions exhibited both temporal and vertical variability, largely due to transport patterns imposed by the Asian summer monsoon. Our results are consistent with backward trajectory analyses. We found that anthropogenic SO(2) emissions from China produce significant quantities of summertime sulfate aerosols downwind of source areas. We used a parametric scaling method for estimating anthropogenic SO(2) emissions in China. Using column amounts of SO(2) derived from satellite data, and relationships between the column amounts of SO(2) and anthropogenic emissions, 2009 emissions were diagnosed. The results showed that 2009 emissions of SO(2) from China were equivalent to 2004 levels. PMID:22642816

  3. Sources and formation pathways of organic aerosol in a subtropical metropolis during summer

    NASA Astrophysics Data System (ADS)

    Tsai, I.-Chun; Chen, Jen-Ping; Lung, Candice Shi-Chun; Li, Nan; Chen, Wei-Nai; Fu, Tzung-May; Chang, Chih-Chung; Hwang, Gong-Do

    2015-09-01

    A field campaign combined with numerical simulations was designed to better understand the emission sources and formation processes of organic aerosols (OA) in a subtropical environment. The field campaign measured total and water soluble organic carbon (OC) in aerosol, as well as its precursor gases in the Taipei metropolis and a nearby rural forest during the summer of 2011. A regional air-quality model modified with an additional secondary organic aerosol (SOA) formation pathway was used to decipher the observed variations in OA, with focus on various formation pathways and the relative contributions from anthropogenic and biogenic sources. According to the simulations, biogenic sources contributed to 60% and 72% of total OA production at the NTU (urban) and HL (rural) sites. The simulated fractions of SOA in total OA were 67% and 79% near the surface of NTU and HL, respectively, and these fractions increased with height and reach over 90% at the 1-km altitude. Estimated from the simulation results, aqueous-phase dicarbonyl uptake was responsible of 51% of OA production in the urban area, while the primary emissions, reversible partitioning of semi-volatile oxidation products, oligomerization of semi-volatile SOA in the particulate phase and acid-enhanced oxidation contributed to 33%, 10%, 5% and 1% respectively; in the rural area, the percentages were 59%, 21%, 13%, 7% and 1%, respectively. Meteorological factors, including large-scale wind direction, local circulation and planetary boundary layer height, all have strong influences on the source contributions and diurnal variations of OA concentration.

  4. Long-Term Variation of Stratospheric Aerosols Observed With Lidar from 1982 to 2014 Over Tsukuba, Japan

    NASA Astrophysics Data System (ADS)

    Sakai, Tetsu; Uchino, Osamu; Nagai, Tomohiro; Fujimoto, Toshifumi; Tabata, Isao

    2016-06-01

    The vertical distribution of stratospheric aerosols has been measured with lidars at the Meteorological Research Institute (MRI) over Tsukuba since 1982. After two major volcanic eruptions (Mt. El Chichón in 1982 and Mt. Pinatubo in 1991), stratospheric aerosol loading increased about 50-100 times compared with the background level which was observed for 1997-2000. From 2000 to 2012, a slight increase (5.3% year-1) was observed by some volcanic eruptions. This long-term lidar data have been used for assessing of impact of the stratospheric aerosols on climate and the ozone layer.

  5. Optimum target source term estimation for high energy electron accelerators

    NASA Astrophysics Data System (ADS)

    Nayak, M. K.; Sahu, T. K.; Nair, Haridas G.; Nandedkar, R. V.; Bandyopadhyay, Tapas; Tripathi, R. M.; Hannurkar, P. R.

    2016-05-01

    Optimum target for bremsstrahlung emission is defined as the thickness of the target material, which produces maximum bremsstrahlung yield, on interaction of electron with the target. The bremsstrahlung dose rate per unit electron beam power at a distance of 1 m from the target material gives the optimum target source term. In the present work, simulations were performed for three different electron energies, 450, 1000 and 2500 MeV using EGSnrc Monte-Carlo code to determine the optimum thickness. An empirical relation for optimum target as a function of electron energy and atomic number of the target materials is found out from results. Using the simulated optimum target thickness, experiments are conducted to determine the optimum target source term. For the experimental determination, two available electron energies, 450 MeV and 550 MeV from booster synchrotron of Indus facility is used. The optimum target source term for these two energies are also simulated. The experimental and simulated source term are found to be in very good agreement within ±3%. Based on the agreement of the simulated source term with the experimental source term at 450 MeV and 550 MeV, the same simulation methodology is used to simulate optimum target source term up to 2500 MeV. The paper describes the simulations and experiments carried out on optimum target bremsstrahlung source term and the results obtained.

  6. Oil sands operations as a large source of secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Liggio, John; Li, Shao-Meng; Hayden, Katherine; Taha, Youssef M.; Stroud, Craig; Darlington, Andrea; Drollette, Brian D.; Gordon, Mark; Lee, Patrick; Liu, Peter; Leithead, Amy; Moussa, Samar G.; Wang, Danny; O’Brien, Jason; Mittermeier, Richard L.; Brook, Jeffrey R.; Lu, Gang; Staebler, Ralf M.; Han, Yuemei; Tokarek, Travis W.; Osthoff, Hans D.; Makar, Paul A.; Zhang, Junhua; L. Plata, Desiree; Gentner, Drew R.

    2016-06-01

    Worldwide heavy oil and bitumen deposits amount to 9 trillion barrels of oil distributed in over 280 basins around the world, with Canada home to oil sands deposits of 1.7 trillion barrels. The global development of this resource and the increase in oil production from oil sands has caused environmental concerns over the presence of toxic compounds in nearby ecosystems and acid deposition. The contribution of oil sands exploration to secondary organic aerosol formation, an important component of atmospheric particulate matter that affects air quality and climate, remains poorly understood. Here we use data from airborne measurements over the Canadian oil sands, laboratory experiments and a box-model study to provide a quantitative assessment of the magnitude of secondary organic aerosol production from oil sands emissions. We find that the evaporation and atmospheric oxidation of low-volatility organic vapours from the mined oil sands material is directly responsible for the majority of the observed secondary organic aerosol mass. The resultant production rates of 45–84 tonnes per day make the oil sands one of the largest sources of anthropogenic secondary organic aerosols in North America. Heavy oil and bitumen account for over ten per cent of global oil production today, and this figure continues to grow. Our findings suggest that the production of the more viscous crude oils could be a large source of secondary organic aerosols in many production and refining regions worldwide, and that such production should be considered when assessing the environmental impacts of current and planned bitumen and heavy oil extraction projects globally.

  7. Determination of primary and secondary sources of organic acids and carbonaceous aerosols using stable carbon isotopes

    NASA Astrophysics Data System (ADS)

    Fisseha, Rebeka; Saurer, Matthias; Jäggi, Maya; Siegwolf, Rolf T. W.; Dommen, Josef; Szidat, Sönke; Samburova, Vera; Baltensperger, Urs

    Stable carbon isotope ratio ( δ13C) data can provide important information regarding the sources and the processing of atmospheric organic carbon species. Formic, acetic and oxalic acid were collected from Zurich city in August-September 2002 and March 2003 in the gas and aerosol phase, and the corresponding δ13C analysis was performed using a wet oxidation method followed by isotope ratio mass spectrometry. In August, the δ13C values of gas phase formic acid showed a significant correlation with ozone (coefficient of determination ( r2) = 0.63) due to the kinetic isotope effect (KIE). This indicates the presence of secondary sources (i.e. production of organic acids in the atmosphere) in addition to direct emission. In March, both gaseous formic and acetic acid exhibited similar δ13C values and did not show any correlation with ozone, indicating a predominantly primary origin. Even though oxalic acid is mainly produced by secondary processes, the δ13C value of particulate oxalic acid was not depleted and did not show any correlation with ozone, which may be due to the enrichment of 13C during the gas - aerosol partitioning. The concentrations and δ13C values of the different aerosol fractions (water soluble organic carbon, water insoluble organic carbon, carbonate and black carbon) collected during the same period were also determined. Water soluble organic carbon (WSOC) contributed about 60% to the total carbon and was enriched in 13C compared to other fractions indicating a possible effect of gas - aerosol partitioning on δ13C of carbonaceous aerosols. The carbonate fraction in general was very low (3% of the total carbon).

  8. Oil sands operations as a large source of secondary organic aerosols.

    PubMed

    Liggio, John; Li, Shao-Meng; Hayden, Katherine; Taha, Youssef M; Stroud, Craig; Darlington, Andrea; Drollette, Brian D; Gordon, Mark; Lee, Patrick; Liu, Peter; Leithead, Amy; Moussa, Samar G; Wang, Danny; O'Brien, Jason; Mittermeier, Richard L; Brook, Jeffrey R; Lu, Gang; Staebler, Ralf M; Han, Yuemei; Tokarek, Travis W; Osthoff, Hans D; Makar, Paul A; Zhang, Junhua; Plata, Desiree L; Gentner, Drew R

    2016-06-01

    Worldwide heavy oil and bitumen deposits amount to 9 trillion barrels of oil distributed in over 280 basins around the world, with Canada home to oil sands deposits of 1.7 trillion barrels. The global development of this resource and the increase in oil production from oil sands has caused environmental concerns over the presence of toxic compounds in nearby ecosystems and acid deposition. The contribution of oil sands exploration to secondary organic aerosol formation, an important component of atmospheric particulate matter that affects air quality and climate, remains poorly understood. Here we use data from airborne measurements over the Canadian oil sands, laboratory experiments and a box-model study to provide a quantitative assessment of the magnitude of secondary organic aerosol production from oil sands emissions. We find that the evaporation and atmospheric oxidation of low-volatility organic vapours from the mined oil sands material is directly responsible for the majority of the observed secondary organic aerosol mass. The resultant production rates of 45-84 tonnes per day make the oil sands one of the largest sources of anthropogenic secondary organic aerosols in North America. Heavy oil and bitumen account for over ten per cent of global oil production today, and this figure continues to grow. Our findings suggest that the production of the more viscous crude oils could be a large source of secondary organic aerosols in many production and refining regions worldwide, and that such production should be considered when assessing the environmental impacts of current and planned bitumen and heavy oil extraction projects globally. PMID:27251281

  9. Assessment of the sources of suspended particulate matter aerosol using US EPA PMF 3.0.

    PubMed

    Khan, Md Firoz; Hirano, Koichiro; Masunaga, Shigeki

    2012-01-01

    The main purpose of this paper was to carry out a source apportionment of suspended particulate matter (SPM) samples using positive matrix factorization procedure. The central and local Government of Japan introduced strict emission regulations in 2002/10 and 2003/10, respectively, in curbing SPM pollution from major metropolitans. This paper also highlighted the impact of the measures taken by the central and local Government of Japan on the reduction of SPM and the contributions of sources. SPM samples were collected for 6 years starting from 1999 to 2005 at two sites, i.e., site A (urban) and site B (suburban) of Yokohama, Japan. Microwave digestion and inductively coupled plasma-mass spectroscopy (ICP-MS) were employed to measure Mg, Al, Ca, V, Cr, Mn, Ni, Cu, Zn, Ga, As, Se, Rb, Sr, Ag, Cd, Cs, Ba, Pb and Bi, while water soluble ions (Na(+), NH₄⁺, K(+), Ca(2+), Mg(2+), Cl(-), NO₃⁻ and SO₄²⁻ as well as carbonaceous mass (EC and OC) were analyzed using ion chromatograph and CHN analyzer, respectively. The sources identified at two sites were automobile, soil dust, marine aerosol, mixed sources, and secondarily formed aerosol. Also, source quantification was performed. Automobile and soil dust were striking contributors at site A. Automobile and soil dust of SPM aerosol might be produced from local origin at current study areas. Besides, Asian dust had an impact on high concentrations of SPM aerosol in some certain period of the year due to the outflows of East Asian emission. In contrast, secondary aerosol in the form of sulfate and ammonium as well as mixed sources (coal, long-transported Cs, and other unknown sources) were remarkable at site B. Stationary/industrial combustion has apparently more impact on the release of SPM components at site B than A. Automobile regulations in 2002 and 2003, respectively, resulted in reduction of SPM by 28% for site A and 16% for site B. There was also net reduction of automobile contribution at both sites due

  10. Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

    SciTech Connect

    Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

    2010-03-15

    Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

  11. Aerosol Composition, Chemistry, and Source Characterization during the 2008 VOCALS Experiment

    NASA Astrophysics Data System (ADS)

    Lee, Y.; Springston, S.; Jayne, J. T.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L. I.; Daum, P. H.

    2009-12-01

    Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined on board the US DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field experiment between October 16 and November 15, 2008. Chemical species determined included SO42-, NO3-, NH4+, and total organics (Org) using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only ~0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are believed to be externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on non-acidic sea-salt aerosols, responsible partly for the Cl- deficit. Dust particles appeared to play a minor role judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations in the study domain were substantial (~0.5 - ~3 μg/m3) with a strong gradient (highest near the shore decreasing with distance from land), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., ≤ 40 parts per trillion and <0.05 μg/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4

  12. Impact of biomass burning sources on seasonal aerosol air quality

    NASA Astrophysics Data System (ADS)

    Reisen, Fabienne; Meyer, C. P. (Mick); Keywood, Melita D.

    2013-03-01

    In the Huon Valley, Tasmania, current public perception is that smoke from regeneration burning is the principal cause of pollution events in autumn. These events lead to exceedences of national air quality standards and to significant health impacts on the rural population. To date there is little data on the significance of the impact. The aim of the study was to quantitatively assess the seasonal atmospheric particle loadings in the Huon Valley and determine the impact of smoke pollution. The study monitored fine (PM2.5) and coarse (PM10) particle concentrations and their chemical composition at two locations in the Huon Valley, Geeveston, an urban site and Grove, a rural site, between March 2009 and November 2010. The monitoring program clearly showed that biomass burning was a significant source of PM2.5 in the Huon Valley, leading to exceedences of the 24 h PM2.5 Ambient Air Quality National Environment Protection Measures advisory standard on a number of occasions. Significant increases of PM2.5 concentrations above background occurred during periods of prescribed burning as well as during the winter season. Although the intensity of emissions from prescribed burns (PB) and residential woodheaters (WH) was similar, emissions from WH were the largest source of PM2.5, with a contribution of 77% to the ambient PM2.5 load compared to an 11% contribution from PB. The results have also shown a greater impact on air quality at the urban site than at the rural site, indicating that PM2.5 concentrations are primarily influenced by localised sources rather than by regional pollution. The potential impact on local residents of the high PM concentrations during the PB and WH season was assessed. WH pollution is largely a persistent night-time issue in contrast to PB events which generally occur during the day and are of short duration. Due to the long persistence of high PM concentrations in winter, indoor PM concentrations are unlikely to be substantially lower than

  13. Quantifying the sources of atmospheric ice nuclei from carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Schill, G. P.; Jathar, S.; Galang, A.; Farmer, D.; Friedman, B.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.

    2015-12-01

    Ice nucleation on particles is a fundamental atmospheric process, which governs precipitation, cloud lifetimes, and climate. Despite being a basic atmospheric process, our current understanding of ice nucleation in the atmosphere is low. One reason for this low understanding is that ice nuclei concentrations are low (only ~1 in 105 particles in the free troposphere nucleate ice), making it challenging to identify both the composition and sources of ambient ice nuclei. Carbonaceous combustion aerosol produced from biomass and fossil fuel combustion are one potential source of these ice nuclei, as they contribute to over one-third of all aerosol in the North American free troposphere. Unfortunately, previous results from field measurements in-cloud, aircraft measurements, and laboratory studies are in conflict, with estimates of the impact of combustion aerosol ranging from no effect to rivaling the well-known atmospheric ice nuclei mineral dust. It is, however, becoming clear that aerosols from combustion processes are more complex than model particles, and their ice activity depends greatly on both fuel type and combustion conditions. Given these dependencies, we propose that sampling from real-world biomass burning and fossil fuel sources would provide the most useful new information on the contribution of carbonaceous combustion aerosols to atmospheric ice nuclei particles. To determine the specific contribution of refractory black carbon (rBC) to ice nuclei concentrations, we have coupled the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. In this work, we will present recent results looking at contribution of diesel

  14. The Role of Local and Remote Anthropogenic Aerosol Forcing on Long-term Variations in the South Asian Monsoon Annual Cycle

    NASA Astrophysics Data System (ADS)

    Bollasina, M. A.; Ming, Y.; Ramaswamy, V.

    2013-12-01

    Detection and attribution of long-term variations of the South Asian monsoon is of extreme importance: even small changes in the onset and duration of the monsoon season or in the spatial distribution of the seasonal mean precipitation may severely impact agriculture, health, water availability, ecosystems, and economy for a substantial fraction of the world's population. In the past decades emissions of aerosols have dramatically increased over South Asia due to rapid urbanization and population growth. As a result, the study of the impact of anthropogenic aerosols on the monsoon has recently emerged as one of the topics of highest priority in the scientific community. This study makes use of a state-of-the-art coupled climate model, the GFDL CM3, to investigate two aspects of the aerosol influence on the observed late 20th century changes in the monsoon annual cycle. The model has fully-interactive aerosols and a representation of both direct and indirect aerosol effects. Aerosols are responsible for an earlier shift of the monsoon onset over India, leading, in agreement with observations, to enhanced precipitation in June over most parts of the subcontinent. Our experiments show that the shift is preceded in early spring by strong aerosol forcing over the Bay of Bengal and Indochina, mostly attributable to the direct effect, resulting in increased atmospheric stability that inhibits the monsoon migration in May. The adjusted atmospheric circulation leads to thermodynamical changes over the northwestern continental region, including increased surface heating and near-surface moist static energy, which support a stronger June flow and, facilitated by a relative warming of the Indian Ocean, a vigorous northwestward precipitation shift. These findings underscore the importance of dynamical feedbacks and regional land-surface processes for the aerosol-monsoon link. We also performed historical experiments with time-evolving radiative forcings aimed at isolating the

  15. Integrated Analyses of Multiple Worldwide Aerosol Mass Spectrometer Datasets for Improved Understanding of Aerosol Sources and Processes and for Comparison with Global Models

    SciTech Connect

    Zhang, Qi; Jose, Jimenez Luis

    2014-04-28

    The AMS is the only current instrument that provides real-time, quantitative, and size-resolved data on submicron non-refractory aerosol species with a time resolution of a few minutes or better. The AMS field data are multidimensional and massive, containing extremely rich information on aerosol chemistry, microphysics and dynamics—basic information that is required to evaluate and quantify the radiative climate forcing of atmospheric aerosols. The high time resolution of the AMS data also reveals details of aerosol dynamic variations that are vital to understanding the physico-chemical processes of atmospheric aerosols that govern aerosol properties relevant to the climate. There are two primary objectives of this 3-year project. Our first objective is to perform highly integrated analysis of dozens of AMS datasets acquired from various urban, forested, coastal, marine, mountain peak, and rural/remote locations around the world and synthesize and inter-compare results with a focus on the sources and the physico-chemical processes that govern aerosol properties relevant to aerosol climate forcing. Our second objective is to support our collaboration with global aerosol modelers, in which we will supply the size-resolved aerosol composition and temporal variation data (via a public web interface) and our analysis results for use in model testing and validation and for translation of the rich AMS database into model constraints that can improve climate forcing simulations. Several prominent global aerosol modelers have expressed enthusiastic support for this collaboration. The specific tasks that we propose to accomplish include 1) to develop, validate, and apply multivariate analysis techniques for improved characterization and source apportionment of organic aerosols; 2) to evaluate aerosol source regions and relative contributions based on back-trajectory integration (PSCF method); 3) to summarize and synthesize submicron aerosol information, including

  16. Worldwide impact of aerosol's time scale on the predicted long-term concentrating solar power potential.

    PubMed

    Ruiz-Arias, Jose A; Gueymard, Christian A; Santos-Alamillos, Francisco J; Pozo-Vázquez, David

    2016-01-01

    Concentrating solar technologies, which are fuelled by the direct normal component of solar irradiance (DNI), are among the most promising solar technologies. Currently, the state-of the-art methods for DNI evaluation use datasets of aerosol optical depth (AOD) with only coarse (typically monthly) temporal resolution. Using daily AOD data from both site-specific observations at ground stations as well as gridded model estimates, a methodology is developed to evaluate how the calculated long-term DNI resource is affected by using AOD data averaged over periods from 1 to 30 days. It is demonstrated here that the use of monthly representations of AOD leads to systematic underestimations of the predicted long-term DNI up to 10% in some areas with high solar resource, which may result in detrimental consequences for the bankability of concentrating solar power projects. Recommendations for the use of either daily or monthly AOD data are provided on a geographical basis. PMID:27507711

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  18. Source term calculations for assessing radiation dose to equipment

    SciTech Connect

    Denning, R.S.; Freeman-Kelly, R.; Cybulskis, P.; Curtis, L.A.

    1989-07-01

    This study examines results of analyses performed with the Source Term Code Package to develop updated source terms using NUREG-0956 methods. The updated source terms are to be used to assess the adequacy of current regulatory source terms used as the basis for equipment qualification. Time-dependent locational distributions of radionuclides within a containment following a severe accident have been developed. The Surry reactor has been selected in this study as representative of PWR containment designs. Similarly, the Peach Bottom reactor has been used to examine radionuclide distributions in boiling water reactors. The time-dependent inventory of each key radionuclide is provided in terms of its activity in curies. The data are to be used by Sandia National Laboratories to perform shielding analyses to estimate radiation dose to equipment in each containment design. See NUREG/CR-5175, Beta and Gamma Dose Calculations for PWR and BWR Containments.'' 6 refs., 11 tabs.

  19. Biomass burning in the Amazon region: Aerosol source apportionment and associated health risk assessment

    NASA Astrophysics Data System (ADS)

    de Oliveira Alves, Nilmara; Brito, Joel; Caumo, Sofia; Arana, Andrea; de Souza Hacon, Sandra; Artaxo, Paulo; Hillamo, Risto; Teinilä, Kimmo; Batistuzzo de Medeiros, Silvia Regina; de Castro Vasconcellos, Pérola

    2015-11-01

    The Brazilian Amazon represents about 40% of the world's remaining tropical rainforest. However, human activities have become important drivers of disturbance in that region. The majority of forest fire hotspots in the Amazon arc due to deforestation are impacting the health of the local population of over 10 million inhabitants. In this study we characterize western Amazonia biomass burning emissions through the quantification of 14 Polycyclic Aromatic Hydrocarbons (PAHs), Organic Carbon, Elemental Carbon and unique tracers of biomass burning such as levoglucosan. From the PAHs dataset a toxic equivalence factor is calculated estimating the carcinogenic and mutagenic potential of biomass burning emissions during the studied period. Peak concentration of PM10 during the dry seasons was observed to reach 60 μg m-3 on the 24 h average. Conversely, PM10 was relatively constant throughout the wet season indicating an overall stable balance between aerosol sources and sinks within the filter sampling resolution. Similar behavior is identified for OC and EC components. Levoglucosan was found in significant concentrations (up to 4 μg m-3) during the dry season. Correspondingly, the estimated lung cancer risk calculated during the dry seasons largely exceeded the WHO health-based guideline. A source apportionment study was carried out through the use of Absolute Principal Factor Analysis (APFA), identifying a three-factor solution. The biomass burning factor is found to be the dominating aerosol source, having 75.4% of PM10 loading. The second factor depicts an important contribution of several PAHs without a single source class and therefore was considered as mixed sources factor, contributing to 6.3% of PM10. The third factor was mainly associated with fossil fuel combustion emissions, contributing to 18.4% of PM10. This work enhances the knowledge of aerosol sources and its impact on climate variability and local population, on a site representative of the

  20. Brown carbon aerosol in the North American continental troposphere: sources, abundance, and radiative forcing

    NASA Astrophysics Data System (ADS)

    Liu, J.; Scheuer, E.; Dibb, J.; Diskin, G. S.; Ziemba, L. D.; Thornhill, K. L.; Anderson, B. E.; Wisthaler, A.; Mikoviny, T.; Devi, J. J.; Bergin, M.; Perring, A. E.; Markovic, M. Z.; Schwarz, J. P.; Campuzano-Jost, P.; Day, D. A.; Jimenez, J. L.; Weber, R. J.

    2015-07-01

    Chemical components of organic aerosol (OA) selectively absorb light at short wavelengths. In this study, the prevalence, sources, and optical importance of this so-called brown carbon (BrC) aerosol component are investigated throughout the North American continental tropospheric column during a summer of extensive biomass burning. Spectrophotometric absorption measurements on extracts of bulk aerosol samples collected from an aircraft over the central USA were analyzed to directly quantify BrC abundance. BrC was found to be prevalent throughout the 1 to 12 km altitude measurement range, with dramatic enhancements in biomass-burning plumes. BrC to black carbon (BC) ratios, under background tropospheric conditions, increased with altitude, consistent with a corresponding increase in the absorption Ångström exponent (AAE) determined from a three-wavelength particle soot absorption photometer (PSAP). The sum of inferred BC absorption and measured BrC absorption at 365 nm was within 3 % of the measured PSAP absorption for background conditions and 22 % for biomass burning. A radiative transfer model showed that BrC absorption reduced top-of-atmosphere (TOA) aerosol forcing by ~ 20 % in the background troposphere. Extensive radiative model simulations applying this study background tropospheric conditions provided a look-up chart for determining radiative forcing efficiencies of BrC as a function of a surface-measured BrC : BC ratio and single scattering albedo (SSA). The chart is a first attempt to provide a tool for better assessment of brown carbon's forcing effect when one is limited to only surface data. These results indicate that BrC is an important contributor to direct aerosol radiative forcing.

  1. Scoping Analysis of Source Term and Functional Containment Attenuation Factors

    SciTech Connect

    Pete Lowry

    2012-01-01

    In order to meet future regulatory requirements, the Next Generation Nuclear Plant (NGNP) Project must fully establish and validate the mechanistic modular high temperature gas-cooled reactor (HTGR) source term. This is not possible at this stage in the project, as significant uncertainties in the final design remain unresolved. In the interim, however, there is a need to establish an approximate characterization of the source term. The NGNP team developed a simplified parametric model to establish mechanistic source term estimates for a set of proposed HTGR configurations.

  2. Scoping Analysis of Source Term and Functional Containment Attenuation Factors

    SciTech Connect

    Pete Lowry

    2012-10-01

    In order to meet future regulatory requirements, the Next Generation Nuclear Plant (NGNP) Project must fully establish and validate the mechanistic modular high temperature gas-cooled reactor (HTGR) source term. This is not possible at this stage in the project, as significant uncertainties in the final design remain unresolved. In the interim, however, there is a need to establish an approximate characterization of the source term. The NGNP team developed a simplified parametric model to establish mechanistic source term estimates for a set of proposed HTGR configurations.

  3. Scoping Analysis of Source Term and Functional Containment Attenuation Factors

    SciTech Connect

    Pete Lowry

    2012-02-01

    In order to meet future regulatory requirements, the Next Generation Nuclear Plant (NGNP) Project must fully establish and validate the mechanistic modular high temperature gas-cooled reactor (HTGR) source term. This is not possible at this stage in the project, as significant uncertainties in the final design remain unresolved. In the interim, however, there is a need to establish an approximate characterization of the source term. The NGNP team developed a simplified parametric model to establish mechanistic source term estimates for a set of proposed HTGR configurations.

  4. Primary to secondary organic aerosol: evolution of organic emissions from mobile combustion sources

    NASA Astrophysics Data System (ADS)

    Presto, A. A.; Gordon, T. D.; Robinson, A. L.

    2014-05-01

    A series of smog chamber experiments were conducted to investigate the transformation of primary organic aerosol (POA) and formation of secondary organic aerosol (SOA) during the photooxidation of dilute exhaust from a fleet of gasoline and diesel motor vehicles and two gas-turbine engines. In experiments where POA was present in the chamber at the onset of photooxidation, positive matrix factorization (PMF) was used to determine separate POA and SOA factors from aerosol mass spectrometer data. A 2-factor solution, with one POA factor and one SOA factor, was sufficient to describe the organic aerosol for gasoline vehicles, diesel vehicles, and one of the gas-turbine engines. Experiments with the second gas-turbine engine required a 3-factor PMF solution with a POA factor and two SOA factors. Results from the PMF analysis were compared to the residual method for determining SOA and POA mass concentrations. The residual method apportioned a larger fraction of the organic aerosol mass as POA because it assumes that all mass at m / z 57 is associated with POA. The POA mass spectrum for the gasoline and diesel vehicles exhibited high abundances of the CnH2n+1 series of ions (m / z 43, 57, etc.) and was similar to the mass spectra of the hydrocarbon-like organic aerosol factor determined from ambient data sets with one exception, a diesel vehicle equipped with a diesel oxidation catalyst. POA mass spectra for the gas-turbine engines are enriched in the CnH2n-1 series of ions (m / z 41, 55, etc.), consistent with the composition of the lubricating oil used in these engines. The SOA formed from the three sources exhibits high abundances of m / z 44 and 43, indicative of mild oxidation. The SOA mass spectra are consistent with less-oxidized ambient SV-OOA (semivolatile oxygenated organic aerosols) and fall within the triangular region of f44 versus f43 defined by ambient measurements. However there is poor absolute agreement between the experimentally derived SOA mass

  5. Discussion on linear long-term trends in aerosol and cloud properties over India and its surrounding waters

    NASA Astrophysics Data System (ADS)

    Sreekanth, V.

    2016-05-01

    Spatial and seasonal variations in the linear long-term trend estimates of aerosol and cloud properties over Indian subcontinent and the surrounding oceanic regions of Bay of Bengal (BoB) and Arabian Sea (AS) are studied and discussed utilizing 12 complete years (2003-2014) of Moderate Resolution Imaging Spectroradiometer (MODIS) derived Aerosol and cloud products. Annual Aerosol Optical Depth (AOD) trends (in terms of AOD/year) are found to be positive (upward) over most of the study region with a spatial mean (median) value of ∼0.0065 (0.0064) and exhibited significant spatial and seasonal heterogeneity. Over Indian landmass AOD trends and their statistical significance decreased towards north along the Indo-Gangetic plains (IGP), for which the probable causes are discussed. Same kind of pattern in AOD trends has been observed as we move deeper into the oceanic regions of BoB and AS, away from Indian subcontinent. Observed trend patterns are discussed in light of the possible increase in emissions (over Indian landmass) and transported aerosol component, co-variation with trends in meteorological parameters and their possible feedbacks. Trend maps in seasonal AOD are shown to understand the aerosol build up over the study region under varying meteorological conditions. Seasonal AOD trend patterns resembled the synoptic scale wind circulation over the study region revealing that the upward trend in aerosol abundance over the adjoining oceanic regions of India is a result of effective transport of increasing emissions over India on to them. No significant trends in cloud properties (over the whole study region) are depicted in concert with that of aerosols, except over few pockets. The study also highlighted the role of large scale atmospheric processes in modulating the shape of the AOD time series over the regions with significant abundance of natural aerosol component (dust).

  6. Composition and sources of carbonaceous aerosols at three contrasting sites in Hong Kong

    NASA Astrophysics Data System (ADS)

    Zheng, Mei; Hagler, Gayle S. W.; Ke, Lin; Bergin, Michael H.; Wang, Fu; Louie, Peter K. K.; Salmon, Lynn; Sin, Della W. M.; Yu, Jian Zhen; Schauer, James J.

    2006-10-01

    A significant fraction of the fine particulate matter in Hong Kong is made up of organic carbon. In order to quantitatively assess the contributions of various sources to carbonaceous aerosol in Hong Kong, a chemical mass balance (CMB) receptor model in combination with organic tracers was employed. Organic tracers including n-alkanes, polycyclic aromatic hydrocarbons (PAHs), steranes, hopanes, resin acids, cholesterol, levoglucosan, and picene in PM2.5 collected from three air monitoring sites located at roadside, urban, and rural areas in Hong Kong are quantified using gas chromatography-mass spectrometry (GC/MS) in the present study. Analyses of some overlapping species from two separate laboratories will be compared for the first time. Spatial and seasonal source contributions to organic carbon (OC) in PM2.5 from up to nine air pollution sources are assessed, including diesel engine exhaust, gasoline engine exhaust, meat cooking, cigarette smoke, biomass burning, road dust, vegetative detritus, coal combustion, and natural gas combustion. Diesel engine exhaust dominated fine organic carbon in Hong Kong (57 ± 13% at urban sites and 25 ± 2% at the rural site). Other sources that play an important role are meat cooking and biomass burning, which can account for as much as 14% of fine organic carbon. The primary sources identified by this technique explained 49%, 79%, and 94% of the measured fine organic carbon mass concentration at the rural, the urban, and the roadside sites, respectively. The unexplained fine OC is likely due to secondary organic aerosol formation.

  7. Sources of PM10 and sulfate aerosol at McMurdo Station, Antarctica.

    PubMed

    Mazzera, D M; Lowenthal, D H; Chow, J C; Watson, J G

    2001-10-01

    Source contributions to PM10 and sulfate aerosol at McMurdo Station, Antarctica during the austral summers of 1995-1996 and 1996-1997 were estimated using Chemical Mass Balance (CMB) receptor modeling. The average PM10 (particles with aerodynamic diameters less than 10 microm) concentration at Hut Point, located less than 1 km downwind of downtown McMurdo, was 3.4 microg/m3. Emissions profiles were determined for potentially important aerosol source types in McMurdo: exposed soil, power generation, space heating, and surface vehicles. Soil dust, sea salt, combustion emissions, sulfates, marine biogenic emissions as methanesulfonate, and nitrates contributed 57%, 15%, 14%, 10%, 3%, and 1%, respectively, of average estimated PM10 at Hut Point (3.2 microg/m3). Soil dust, sea salt, and combustion sources contributed 12%, 8%, and 20%, respectively, of the average PM10 sulfate concentration of 0.46 microg/m3. Marine biogenic sources contributed 0.17 microg/m3 (37%). The remaining sulfate is thought to have come from emissions from Mt. Erebus or hemispheric pollution sources. PMID:11592425

  8. Sources of light-absorbing aerosol in arctic snow and their seasonal variation

    NASA Astrophysics Data System (ADS)

    Hegg, Dean A.; Warren, Stephen G.; Grenfell, Thomas C.; Doherty, Sarah J.; Clarke, Antony D.

    2010-11-01

    Two data sets consisting of measurements of light absorbing aerosols (LAA) in arctic snow together with suites of other corresponding chemical constituents are presented; the first from Siberia, Greenland and near the North Pole obtained in 2008, and the second from the Canadian arctic obtained in 2009. A preliminary differentiation of the LAA into black carbon (BC) and non-BC LAA is done. Source attribution of the light absorbing aerosols was done using a positive matrix factorization (PMF) model. Four sources were found for each data set (crop and grass burning, boreal biomass burning, pollution and marine). For both data sets, the crops and grass biomass burning was the main source of both LAA species, suggesting the non-BC LAA was brown carbon. Depth profiles at most of the sites allowed assessment of the seasonal variation in the source strengths. The biomass burning sources dominated in the spring but pollution played a more significant (though rarely dominant) role in the fall, winter and, for Greenland, summer. The PMF analysis is consistent with trajectory analysis and satellite fire maps.

  9. Sources and chemical characterization of organic aerosol during the summer in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Kostenidou, E.; Florou, K.; Kaltsonoudis, C.; Tsiflikiotou, M.; Vratolis, S.; Eleftheriadis, K.; Pandis, S. N.

    2015-10-01

    The concentration and chemical composition of non-refractory fine particulate matter (NR-PM1) and black carbon (BC) levels were measured during the summer of 2012 in the suburbs of two Greek cities, Patras and Athens, in an effort to better understand the chemical processing of particles in the high photochemical activity environment of the eastern Mediterranean. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources for the corresponding pollution levels. The PM1 average mass concentration was 9-14 μg m-3. The contribution of sulfate was around 38 %, while organic aerosol (OA) contributed approximately 45 % in both cases. PM1 nitrate levels were low (2 %). The oxygen to carbon (O : C) atomic ratio was 0.50 ± 0.08 in Patras and 0.47 ± 0.11 in Athens. In both cases PM1 was acidic. Positive matrix factorization (PMF) was applied to the high-resolution organic aerosol mass spectra obtained by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). For Patras, five OA sources could be identified: 19 % very oxygenated OA (V-OOA), 38 % moderately oxygenated OA (M-OOA), 21 % biogenic oxygenated OA (b-OOA), 7 % hydrocarbon-like OA (HOA-1) associated with traffic sources and 15 % hydrocarbon-like OA (HOA-2) related to other primary emissions (including cooking OA). For Athens, the corresponding source contributions were: V-OOA (35 %), M-OOA (30 %), HOA-1 (18 %) and HOA-2 (17 %). In both cities the major component was OOA, suggesting that under high photochemical conditions most of the OA in the eastern Mediterranean is quite aged. The contribution of the primary sources (HOA-1 and HOA-2) was important (22 % in Patras and 35 % in Athens) but not dominant.

  10. Sources and chemical characterization of organic aerosol during the summer in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Kostenidou, E.; Florou, K.; Kaltsonoudis, C.; Tsiflikiotou, M.; Vratolis, S.; Eleftheriadis, K.; Pandis, S. N.

    2015-02-01

    The concentration and chemical composition of the non-refractory fine particulate matter (NR-PM1) and black carbon (BC) levels were measured during the summer of 2012 in the suburbs of two Greek cities, Patras and Athens, in an effort to better understand the chemical processing of particles in the high photochemical activity environment of the Eastern Mediterranean. The composition of PM1 was surprisingly similar in both areas demonstrating the importance of regional sources for the corresponding pollution levels. The PM1 average mass concentration was 9-14 μg m-3. The contribution of sulphate was around 38%, while organic aerosol (OA) contributed approximately 45% in both cases. PM1 nitrate levels were low (2%). The oxygen to carbon (O : C) atomic ratio was 0.50 ± 0.08 in Patras and 0.47 ± 0.11 in Athens. In both cases the PM1 was acidic. Positive matrix factorization (PMF) was applied to the high resolution organic aerosol mass spectra obtained by an Aerodyne High Resolution Aerosol Mass Spectrometer (HR-AMS). For Patras five OA sources could be identified: 19% very oxygenated OA (V-OOA), 38% moderately oxygenated OA (M-OOA), 21% biogenic oxygenated OA (b-OOA), 7% hydrocarbon-like OA (HOA-1) associated with traffic sources and 15% hydrocarbon-like OA (HOA-2) related to other primary emissions (including cooking OA). For Athens the corresponding source contributions were: V-OOA (35%), M-OOA (30%), HOA-1 (18%) and HOA-2 (17%). In both cities the major component was OOA, suggesting that under high photochemical conditions most of the OA in the Eastern Mediterranean is quite aged. The contribution of the primary sources (HOA-1 and HOA-2) was important (22% in Patras and 33% in Athens) but not dominant.

  11. 13C measurements on organic aerosol - ambient samples versus source studies

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike; Meusinger, Carl; Oyama, Beatriz; Ramon, Wichert; de Wilde, Peter A.; Holzinger, Rupert; Röckmann, Thomas

    2013-04-01

    The stable carbon isotopes 12C and 13C can be used to get information about sources and processing of organic aerosol (OA). We developed and tested a method to measure δ13C values of OA collected on filter samples in different volatility classes. These filter samples are introduced into an oven, where organic compounds are thermally desorbed in He at different temperatures. The compounds released at each temperature step are oxidized to CO2 using a platinum catalyst at 550 °C. The CO2 is then passed on to an isotope ratio mass spectrometer (IRMS) to measure δ13C ratios. With a similar setup the chemical composition at each temperature step can be determined using a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). System evaluation with controlled test compounds showed that organic compounds usually start evaporating from the filter when their melting point is reached. Isotopic fractionation occurs only, if one temperature step is within a few degrees of the melting point of the substance, so that the substance only partially evaporates. However, this effect should be limited in an ambient sample containing thousands of individual chemical compounds. We analysed aerosol samples collected in a tunnel in Brazil (vehicular emissions), laboratory generated secondary organic aerosol (SOA) from alpha-pinene ozonolysis, and ambient filter samples from a regional site in the Netherlands and an urban site in Belgium. First results indicate that SOA is more volatile than organic aerosol from ambient or tunnel filters. The δ13C ratios of SOA and vehicular emissions do not change strongly with oven temperature, i.e. the more refractory organic compounds have similar isotopic composition as the more volatile compounds. This is in contrast to ambient organic aerosol where the more volatile compounds evaporating below 200°C are depleted with respect to the refractory compounds. Possible reasons for this difference (mixture of sources vs the role of

  12. Carbonaceous aerosol over semi-arid region of western India: Heterogeneity in sources and characteristics

    NASA Astrophysics Data System (ADS)

    Sudheer, A. K.; Aslam, M. Y.; Upadhyay, M.; Rengarajan, R.; Bhushan, R.; Rathore, J. S.; Singh, S. K.; Kumar, S.

    2016-09-01

    Carbonaceous species (elemental carbon (EC), organic carbon (OC), water-soluble organic carbon (WSOC)) and water-soluble inorganic species (Na+, NH4+, K+, Ca2 +, Mg2 +, Cl-, NO3-, SO42 -) in PM10 and PM2.5 from Ahmedabad and Jodhpur (urban and semi-urban locations, respectively) in western India were measured during May-September, 2011. Stable isotope composition of carbonaceous aerosol (δ13C of TC) in PM10 samples was also determined. Average EC concentration in PM10 at Ahmedabad was 1 μg m- 3 (range: 0.34 to 3.4 μg m- 3), almost 80% of which remained in PM2.5. Similarly, 70% of EC in PM10 (average: 0.9 μg m- 3) resided in PM2.5 at Jodhpur. Average OC concentration at Ahmedabad was 6.4 μg m- 3 and ~ 52% of this was found in PM2.5. On the contrary, OC concentration at Jodhpur was 40 μg m- 3, 80% of which was found in coarse particles contributing substantially to aerosol mass. δ13C of TC (average: - 27.5‰, range: - 29.6 to - 25.8‰) along with WSOC/EC ratio shows an increasing trend at Jodhpur suggesting the possibility of aging of aerosol, since aging results in enrichment of heavier isotope. OC and WSOC show significant correlations with K+ and not with EC, indicating biogenic origin of OC. Different size distributions are also exhibited by WSOC at the two stations. On the other hand, δ13C exhibits an inverse trend with sea-salt constituents at Ahmedabad, indicating the influence of air masses transported from the western/south-western region on carbonaceous aerosol. These results suggest that a strong heterogeneity exists in the sources of carbonaceous aerosol over this region and potential sources of non-combustion emissions such as bio-aerosol that need further investigation.

  13. Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

    SciTech Connect

    Thornton, Joel

    2015-01-26

    The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

  14. Characterization of polar organic compounds and source analysis of fine organic aerosols in Hong Kong

    NASA Astrophysics Data System (ADS)

    Li, Yunchun

    Organic aerosols, as an important fraction of airborne particulate mass, significantly affect the environment, climate, and human health. Compared with inorganic species, characterization of individual organic compounds is much less complete and comprehensive because they number in thousands or more and are diverse in chemical structures. The source contributions of organic aerosols are far from being well understood because they can be emitted from a variety of sources as well as formed from photochemical reactions of numerous precursors. This thesis work aims to improve the characterization of polar organic compounds and source apportionment analysis of fine organic carbon (OC) in Hong Kong, which consists of two parts: (1) An improved analytical method to determine monocarboxylic acids, dicarboxylic acids, ketocarboxylic acids, and dicarbonyls collected on filter substrates has been established. These oxygenated compounds were determined as their butyl ester or butyl acetal derivatives using gas chromatography-mass spectrometry. The new method made improvements over the original Kawamura method by eliminating the water extraction and evaporation steps. Aerosol materials were directly mixed with the BF 3/BuOH derivatization agent and the extracting solvent hexane. This modification improves recoveries for both the more volatile and the less water-soluble compounds. This improved method was applied to study the abundances and sources of these oxygenated compounds in PM2.5 aerosol samples collected in Hong Kong under different synoptic conditions during 2003-2005. These compounds account for on average 5.2% of OC (range: 1.4%-13.6%) on a carbon basis. Oxalic acid was the most abundant species. Six C2 and C3 oxygenated compounds, namely oxalic, malonic, glyoxylic, pyruvic acids, glyoxal, and methylglyoxal, dominated this suite of oxygenated compounds. More efforts are therefore suggested to focus on these small compounds in understanding the role of oxygenated

  15. Coupling Aerosol-Cloud-Radiative Processes in the WRF-Chem Model: Investigating the Radiative Impact of Elevated Point Sources

    SciTech Connect

    Chapman, Elaine G.; Gustafson, William I.; Easter, Richard C.; Barnard, James C.; Ghan, Steven J.; Pekour, Mikhail S.; Fast, Jerome D.

    2009-02-01

    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 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 slightly overpredicted SO2 mixing ratios and PM2.5 mass, but reproduced the range of observed SO2 to sulfate aerosol ratios, suggesting that atmospheric oxidation processes leading to aerosol sulfate formation are captured in the model. The baseline simulation was compared to a sensitivity simulation in which all emissions at model levels above the surface layer were set to zero, thus removing stack emissions. Instantaneous, site-specific differences for aerosol and cloud related properties between the two simulations could be quite large, as removing above-surface emission sources influenced when and where clouds formed within the modeling domain. When summed spatially over the finest resolution model domain (the extent of which corresponds to

  16. Source Term Model for an Array of Vortex Generator Vanes

    NASA Technical Reports Server (NTRS)

    Buning, P. G. (Technical Monitor); Waithe, Kenrick A.

    2003-01-01

    A source term model was developed for numerical simulations of an array of vortex generators. The source term models the side force created by a vortex generator being modeled. The model is obtained by introducing a side force to the momentum and energy equations that can adjust its strength automatically based on a local flow. The model was tested and calibrated by comparing data from numerical simulations and experiments of a single low-profile vortex generator vane, which is only a fraction of the boundary layer thickness, over a flat plate. The source term model allowed a grid reduction of about seventy percent when compared with the numerical simulations performed on a fully gridded vortex generator without adversely affecting the development and capture of the vortex created. The source term model was able to predict the shape and size of the stream wise vorticity and velocity contours very well when compared with both numerical simulations and experimental data.

  17. Carbonaceous aerosol characteristics over Delhi in Northern India: Seasonal variability and possible sources

    NASA Astrophysics Data System (ADS)

    Srivastava, Atul Kumar; Bisht, Ds; Tiwari, S.

    Carbonaceous aerosols have been the focus of extensive studies during the last decade due to its significant impacts on human health, visibility and climate change. As per Asian regions are concerned, aerosols in south-Asia are gaining considerable importance because of their potential impacts on regional climate, yet their possible sources are poorly understood. Semi-continuous measurements of organic carbon (OC) and elemental carbon (EC) and continuous measurements of black carbon (BC) aerosols were conducted simultaneously at Delhi during the period from January 2011 to May 2012. Delhi is the capital city of India and one of the densely populated and industrialized urban megacities in Asia, located at the Ganga basin in the northern part of India. Being highly polluted region, mass concentrations of OC, EC and BC over Delhi were found to vary from about 6-92 mug m (-3) (mean: 23±16 mug m (-3) ), 3-38 mug m (-3) (mean: 11±7 mug m (-3) ) and 1-24 mug m (-3) (mean: 7±5 mug m (-3) ), respectively during the entire measurement period, with about two times higher concentration during winter as compared to summer. A significant correlation between OC and EC (R=0.95, n=232) and relatively lower OC/EC ratio (range: 1.0-3.6; mean: 2.2±0.5) suggest fossil fuel emission as a dominant source of carbonaceous aerosols over the station. The average mass concentration of EC was found about 38% higher than BC during the study period, which is interestingly different as reported at other locations over Ganga basin. We also determined the associated optical properties of carbonaceous species (e.g. absorption coefficient and mass absorption efficiency) over the station. Significant loading of carbonaceous species over such regions emphasize an urgent need to focus on air quality management and proper impact assessment on health perspective.

  18. Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

    SciTech Connect

    Lee, Y. -N.; Springston, S.; Jayne, J.; Wang, J.; Hubbe, J.; Senum, G.; Kleinman, L.; Daum, P. H.

    2014-01-01

    The chemical composition of aerosol particles (Dp ≤ 1.5 μm) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42−, followed by Na+, Cl, Org (total organics), NH4+, and NO3, in decreasing order of importance; CH3SO3 (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH4+ to SO42− equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO42−. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72° W and 76° W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol

  19. Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq

    NASA Astrophysics Data System (ADS)

    Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.

    2015-04-01

    Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.

  20. Submicron organic aerosol in Tijuana, Mexico, from local and Southern California sources during the CalMex campaign

    NASA Astrophysics Data System (ADS)

    Takahama, S.; Johnson, A.; Guzman Morales, J.; Russell, L. M.; Duran, R.; Rodriguez, G.; Zheng, J.; Zhang, R.; Toom-Sauntry, D.; Leaitch, W. R.

    2013-05-01

    The CalMex campaign was conducted from May 15 to June 30 of 2010 to study the properties and sources of air pollution in Tijuana, Mexico. In this study, submicron organic aerosol mass (OM) composition measured by Fourier Transform Infrared Spectroscopy (FTIR), Aerosol Chemical Speciation Monitor (ACSM), and X-ray spectromicroscopy are combined with statistical analysis and measurements of other atmospheric constituents. The average (±one standard deviation) OM concentration was 3.3 ± 1.7 μg m-3. A large source of submicron aerosol mass at this location was determined to be vehicular sources, which contributed approximately 40% to the submicron OM; largely during weekday mornings. The O/C ratio estimated from ACSM measurements was 0.64 ± 0.19; diurnal variations in this value and the more oxygenated fraction of OM as determined from Positive Matrix Factorization and classification analyses suggest the high degree of oxygenation originates from aged OM, rather than locally-produced secondary organic aerosol. A large contribution of this oxygenated aerosol to Tijuana from various source classes was observed; some fraction of this aerosol mass may be associated with non-refractory components, such as dust or BC. Backtrajectory simulations using the HYSPLIT model suggest that the mean wind vector consistently originated from the northwest region, over the Pacific Ocean and near the Southern California coast, which suggests that the origin of much of the oxygenated organic aerosol observed in Tijuana (as much as 60% of OM) may have been the Southern California Air Basin. The marine aerosol contribution to OM during the period was on average 23 ± 24%, though its contribution varied over synoptic rather than diurnal timescales. BB aerosol contributed 20 ± 20% of the OM during the campaign period, with notable BB events occurring during several weekend evenings.

  1. Revised accident source terms for light-water reactors

    SciTech Connect

    Soffer, L.

    1995-02-01

    This paper presents revised accident source terms for light-water reactors incorporating the severe accident research insights gained in this area over the last 15 years. Current LWR reactor accident source terms used for licensing date from 1962 and are contained in Regulatory Guides 1.3 and 1.4. These specify that 100% of the core inventory of noble gases and 25% of the iodine fission products are assumed to be instantaneously available for release from the containment. The chemical form of the iodine fission products is also assumed to be predominantly elemental iodine. These assumptions have strongly affected present nuclear air cleaning requirements by emphasizing rapid actuation of spray systems and filtration systems optimized to retain elemental iodine. A proposed revision of reactor accident source terms and some im implications for nuclear air cleaning requirements was presented at the 22nd DOE/NRC Nuclear Air Cleaning Conference. A draft report was issued by the NRC for comment in July 1992. Extensive comments were received, with the most significant comments involving (a) release fractions for both volatile and non-volatile species in the early in-vessel release phase, (b) gap release fractions of the noble gases, iodine and cesium, and (c) the timing and duration for the release phases. The final source term report is expected to be issued in late 1994. Although the revised source terms are intended primarily for future plants, current nuclear power plants may request use of revised accident source term insights as well in licensing. This paper emphasizes additional information obtained since the 22nd Conference, including studies on fission product removal mechanisms, results obtained from improved severe accident code calculations and resolution of major comments, and their impact upon the revised accident source terms. Revised accident source terms for both BWRS and PWRS are presented.

  2. 13C measurements on organic aerosol - a comparison of sources with ambient samples

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike; Meusinger, Carl; Oyama, Beatriz; Holzinger, Rupert; Röckmann, Thomas

    2014-05-01

    The stable carbon isotopes 12C and 13C can be used to get information about sources and processing of organic aerosol (OA). We developed and tested a method to measure δ13C values of OA collected on filter samples in different volatility classes. These filter samples are introduced into an oven, where organic compounds are thermally desorbed in He at different temperatures. The compounds released at each temperature step are oxidized to CO2 using a platinum catalyst at 550 °C. The CO2 is then passed on to an isotope ratio mass spectrometer (IRMS) to measure d13C ratios. With a similar setup the chemical composition at each temperature step can be determined using a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). System evaluation with controlled test compounds showed that organic compounds usually start evaporating from the filter when their melting point is reached. Isotopic fractionation occurs only if one temperature step is within a few degrees of the melting point of the substance, so that the substance only partially evaporates. However, this effect should be limited in an ambient sample containing thousands of individual chemical compounds. δ13C values of aerosol filter samples do not depend on the sample amount used, i.e. the system shows good linearity. The reproducibility depends somewhat on the sample amount and is usually < ± 0.3 ‰ for oven temperatures up to 200 °C and < ± 0.5 ‰ for oven temperatures greater than 200 °C. We analysed aerosol samples collected in a tunnel in Brazil (vehicular emissions), laboratory generated secondary organic aerosol (SOA) from alpha-pinene ozonolysis, and ambient filter samples from a regional site in the Netherlands, an urban site in Belgium, and Sao Paulo Brazil. First results show that δ13C ratios of SOA and vehicular emissions do not change strongly with oven temperature, i.e. the more refractory organic compounds have similar isotopic composition as the more volatile compounds

  3. New insights on aerosol sources and properties of Organics in the west Mediterranean basin

    NASA Astrophysics Data System (ADS)

    Nicolas, José B.; Sciare, Jean; Petit, Jean-Eudes; Bonnaire, Nicolas; Féron, Anais; Dulac, François; Hamonou, Eric; Gros, Valérie; Mallet, Marc; Lambert, Dominique; Sauvage, Stéphane; Léonardis, Thierry; Tison, Emmanuel; Colomb, Aurélie; Fresney, Evelyn; Pichon, Jean-Marc; Bouvier, Laetitia; Bourrianne, Thierry; Roberts, Gregory

    2013-04-01

    The Mediterranean basin exhibits high PM concentrations for a marine area, in particular during the dry season (summer), associated with high photochemistry. The large population of the basin is impacted by both natural and anthropogenic aerosols of various sources from Europe and North Africa. Simulations predict significant climate changes in that area, with less precipitation and hotter temperatures, reinforced by an increasing anthropogenic pressure, which will be linked by higher emissions of pollutants and also by higher impacts on the health. Nevertheless the aerosol models in that area currently suffer from large uncertainties, due to a lack of knowledge in organic aerosol (OA) sources and processes. As part of the French program ChArMEx (The Chemistry-Aerosol Mediterranean Experiment, http://charmex.lsce.ipsl.fr), a 5-week intensive campaign has been performed in June - July 2012 at the new Cape Corsica station (see Dulac et al. in that session), and aiming at a better characterization of anthropogenic versus biogenic aerosols, long range transport versus local influence, with a focus on fine OA. A complete instrumental strategy was deployed thanks to the contribution of a large French community: PM1 concentration every 6 min with a TEOM-FDMS 1405 (Thermo), major aerosol components in PM1 every 30 min (Organics, SO4, NO3, NH4) by Aerosol Chemical Speciation Monitor (Aerodyne), Equivalent Black Carbon every 5 min with a 7-? aethalometer AE31 (Magee Scientific), on-line major anions and cations (incl. light organics like oxalate & MSA) every 10 min with Particle-Into-Liquid Sampler (PILS, Metrohm) coupled with Ion Chromatographs (Dionex), on-line water-soluble organic carbon (WSOC) every 4 min with a PILS (Applikon) coupled with a Total Organic Carbon instrument (Ionics). Filter sampling in PM2.5 and PM10 was also performed every 12h for quality purposes (PM, EC/OC, ions) and for complementary measurements (metals by ICP-MS and organic tracers by LC

  4. Global Long-Term SeaWiFS Deep Blue Aerosol Products available at NASA GES DISC

    NASA Astrophysics Data System (ADS)

    Shen, S.; Sayer, A. M.; Bettenhausen, C.; Wei, J. C.; Ostrenga, D.; Vollmer, B.; Hsu, N. C.

    2012-12-01

    Long-term climate data records of aerosols are needed in order to study regional air quality and the uncertainty of aerosol radiative forcing with numerical models. Recently, global long-term (over 13 years from 1997 to 2010) SeaWiFS Deep Blue (SWDB) aerosol products have become available. The SWDB aerosol dataset has been produced by the "Consistent Long-Term Aerosol Data Records over Land and Ocean from SeaWIFS" project led by Dr. N. Christina Hsu as part of the Making Earth Science data records for Use in Research for Earth Science (MEaSUREs) program. The latest Deep Blue algorithm retrieves aerosol properties not only over bright desert surfaces, but also vegetated surfaces, oceans, and inland water bodies. Comparisons with AERONET observations have shown that the data are suitable for quantitative scientific use. The resolution of the Level 2 pixels is 13.5x13.5 km2 at the center of the swath. The Level 3 daily and monthly data are composed by using best quality level 2 pixels at resolution of both 0.5x0.5 and 1.0x1.0 degrees. This presentation, focusing over the south Asia region, will show sample higher resolution Level 2 images of dust events and the Level 3 monthly climatology at large scale. The data are compared with the widely-used MODIS (Deep Blue and Dark Target) aerosol dataset. The SWDB aerosol data are available from NASA Goddard Earth Sciences Data and Information Services Center (GES DISC) through a number of data services, such as FTP; the data search system, Mirador; OPeNDAP; and online subsetting services. The global daily and monthly Level 3 products are also available in the innovative online visualization and analysis system, Giovanni. More information about SWBD aerosol products can be found from the project portal: http://disc.gsfc.nasa.gov/dust. Seasonal climatology of SeaWiFS Deep Blue Aerosol Optical Depth at 550nm for the period from 1997.09 to 2010.12.

  5. Water soluble ions in aerosols (TSP) : Characteristics, sources and seasonal variation over the central Himalayas, Nepal

    NASA Astrophysics Data System (ADS)

    Tripathee, Lekhendra; Kang, Shichang; Zhang, Qianggong; Rupakheti, Dipesh

    2016-04-01

    Atmspheric pollutants transported from South Asia could have adverse impact on the Himalayan ecosystems. Investigation of aerosol chemistry in the Himalayan region in Nepal has been limited on a temporal and spatial scale to date. Therefore, the water-soluble ionic composition of aerosol using TSP sampler was investigated for a year period from April 2013 to March 2014 at four sites Bode, Dhunche, Lumbini and Jomsom characterized as an urban, rural, semi-urban and remote sites in Nepal. During the study period, the highest concentration of major cation was Ca2+ with an average concentration of 8.91, 2.17, 7.85 and 6.42 μg m-3 and the highest concentration of major anion was SO42- with an average of 10.96, 4.06, 6.85 and 3.30 μg m-3 at Bode, Dhunche, Lumbini and Jomsom respectively. The soluble ions showed the decrease in concentrations from urban to the rural site. Correlations and PCA analysis suggested that that SO42-, NO3- and NH4+ were derived from the anthropogenic sources where as the Ca2+ and Mg2+ were from crustal sources. Our results also suggest that the largest acid neutralizing agent at our sampling sites in the central Himalayas are Ca2+ followed by NH4+. Seasonal variations of soluble ions in aerosols showed higher concentrations during pre-monsoon and winter (dry-periods) due to limited precipitation amount and lower concentrations during the monsoon which can be explained by the dilution effect, higher the precipitation lower the concentration. K+ which is regarded as the tracer of biomss burning had a significant peaks during pre-monsoon season when the forest fires are active around the regions. In general, the results of this study suggests that the atmospheric chemistry is influenced by natural and anthropogenic sources. Thus, soluble ionic concentrations in aerosols from central Himalayas, Nepal can provide a useful database to assess atmospheric environment and its impacts on human health and ecosystem in the southern side of central

  6. Comparative application of multiple receptor methods to identify aerosol sources in northern Vermont.

    PubMed

    Poirot, R L; Wishinski, P R; Hopke, P K; Polissar, A V

    2001-12-01

    This study applies and compares results of four receptor modeling techniques to a common set of speciated fine particle measurement data collected ata remote site in northwestern Vermont between 1988 and 1995. Two multivariate mathematical models, positive matrix factorization and UNMIX, were applied to the measurement data and identified seven "common" sources that had similar compositions and similar fine mass contributions in both models. Two ensemble backward trajectory techniques, potential source contribution function and residence-time analysis, were also applied to evaluate and interpret the mathematical model results. The trajectory techniques indicate a strong regional character to the upwind locations associated with aerosol contributions from most of the sources identified independently by the mathematical models and help in the interpretation of those results. The process of model comparison provides insights on the strengths and limitations of the individual and combined source attribution techniques. Convergent results among the multiple methods provide a degree of confidence that each of the receptor methods may represent useful tools for future air quality management. Divergent or inconsistent results among the models can help identify limitations of the individual models and of the underlying aerosol and meteorological data sets. PMID:11770763

  7. Source apportionment of carbonaceous aerosol in Sao Paulo using 13C and 14C measurements

    NASA Astrophysics Data System (ADS)

    Oyama, Beatriz; Andrade, Maria de Fatima; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro A. J.; Dusek, Ulrike

    2016-04-01

    The Metropolitan Area of Sao Paulo is affected by high aerosol concentrations, which contain a large fraction of organic material. Up to date, not much is known about the composition and origin of the organic aerosol in this city. We present the first source apportionment of the carbonaceous aerosol fraction in Sao Paulo, using stable (13C) and radioactive carbon isotopes (14C). 14C provides a clear-cut distinction between fossil sources, which contain no 14C, and contemporary sources such as biofuels, biomass burning, or biogenic sources, which contain a typical contemporary 14C/12C ratio. 13C can be used to distinguish C3 plants, such as maize and sugarcane, from C4 plants. This can help to identify a possible impact of sugarcane field burning in the rural areas of Sao Paulo State on the aerosol carbon in the city. In the first part of the study, we compare two tunnel studies: Tunnel 1 is frequented only by light duty vehicles, which run mainly on mixtures of gasoline with ethanol (gasohol, 25% ethanol and 85% gasoline) or hydrated ethanol (5% water and 95% ethanol). Tunnel 2 contains a significant fraction of heavy-duty diesel vehicles, and therefore the fraction of biofuels in the average fleet is lower. Comparison of 14C in organic and elemental carbon (OC and EC) shows that in both tunnels there is no significant contribution of biofuels to EC. Combusting ethanol-gasoline fuels in a vehicle engine does apparently not result in significant EC formation from ethanol. Biofuels contribute around 45% to OC in Tunnel 1 an only 20% in Tunnel 2, reflecting a strong impact of diesel vehicles in Tunnel 2. In the second part of the study we conduct a source apportionment of ambient aerosol carbon collected in a field study during winter (July-August) 2012. Ambient EC has two main sources, vehicular emissions and biomass burning. We estimate a contribution of vehicular sources to EC of roughly 90% during weekdays and 80% during weekends, using the 14C values measured in

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

    NASA Astrophysics Data System (ADS)

    Guo, S.; Hu, M.; Guo, Q.; Zhang, X.; Schauer, J. J.; Zhang, R.

    2013-08-01

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

  9. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2014-10-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Mt. Everest (Qomolangma Station for Atmospheric and Environmental Observation and Research, briefly QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The samples were analyzed for organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and major ions. The average concentrations of OC, EC and WSOC were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high elevation sites on the southern slopes of the Himalayas (Langtang and NCO-P), but three to six times lower than those at Manora Peak, India and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The various aerosol compositions showed distinctive seasonality. The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. While OC, EC and other ionic species (NH4+, K+, NO3-, and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season. Similar seasonal trends of aerosol composition were also reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. This phenomenon indicates that both slopes of Himalayas share a common atmospheric environment regime. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they were mainly originated from biomass burning. The active fire spots observed by MODIS and their backward trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in the northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. In addition to large-scale atmospheric circulation, the unique

  10. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2015-02-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research (QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The average concentrations of organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and Nepal Climate Observatory at Pyramid, or NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH4+, K+, NO3- and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol composition reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they mainly originated from biomass burning. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. Moreover, the CALIOP observations confirmed that air-pollution plumes crossed the Himalayas during this period. The highly coherent variation of daily aerosol optical depth (500 nm) between QOMS and NCO-P indicates that both slopes of the Himalayas share a common atmospheric environment

  11. Long-term Statistics of Continental Cumuli: Does Aerosol Trigger Cumulus Variability?

    SciTech Connect

    Kassianov, Evgueni I.; Berg, Larry K.; McFarlane, Sally A.; Flynn, Connor J.; Turner, David D.

    2009-02-01

    Atmospheric aerosols may control the formation, maintenance, and dissipation of cumuli by changing their microphysics. Recent observational and modeling results exist both in support and against strong potential impacts of aerosol [1-3]. Typically, the aerosol impact on water clouds has been investigated for regions with high aerosol loading and/or large atmospheric moisture [4]. Can we provide observational evidence of the aerosol-cloud relationship for a relatively dry continental region with low/moderate aerosol burden? To address this question, we revisit the aerosol-cloud relationship at the Atmospheric Radiation Measurement (ARM) Climate Research Facility (ACRF) Southern Great Plains (SGP) site. In comparison with highly polluted regions, the SGP site is characterized by relatively small-to-moderate aerosol loading. Also, moisture content is small-to-moderate (compared to marine and coastal regions) for the SGP site. Because cumulus clouds have important impacts on climate forcing estimations [5] and are susceptible to aerosol effects [6], we focus on fair-weather cumuli (FWC) and their association with aerosol concentration and other potentially important factors. This association is investigated using a new 8-year aerosol and cloud climatology (2000-2007) developed with collocated and coincident surface and satellite observations.

  12. The AIRPARIF-AEROSOL project: A comprehensive source apportionment study of fine aerosols (PM2.5) in the region of Paris (France)

    NASA Astrophysics Data System (ADS)

    Sciare, Jean; Ghersi, Veronique; Bressi, Michael; Lameloise, Philippe; Bonnaire, Nicolas; Rosso, Amandine; Nicolas, Jose; Moukhtar, Sophie; Ferron, Anais; Baumier, Dominique

    2010-05-01

    With a population of about 12 millions inhabitants (20% of the French population), Greater Paris (France) is one of the most populated megacity in Europe and among the few located in developed countries. Due to its favorable geographical situation (far from other big European cities and influenced very often by clean oceanic air masses), it may be considered as a good candidate for investigating the build-up of urban air pollution from temperate industrialized countries. Particulate mass of fine aerosols with aerodynamic diameter below 2.5μm (PM2.5) is continuously monitored at several stations from great Paris for almost 8 years by the local air quality network (AIRPARIF), using a conventional on-line automatic system (R&P TEOM; see Patashnik and Rupprecht, 1991). During the period 2000-2006, levels of PM2.5 in the region of Paris have shown rather stable yearly mean values ranging 13 to 16?g/m3 whereas most of the other pollutants monitored by AIRPARIF have shown a net decrease during this period (http:\\www.airparif.asso.fr). Since the year 2007, this situation has becoming worse for particulate pollution with a net increase of the yearly mean concentration of PM2.5 (up to 21?g/m3), which increase is partly due to the use of a new PM2.5 measurement technique (R&P TEOM-FDMS instrument) enabling a proper determination of the semi-volatile fraction of fine aerosols. Although this new method greatly improves the determination of PM2.5, it has also brought PM2.5 levels in the region of Paris closer to the 25?g/m3 yearly mean targeted value recommended by Europe for 2010 (limit value for 2015). Efficient abatement policies aiming at reducing levels of PM2.5 in the region of Paris will have to be fed by preliminary PM2.5 source apportionment studies and exhaustive aerosol chemistry studies (chemical mass balance) allowing a better separation between regional to continental aerosol sources. The objective of the AIRPARIF-AEROSOL project aims to perform a spatially- and

  13. Source categories and contribution of biomass smoke to organic aerosol over the southeastern Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Sang, Xuefang; Zhang, Zhisheng; Chan, Chuenyu; Engling, Guenter

    2013-10-01

    An intensive measurement campaign was conducted at a mountain and suburban site at the edge of the southeastern Tibetan Plateau during spring. Concentrations of PM2.5, carbonaceous species (OC and EC) and anhydrosugars (levoglucosan, mannosan and galactosan) as well as their ratios were utilized to identify possible biomass burning categories and contributions of biomass burning smoke to ambient aerosols. The average concentrations of levoglucosan and mannosan were 193.8 and 12.4 ng m-3, respectively at the mountain site, and 713 and 61.5 ng m-3 respectively at the suburban site. According to characteristic levoglucosan/mannosan (Lev/Man) and mannosan/galactosan (Man/Gal) ratios, we identified for the first time that mixed smoke particles (18.5, 72.3 and 9.1% for crop residues, softwood and hard wood respectively) derived from the study region and Southeast Asia contributed to the aerosol burden in the southeastern Tibetan Plateau. The biomass smoke contributions to organic carbon and organic matter were estimated to be 28.4% and 18.9-25.7% respectively at the mountain site and 38.3% and 33.5-45.4% respectively at the suburban site. The large contribution estimates indicate that biomass burning was an important anthropogenic/natural source of aerosol particles which impact regional atmospheric chemistry and climate in the southeastern Tibetan Plateau.

  14. Sensitivity Study of The Sulfate Aerosol Indirect Radiative Forcing To The Dms Source Representation

    NASA Astrophysics Data System (ADS)

    Boucher, O.; Aumont, O.; Belviso, S.; Cosme, E.; Moulin, C.; Pham, M.

    We use a global sulfur cycle model (LMD-ZT) to study the sensitivity of the dimethyl- sulfide (DMS) atmospheric concentrations and sulfur cycle to the representation of the DMS oceanic source. We test four different distributions of the oceanic DMS concen- trations: the Kettle et al. DMS dataset, two datasets built from Seawifs measurements of the ocean color (but with different , and one distribution from a coupled oceanic bi- ological model. There is a convergence for 3 out of 4 DMS datasets to produce a global DMS flux of 18-20 TgS/yr. There are however significant disagreements on the spa- tial and seasonal distribution of the DMS flux. A comparison of the DMS atmospheric concentrations with observations will be presented. The sulfate aerosol indirect radia- tive forcing depends strongly on the concentration of pre-industrial aerosols, which itself depends on the DMS sea-air flux. The subsequent uncertainty on the aerosol in- direct radiative forcing and the implication for climate-chemistry interactions will be discussed.

  15. Trends and sources of particulate matter in the Superstition Wilderness using air trajectory and aerosol cluster analysis

    NASA Astrophysics Data System (ADS)

    Coury, Charity; Dillner, Ann M.

    Ambient aerosols adversely affect human health and visibility and impact climate. Identification of sources of particulate matter and its precursors is necessary for developing control strategies. The goal of this research is to utilize long-term speciated particulate matter data and back-trajectory cluster analyses to determine trends and sources of particulate matter in the Superstition Wilderness, a rural area east of Phoenix, Arizona. Twenty-four hour back-trajectories were calculated for every hour of every 24-h particulate matter sample obtained by IMPROVE from 1991 to 2004. Days that included back-trajectories with considerable spatial variance were excluded from further analyses. To minimize uncertainties inherent in single trajectories, all calculated trajectories for each sampling day were averaged to represent the air mass sampled during that day. Cluster analysis of trajectories identified four unique regions, including a region with Phoenix, a region with copper smelters, and one with coal-fired power plants. Yearly averages of sulfate, nitrate, soil, and carbon concentrations were calculated for each region. Statistically significant trends in species concentrations by region and independent of region and differences in concentrations between regions were examined. Sulfate concentrations from the region with smelters were higher than other regions but decreased during the study period. Emissions data from the smelters indicate that much of the sulfate from the region was due to the smelters. The overall 2.2% year -1 decrease in sulfate concentrations at TNM is likely due to decreased emissions from the copper smelters. A 3.6% year -1 increase in nitrate concentrations was driven largely by increasing NO x concentrations from Phoenix and to a lesser extent the region southwest of the site which includes Tucson and suburban/urban areas between Phoenix and Tucson. Soil concentrations were higher from regions with deserts than the region without desert

  16. Assessment of source apportionment by Positive Matrix Factorization analysis on fine and coarse urban aerosol size fractions

    NASA Astrophysics Data System (ADS)

    Karanasiou, A. A.; Siskos, P. A.; Eleftheriadis, K.

    This study was conducted in order to investigate the differences observed in source profiles in the urban environment, when chemical composition parameters from different aerosol size fractions are subjected to factor analysis. Source apportionment was performed in an urban area where representative types of emission sources are present. PM 10 and PM 2 samples were collected within the Athens Metropolitan area and analysed for trace elements, inorganic ions and black carbon. Analysis by two-way and three-way Positive Matrix Factorization was performed, in order to resolve sources from data obtained for the fine and coarse aerosol fractions. A difference was observed: seven factors describe the best solution in PMF3 while six factors in PMF2. Six factors derived from PMF3 analysis correspond to those described by the PMF2 solution for the fine and coarse particles separately. These sources were attributed to road dust, marine aerosol, soil, motor vehicles, biomass burning, and oil combustion. The additional source resolved by PMF3 was attributed to a different type of road dust. Combustion sources (oil combustion and biomass burning) were correctly attributed by PMF3 solely to the fine fraction and the soil source to the coarse fraction. However, a motor vehicle's contribution to the coarse fraction was found only by three-way PMF. When PMF2 was employed in PM 10 concentrations the optimum solution included six factors. Four source profiles corresponded to the previously identified as vehicles, road dust, biomass burning and marine aerosol, while two could not be clearly identified. Source apportionment by PMF2 analysis based solely on PM 10 aerosol composition data, yielded unclear results, compared to results from PMF2 and PMF3 analyses on fine and coarse aerosol composition data.

  17. Sources of excess urban carbonaceous aerosol in the Pearl River Delta Region, China

    NASA Astrophysics Data System (ADS)

    Zheng, Mei; Wang, Fu; Hagler, G. S. W.; Hou, Ximei; Bergin, Michael; Cheng, Yuan; Salmon, L. G.; Schauer, James J.; Louie, Peter K. K.; Zeng, Limin; Zhang, Yuanhang

    2011-02-01

    Carbonaceous aerosol is one of the important constituents of fine particulate matter (PM 2.5) in southern China, including the Pearl River Delta (PRD) region and Hong Kong (HK). During the study period (October and December of 2002, and March and June of 2003), the monthly average organic carbon (OC) ranged from 3.52 to 7.87 μg m -3 in Hong Kong and 4.14-20.19 μg m -3 in the PRD from simultaneous measurements at three sites in HK and four sites in the PRD. Compared to the PRD, the spatial distribution of carbonaceous aerosol in Hong Kong was relatively homogeneous. Sources contributing to excess OC in the PRD were examined, which is the difference between OC concentrations measured at the PRD sites to the average level in Hong Kong. Eight primary sources contributing to excess OC were identified with chemical mass balance modeling in a combination with molecular markers analyzed by gas chromatography/mass spectrometry. Excess OC at Guangzhou, the capital city of Guangdong province, was consistently high, ranging from 9.77 to 13.6 μg m -3. Four primary sources including gasoline engine exhaust, diesel engine exhaust, biomass burning, and coal combustion accounted for more than 50% of excess OC in the PRD, especially in December (up to 76%). Mobile source emissions alone can contribute about 30% of excess OC. The unexplained or other excess OC was the highest at the rural site, but in general less than 20% at other sites. The coal combustion source contribution was unique in that it exhibited relatively homogeneous spatial distribution, indicating it was still an important source of carbonaceous aerosol in the PRD (17% of excess OC) during the study period. This analysis revealed that primary emissions are important sources of excess OC in the PRD and there is a need to reduce the emissions of mobile sources, biomass burning, and coal combustion in order to improve air quality in southern China.

  18. Demonstration of a VUV lamp photoionization source for improvedorganic speciation in an aerosol mass spectrometer

    SciTech Connect

    Northway, M.J.; Jayne, J.T.; Toohey, D.W.; Canagaratna, M.R.; Trimborn, A.; Akiyama, K-I.; Shimono, A.; Jimenez, J.L.; DeCarlo, P.F.; Wilson, K.R.; Worsnop, D.R.

    2007-10-03

    In recent years, the Aerodyne AerosolMass Spectrometer(AMS) has become a widely used tool for determining aerosol sizedistributions and chemical composition for non-refractory inorganic andorganic aerosol. The current version of the AMS uses a combination offlash thermal vaporization and 70 eV electron impact (EI) ionization.However, EI causes extensive fragmentation and mass spectra of organicaerosols are difficult to deconvolute because they are composites of theoverlapping fragmentation patterns of all species present. Previous AMSstudies have been limited to classifying organics in broad categoriessuch as oxidized and hydrocarbon-like." In this manuscript we present newefforts to gain more information about organic aerosol composition byemploying the softer technique of vacuum ultraviolet (VUV) ionization ina Time-of-Flight AMS (ToF-AMS). In our novel design a VUV lamp is placedin direct proximity of the ionization region of the AMS, with only awindow separating the lamp and the ionizer. This design allows foralternation of photoionization and electron impact ionization within thesame instrument on the timescale of minutes. Thus, the EI-basedquantification capability of the AMS is retained while improved spectralinterpretation is made possible by combined analysis of the complementaryVUV and EI ionization spectra. Photoionization and electron impactionization spectra are compared for a number of compounds including oleicacid, long chain hydrocarbons, and cigarette smoke. In general, the VUVspectra contain much less fragmentation than the EI spectra and for manycompounds the parent ion is the dominant ion in the VUV spectrum. As anexample of the usefulness of the integration of PI within the fullcapability of the ToF-AMS, size distributions and size-segregated massspectra are examined for the cigarette smoke analysis. As a finalevaluation of the new VUV module, spectra for oleic acid are compared tosimilar experiments conducted using the tunable VUV radiation

  19. Developing a stronger understanding of aerosol sources and the impact of aqueous phase processing on coastal air quality

    NASA Astrophysics Data System (ADS)

    Prather, K. A.

    2014-12-01

    Atmospheric aerosols are produced by a variety of sources including emissions from cars and trucks, wildfires, ships, dust, and sea spray and play a significant role in impacting air pollution and regional climate. The ability of an aerosol to uptake water and undergo aqueous phase processing strongly depends on composition. On-line single particle mass spectrometry can provide insight into how particle composition impacts the degree of photochemical and aging processes atmospheric aerosols undergo. In particular, specific sulfur species including sulfate, hydroxymethanesulfate (HMS), and methanesulfonic acid (MSA) can serve as indicators of when an air mass has undergone aqueous phase processing. This presentation will describe recent field studies conducted at coastal sites to demonstrate how different aerosol sources and secondary processing impact coastal air quality.

  20. Spatial and Temporal Variations of EC and OC Aerosol Combustion Sources in a Polluted Metropolitan Area

    NASA Astrophysics Data System (ADS)

    Mouteva, G.; Randerson, J. T.; Fahrni, S.; Santos, G.; Bush, S. E.; Ehleringer, J. R.; Czimczik, C. I.

    2015-12-01

    Anthropogenic emissions of carbonaceous aerosols are a major component of fine air particulate matter (PM2.5) in polluted metropolitan areas and in the global atmosphere. Elemental (EC) and organic carbon (OC) aerosols influence Earth's energy balance by means of direct and indirect pathways and EC has been suggested as a better indicator of public health impacts from combustion-related sources than PM mass. Quantifying the contribution of fossil fuel and biomass combustion to the EC and OC emissions and their temporal and spatial variations is critical for developing efficient legislative air pollution control measures and successful climate mitigation strategies. In this study, we used radiocarbon (14C) to separate and quantify fossil and biomass contributions to a time series of EC and OC collected at 3 locations in Salt Lake City (SLC). Aerosol samples were collected on quartz fiber filters and a modified OC/EC analyzer was used with the Swiss_4S protocol to isolate and trap the EC fraction. Together with the total carbon (TC) content of the samples, the EC was analyzed for its 14C content with accelerator mass spectrometry. The 14C of OC was derived as a mass balance difference between TC and EC. EC had an annual average fraction modern of 0.13±0.06 and did not vary significantly across seasons. OC had an annual average FM of 0.49±0.13, with the winter mean (0.43±0.11) lower than the summer mean (0.64±0.13) at the 5% significance level. While the 3 stations were chosen to represent a variety of environmental conditions within SLC, no major differences in this source partitioning were observed between stations. During winter, the major sources of air pollutants in SLC are motor vehicles and wood stove combustion and determining their relative contributions has been the subject of debate. Our results indicated that fossil fuels were the dominant source of carbonaceous aerosols during winter, contributing 87% or more of the total EC mass and 40-75% of the OC

  1. Maillard Chemistry in Clouds and Aqueous Aerosol As a Source of Atmospheric Humic-Like Substances.

    PubMed

    Hawkins, Lelia N; Lemire, Amanda N; Galloway, Melissa M; Corrigan, Ashley L; Turley, Jacob J; Espelien, Brenna M; De Haan, David O

    2016-07-19

    The reported optical, physical, and chemical properties of aqueous Maillard reaction mixtures of small aldehydes (glyoxal, methylglyoxal, and glycolaldehyde) with ammonium sulfate and amines are compared with those of aqueous extracts of ambient aerosol (water-soluble organic carbon, WSOC) and the humic-like substances (HULIS) fraction of WSOC. Using a combination of new and previously published measurements, we examine fluorescence, X-ray absorbance, UV/vis, and IR spectra, complex refractive indices, (1)H and (13)C NMR spectra, thermograms, aerosol and electrospray ionization mass spectra, surface activity, and hygroscopicity. Atmospheric WSOC and HULIS encompass a range of properties, but in almost every case aqueous aldehyde-amine reaction mixtures are squarely within this range. Notable exceptions are the higher UV/visible absorbance wavelength dependence (Angström coefficients) observed for methylglyoxal reaction mixtures, the lack of surface activity of glyoxal reaction mixtures, and the higher N/C ratios of aldehyde-amine reaction products relative to atmospheric WSOC and HULIS extracts. The overall optical, physical, and chemical similarities are consistent with, but not demonstrative of, Maillard chemistry being a significant secondary source of atmospheric HULIS. However, the higher N/C ratios of aldehyde-amine reaction products limits the source strength to ≤50% of atmospheric HULIS, assuming that other sources of HULIS incorporate only negligible quantities of nitrogen. PMID:27227348

  2. Identification of the sources of primary organic aerosols at urban schools: a molecular marker approach.

    PubMed

    Crilley, Leigh R; Qadir, Raeed M; Ayoko, Godwin A; Schnelle-Kreis, Jürgen; Abbaszade, Gülcin; Orasche, Jürgen; Zimmermann, Ralf; Morawska, Lidia

    2014-08-01

    Children are particularly susceptible to air pollution and schools are examples of urban microenvironments that can account for a large portion of children's exposure to airborne particles. Thus this paper aimed to determine the sources of primary airborne particles that children are exposed to at school by analyzing selected organic molecular markers at 11 urban schools in Brisbane, Australia. Positive matrix factorization analysis identified four sources at the schools: vehicle emissions, biomass burning, meat cooking and plant wax emissions accounting for 45%, 29%, 16% and 7%, of the organic carbon respectively. Biomass burning peaked in winter due to prescribed burning of bushland around Brisbane. Overall, the results indicated that both local (traffic) and regional (biomass burning) sources of primary organic aerosols influence the levels of ambient particles that children are exposed at the schools. These results have implications for potential control strategies for mitigating exposure at schools. PMID:24842381

  3. THE TAPERED ELEMENT OSCILLATING MICROBALANCE: A MONITOR FOR SHORT-TERM MEASUREMENT OF FINE AEROSOL MASS CONCENTRATION

    EPA Science Inventory

    A new instrument for short-term monitoring of ambient aerosol fine mass concentration has been developed based on a unique device called a Tapered Element Oscillating Microbalance (TEOM). The detector consists of a tapered hollow tube fixed at the wide end and holding an exchange...

  4. EFFECTS OF SHORT-TERM EXPOSURES TO SULFURIC ACID AND AMMONIUM SULFATE AEROSOLS UPON BRONCHIAL AIRWAY FUNCTION IN THE DONKEY

    EPA Science Inventory

    The effects of one-hour inhalation exposures to 0.3-0.6 micrometers H2SO4 and (NH4)2 aerosols in the donkey were studied in terms of alterations in pulmonary flow resistance and dynamic compliance, and changes in the regional deposition and tracheobronchial mucociliary clearance ...

  5. Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach

    NASA Astrophysics Data System (ADS)

    Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Ceburnis, D.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J. L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Laaksonen, A.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

    2014-06-01

    Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

  6. The long term Lampedusa data set of aerosol optical properties based on AERONET and MFRSR measurements

    NASA Astrophysics Data System (ADS)

    di Sarra, Alcide; Meloni, Daniela; Sferlazzo, Damiano; Pugnaghi, Sergio; Anello, Fabrizio; Bommarito, Carlo; Di Iorio, Tatiana; Monteleone, Francesco; Pace, Giandomenico; Piacentino, Salvatore

    2014-05-01

    which correspond with elevated AODs. A correction of the MFRSR measurements, derived from the comparison of simultaneous observations, was applied. The combined mesurements also allow to identify periods with instrumental problems, incorrect cloud screening, and problematic calibrations. Secondly, a combined intercalibrated dataset is constructed after careful verification of the avaliable data. The dataset is based on corrected MFRSR measurements, which guarantee high resolution observations and a better cloud screening, and AERONET data in the period when MFRSR measurements are not available. The evolution of the AOD at Lampedusa during the 2001-2013 period is discussed, in relation with long-term evolution, interannual variability, and seasonal changes. The data series display a very limited long-term change over the investigation period, and a relatively large interannual variability, with minima of the AOD occurring during years 2004, 2006, and 2009. The minimum in 2009, with an annual average of 0.14 against an overall annual average of 0.185, stands as a singularity in the record. The combined Lampedusa dataset will be used for aerosol climatological studies, and for verification of satellite observations and model analyses.

  7. Selection of models to calculate the LLW source term

    SciTech Connect

    Sullivan, T.M. )

    1991-10-01

    Performance assessment of a LLW disposal facility begins with an estimation of the rate at which radionuclides migrate out of the facility (i.e., the source term). The focus of this work is to develop a methodology for calculating the source term. In general, the source term is influenced by the radionuclide inventory, the wasteforms and containers used to dispose of the inventory, and the physical processes that lead to release from the facility (fluid flow, container degradation, wasteform leaching, and radionuclide transport). In turn, many of these physical processes are influenced by the design of the disposal facility (e.g., infiltration of water). The complexity of the problem and the absence of appropriate data prevent development of an entirely mechanistic representation of radionuclide release from a disposal facility. Typically, a number of assumptions, based on knowledge of the disposal system, are used to simplify the problem. This document provides a brief overview of disposal practices and reviews existing source term models as background for selecting appropriate models for estimating the source term. The selection rationale and the mathematical details of the models are presented. Finally, guidance is presented for combining the inventory data with appropriate mechanisms describing release from the disposal facility. 44 refs., 6 figs., 1 tab.

  8. Global Aerosols

    Atmospheric Science Data Center

    2013-04-19

    ... sizes and from multiple sources, including biomass burning, mineral dust, sea salt and regional industrial pollution. A color scale is ... desert source region. Deserts are the main sources of mineral dust, and MISR obtains aerosol optical depth at visible wavelengths ...

  9. Source apportionment of size and time resolved trace elements and organic aerosols from an urban courtyard site in Switzerland

    NASA Astrophysics Data System (ADS)

    Richard, A.; Gianini, M. F. D.; Mohr, C.; Furger, M.; Bukowiecki, N.; Minguillón, M. C.; Lienemann, P.; Flechsig, U.; Appel, K.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Baltensperger, U.; Prévôt, A. S. H.

    2011-02-01

    Time and size resolved data of trace elements were obtained from measurements with a rotating drum impactor (RDI) and subsequent X-ray fluorescence spectrometry. Trace elements can act as indicators for the identification of sources of particulate matter <10 μm (PM10) in ambient air. Receptor modeling was performed with positive matrix factorization (PMF) for trace element data from an urban background site in Zürich, Switzerland. Eight different sources were identified for the three examined size ranges (PM1-0.1, PM2.5-1 and PM10-2.5): secondary sulfate, wood combustion, fire works, road traffic, mineral dust, de-icing salt, industrial and local anthropogenic activities. The major component was secondary sulfate for the smallest size range; the road traffic factor was found in all three size ranges. This trace element analysis is complemented with data from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS), assessing the PM1 fraction of organic aerosols. A separate PMF analysis revealed three factors related to three of the sources found with the RDI: oxygenated organic aerosol (OOA, related to inorganic secondary sulfate), hydrocarbon like organic aerosol (HOA, related to road traffic) and biomass burning organic aerosol (BBOA), explaining 60%, 22% and 17% of total measured organics, respectively. Since different compounds are used for the source classification, a higher percentage of the ambient PM10 mass concentration can be apportioned to sources by the combination of both methods.

  10. Source apportionment of size and time resolved trace elements and organic aerosols from an urban courtyard site in Switzerland

    NASA Astrophysics Data System (ADS)

    Richard, A.; Gianini, M. F. D.; Mohr, C.; Furger, M.; Bukowiecki, N.; Minguillón, M. C.; Lienemann, P.; Flechsig, U.; Appel, K.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Baltensperger, U.; Prévôt, A. S. H.

    2011-09-01

    Time and size resolved data of trace elements were obtained from measurements with a rotating drum impactor (RDI) and subsequent X-ray fluorescence spectrometry. Trace elements can act as indicators for the identification of sources of particulate matter <10 μm (PM10) in ambient air. Receptor modeling was performed with positive matrix factorization (PMF) for trace element data from an urban background site in Zürich, Switzerland. Eight different sources were identified for the three examined size ranges (PM1-0.1, PM2.5-1 and PM10-2.5): secondary sulfate, wood combustion, fire works, road traffic, mineral dust, de-icing salt, industrial and local anthropogenic activities. The major component was secondary sulfate for the smallest size range; the road traffic factor was found in all three size ranges. This trace element analysis is complemented with data from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS), assessing the PM1 fraction of organic aerosols. A separate PMF analysis revealed three factors related to three of the sources found with the RDI: oxygenated organic aerosol (OOA, related to inorganic secondary sulfate), hydrocarbon-like organic aerosol (HOA, related to road traffic) and biomass burning organic aerosol (BBOA), explaining 60 %, 22 % and 17 % of total measured organics, respectively. Since different compounds are used for the source classification, a higher percentage of the ambient PM10 mass concentration can be apportioned to sources by the combination of both methods.

  11. Plant and Soil Emissions of Amines and Amino Acids: A Source of Secondary Aerosol Precursors

    NASA Astrophysics Data System (ADS)

    Jackson, M. L.; Doskey, P. V.; Pypker, T. G.

    2011-12-01

    Ammonia (NH3) is the most abundant alkaline gas in the atmosphere and forms secondary aerosol by neutralizing sulfuric and nitric acids that are released during combustion of fossil fuels. Ammonia is primarily emitted by cropping and livestock operations. However, C2 and C3 amines (pKb 3.3-3.4), which are stronger bases than NH3 (pKb 4.7) have been observed in nuclei mode aerosol that is the precursor to secondary aerosol. Mixtures of amines and amino acids have been identified in diverse environments in aerosol, fog water, cloud water, the soluble fraction of precipitation, and in dew. Glycine (pKb 4.2), serine (pKb 4.8) and alanine (pKb 3.7 and 4.1 for the D and L forms, respectively) are typically the most abundant species. The only reported values of gas-phase glycine, serine and alanine were in marine air and ranged from 6-14 pptv. The origin of atmospheric amines and amino acids has not been fully identified, although sources are likely similar to NH3. Nitrate assimilation in plants forms glycine, serine, and L-alanine, while D-alanine is present in bacterial cell walls. Glycine is converted to serine during C3 plant photorespiration, producing CO2 and NH3. Bacteria metabolize glycine and alanine to methylamine and ethylamine via decarboxylation. Likely sources of amino acids are plants and bacteria, thus concentrations near continental sources are likely greater than those measured in marine air. The overall goal of the research is to examine seasonal variations and relationships between the exchange of CO2, NH3, amines, and amino acids with a corn/soybean rotation in the Midwest Corn Belt. The study presents gaseous profiles of organic amine compounds from various species of vegetation using a mist chamber trapping technique and analysis of the derivatized species by high pressure liquid chromatography with fluorescence detection. Amino acid and amine profiles were obtained for red oak (Quercus rubra), sugar maple (Acer saccharinum), white pine (Pinus

  12. Turbulent aerosol fluxes over the Arctic Ocean: 2. Wind-driven sources from the sea

    NASA Astrophysics Data System (ADS)

    Nilsson, E. D.; Rannik, Ü.; Swietlicki, E.; Leck, C.; Aalto, P. P.; Zhou, J.; Norman, M.

    2001-12-01

    An eddy-covariance flux system was successfully applied over open sea, leads and ice floes during the Arctic Ocean Expedition in July-August 1996. Wind-driven upward aerosol number fluxes were observed over open sea and leads in the pack ice. These particles must originate from droplets ejected into the air at the bursting of small air bubbles at the water surface. The source flux F (in 106 m-2 s-1) had a strong dependency on wind speed, log>(F>)=0.20U¯-1.71 and 0.11U¯-1.93, over the open sea and leads, respectively (where U¯ is the local wind speed at about 10 m height). Over the open sea the wind-driven aerosol source flux consisted of a film drop mode centered at ˜100 nm diameter and a jet drop mode centered at ˜1 μm diameter. Over the leads in the pack ice, a jet drop mode at ˜2 μm diameter dominated. The jet drop mode consisted of sea-salt, but oxalate indicated an organic contribution, and bacterias and other biogenic particles were identified by single particle analysis. Particles with diameters less than -100 nm appear to have contributed to the flux, but their chemical composition is unknown. Whitecaps were probably the bubble source at open sea and on the leads at high wind speed, but a different bubble source is needed in the leads owing to their small fetch. Melting of ice in the leads is probably the best candidate. The flux over the open sea was of such a magnitude that it could give a significant contribution to the condensation nuclei (CCN) population. Although the flux from the leads were roughly an order of magnitude smaller and the leads cover only a small fraction of the pack ice, the local source may till be important for the CCN population in Arctic fogs. The primary marine aerosol source will increase both with increased wind speed and with decreased ice fraction and extent. The local CCN production may therefore increase and influence cloud or fog albedo and lifetime in response to greenhouse warming in the Arctic Ocean region.

  13. Local source impacts on primary and secondary aerosols in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Jayarathne, Thilina; Rathnayake, Chathurika M.; Stone, Elizabeth A.

    2016-04-01

    Atmospheric particulate matter (PM) exhibits heterogeneity in composition across urban areas, leading to poor representation of outdoor air pollutants in human exposure assessments. To examine heterogeneity in PM composition and sources across an urban area, fine particulate matter samples (PM2.5) were chemically profiled in Iowa City, IA from 25 August to 10 November 2011 at two monitoring stations. The urban site is the federal reference monitoring (FRM) station in the city center and the peri-urban site is located 8.0 km to the west on the city edge. Measurements of PM2.5 carbonaceous aerosol, inorganic ions, molecular markers for primary sources, and secondary organic aerosol (SOA) tracers were used to assess statistical differences in composition and sources across the two sites. PM2.5 mass ranged from 3 to 26 μg m-3 during this period, averaging 11.2 ± 4.9 μg m-3 (n = 71). Major components of PM2.5 at the urban site included organic carbon (OC; 22%), ammonium (14%), sulfate (13%), nitrate (7%), calcium (2.9%), and elemental carbon (EC; 2.2%). Periods of elevated PM were driven by increases in ammonium, sulfate, and SOA tracers that coincided with hot and dry conditions and southerly winds. Chemical mass balance (CMB) modeling was used to apportion OC to primary sources; biomass burning, vegetative detritus, diesel engines, and gasoline engines accounted for 28% of OC at the urban site and 24% of OC at the peri-urban site. Secondary organic carbon from isoprene and monoterpene SOA accounted for an additional 13% and 6% of OC at the urban and peri-urban sites, respectively. Differences in biogenic SOA across the two sites were associated with enhanced combustion activities in the urban area and higher aerosol acidity at the urban site. Major PM constituents (e.g., OC, ammonium, sulfate) were generally well-represented by a single monitoring station, indicating a regional source influence. Meanwhile, nitrate, biomass burning, food cooking, suspended dust, and

  14. Observationally-constrained carbonaceous aerosol source estimates for the Pearl River Delta area of China

    NASA Astrophysics Data System (ADS)

    Li, N.; Fu, T.-M.; Cao, J. J.; Zheng, J. Y.; He, Q. Y.; Long, X.; Zhao, Z. Z.; Cao, N. Y.; Fu, J. S.; Lam, Y. F.

    2015-11-01

    We simulated elemental carbon (EC) and organic carbon (OC) aerosols over the Pearl River Delta (PRD) area of China and compared the results to seasonal surface measurements, with the aim of quantifying carbonaceous aerosol sources from a "top-down" perspective. Our regional model was driven by current-best estimates of PRD EC (39.5 Gg C yr-1) and OC (32.8 Gg C yr-1) emissions and included updated secondary organic aerosol formation pathways. The simulated annual mean EC and OC concentrations were 4.0 and 7.7 μg C m-3, respectively, lower than the observed annual mean EC and OC concentrations (4.5 and 13.1 μg C m-3, respectively). We used multiple regression to match the simulated EC against seasonal mean observations. The resulting top-down estimate for EC emission in the PRD area was 52.9 ± 8.0 Gg C yr-1. We estimated the OC emission in the PRD area to be 60.2 ± 10.3 Gg C yr-1, based on the top-down EC emission estimate and the primary OC / EC ratios derived from bottom-up statistics. Using these top-down emission estimates, the simulated average annual mean EC and OC concentrations were improved to 4.4 and 9.5 μg C m-3, respectively, closer to the observations. Secondary sources accounted for 42 % of annual mean surface OC in our top-down simulations, with biogenic VOCs being the most important precursors.

  15. Global dust sources detection using MODIS Deep Blue Collection 6 aerosol products

    NASA Astrophysics Data System (ADS)

    Pérez García-Pando, C.; Ginoux, P. A.

    2015-12-01

    Our understanding of the global dust cycle is limited by a dearth of information about dust sources, especially small-scale features which could account for a large fraction of global emissions. Remote sensing sensors are the most useful tool to locate dust sources. These sensors include microwaves, visible channels, and lidar. On the global scale, major dust source regions have been identified using polar orbiting satellite instruments. The MODIS Deep Blue algorithm has been particularly useful to detect small-scale sources such as floodplains, alluvial fans, rivers, and wadis , as well as to identify anthropogenic sources from agriculture. The recent release of Collection 6 MODIS aerosol products allows to extend dust source detection to the entire land surfaces, which is quite useful to identify mid to high latitude dust sources and detect not only dust from agriculture but fugitive dust from transport and industrial activities. This presentation will overview the advantages and drawbacks of using MODIS Deep Blue for dust detection, compare to other instruments (polar orbiting and geostationary). The results of Collection 6 with a new dust screening will be compared against AERONET. Applications to long range transport of anthropogenic dust will be presented.

  16. Source term and radiological consequences of the Chernobyl accident

    SciTech Connect

    Mourad, R.; Snell, V.

    1987-01-01

    The objective of this work is to assess the source term and to evaluate the maximum hypothetical individual doses in European countries (including the Soviet Union) from the Chernobyl accident through the analyses of measurements of meteorological data, radiation fields, and airborne and deposited activity in these countries. Applying this information to deduce the source term involves a reversal of the techniques of nuclear accident analysis, which estimate the off-site consequences of postulated accidents. In this study the authors predict the quantities of radionuclides that, if released at Chernobyl and following the calculated trajectories, would explain and unify the observed radiation levels and radionuclide concentrations as measured by European countries and the Soviet Union. The simulation uses the PEAR microcomputer program following the methodology described in Canadian Standards Association standard N288.2. The study was performed before the Soviets published their estimate of the source term and the two results are compared.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  18. Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter

    NASA Astrophysics Data System (ADS)

    Hu, Weiwei; Hu, Min; Hu, Wei; Jimenez, Jose L.; Yuan, Bin; Chen, Wentai; Wang, Ming; Wu, Yusheng; Chen, Chen; Wang, Zhibin; Peng, Jianfei; Zeng, Limin; Shao, Min

    2016-02-01

    To investigate the seasonal characteristics of submicron aerosol (PM1) in Beijing urban areas, a high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) was utilized at an urban site in summer (August to September 2011) and winter (November to December 2010), coupled with multiple state of the art online instruments. The average mass concentrations of PM1 (60-84 µg m-3) and its chemical compositions in different campaigns of Beijing were relatively consistent in recent years. In summer, the daily variations of PM1 mass concentrations were stable and repeatable. Eighty-two percent of the PM1 mass concentration on average was composed of secondary species, where 62% is secondary inorganic aerosol and 20% secondary organic aerosol (SOA). In winter, PM1 mass concentrations changed dramatically because of the different meteorological conditions. The high average fraction (58%) of primary species in PM1 including primary organic aerosol (POA), black carbon, and chloride indicates primary emissions usually played a more important role in the winter. However, aqueous chemistry resulting in efficient secondary formation during occasional periods with high relative humidity may also contribute substantially to haze in winter. Results of past OA source apportionment studies in Beijing show 45-67% of OA in summer and 22-50% of OA in winter can be composed of SOA. Based on the source apportionment results, we found 45% POA in winter and 61% POA in summer are from nonfossil sources, contributed by cooking OA in both seasons and biomass burning OA (BBOA) in winter. Cooking OA, accounting for 13-24% of OA, is an important nonfossil carbon source in all years of Beijing and should not be neglected. The fossil sources of POA include hydrocarbon-like OA from vehicle emissions in both seasons and coal combustion OA (CCOA) in winter. The CCOA and BBOA were the two main contributors (57% of OA) for the highest OA concentrations (>100 µg m-3) in winter. The POA

  19. Oil Sands Operations in Alberta, Canada: A large source of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Liggio, J.; Li, S. M.; Hayden, K.; Taha, Y. M.; Stroud, C.; Darlington, A. L.; Drollette, B.; Gordon, M.; Lee, P.; Liu, P.; Leithead, A.; Moussa, S.; Wang, D.; O'Brien, J.; Mittermeier, R. L.; Brook, J.; Lu, G.; Staebler, R. M.; Han, Y.; Tokarek, T. W.; Osthoff, H. D.; Makar, P.; Zhang, J.; Plata, D.; Gentner, D. R.

    2015-12-01

    Little is known of the reaction products of emissions to the atmosphere from extraction of oil from unconventional sources in the oil sands (OS) region of Alberta, Canada. This study examines these reaction products, and in particular, the extent to which they form secondary organic aerosol (SOA), which can significantly contribute to regional particulate matter formation. An aircraft measurement campaign was conducted over the Athabasca oil sands region between August 13 and September 7, 2013. A broad suite of measurements were made during 22 flights, including organic aerosol mass and composition with a High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and organic aerosol gas-phase precursors by Proton Transfer Reaction (PTR) and off-line gas chromatography mass spectrometry. Large concentrations of organic aerosol were measured downwind of the OS region, which we show to be entirely secondary in nature. Laboratory experiments demonstrated that bitumen (the mined product) contains semi-volatile vapours in the C12-C18 range that will be emitted at ambient temperatures. When oxidized, these vapours form SOA with highly similar HR-ToF-AMS spectra to the SOA measured in the flights. Box modelling of the OS plume evolution indicated that the measured levels of traditional volatile organic compounds (VOCs) are not capable of accounting for the amount of SOA formed in OS plumes. This discrepancy is only reconciled in the model by including bitumen vapours along with their oxidation and condensation into the model. The concentration of bitumen vapours required to produce SOA matching observations is similar to that of traditional VOC precursors of SOA. It was further estimated that the cumulative SOA mass formation approximately 100 km downwind of the OS during these flights, and under these meteorological conditions was up to 82 tonnes/day. The combination of airborne measurements, laboratory experiments and box modelling indicated that semi

  20. Real-time measurements of ambient aerosols in a polluted Indian city: Sources, characteristics, and processing of organic aerosols during foggy and nonfoggy periods

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Bhattu, Deepika; Gupta, Tarun; Tripathi, Sachchida N.; Canagaratna, Manjula R.

    2015-09-01

    A detailed time-resolved chemical characterization of ambient nonrefractory submicron aerosols (NR-PM1) was conducted for the first time in India. The measurements were performed during the winter (November 2011 to January 2012) in a heavily polluted city of Kanpur, which is situated in the Indo-Gangetic Plain. Real-time measurements provided new insights into the sources and evolution of organic aerosols (OA) that could not be obtained using previously deployed filter-based measurements at this site. The average NR-PM1 loading was very high (>100 µg/m3) throughout the study, with OA contributing approximately 70% of the total aerosol mass. Source apportionment of the OA using positive matrix factorization revealed large contributions from fresh and aged biomass burning OA throughout the entire study period. A back trajectory analysis showed that the polluted air masses were affected by local sources and distant source regions where the burning of paddy residues occurs annually during winter. Several fog episodes were encountered during the study, and the OA composition varied between foggy and nonfoggy periods, with higher oxygen to carbon (O/C) ratios during the foggy periods. The evolution of OA and their elemental ratios (O:C and H:C) were investigated for the possible effects of fog processing.

  1. Fingerprinting the Impacts of Aerosols on Long-Term Trends of the Indian Summer Monsoon Regional Rainfall

    NASA Technical Reports Server (NTRS)

    Laul, K. M.; Kim, K. M.

    2010-01-01

    In this paper, we present corroborative observational evidences from satellites, in-situ observations, and re-analysis data showing possible impacts of absorbing aerosols (black carbon and dust) on subseasonal and regional summer monsoon rainfall over India. We find that increased absorbing aerosols in the Indo-Gangetic Plain in recent decades may have lead to long-term warming of the upper troposphere over northern India and the Tibetan Plateau, enhanced rainfall in northern India and the Himalayas foothill regions in the early part (may-June) of the monsoon season, followed by diminished rainfall over central and southern India in the latter part (July-August) of the monsoon season. These signals which are consistent with current theories of atmospheric heating and solar dimming by aerosol and induced cloudiness in modulating the Indian monsoon, would have been masked by conventional method of using al-India rainfall averaged over the entire monsoon season.

  2. Flowsheets and source terms for radioactive waste projections

    SciTech Connect

    Forsberg, C.W.

    1985-03-01

    Flowsheets and source terms used to generate radioactive waste projections in the Integrated Data Base (IDB) Program are given. Volumes of each waste type generated per unit product throughput have been determined for the following facilities: uranium mining, UF/sub 6/ conversion, uranium enrichment, fuel fabrication, boiling-water reactors (BWRs), pressurized-water reactors (PWRs), and fuel reprocessing. Source terms for DOE/defense wastes have been developed. Expected wastes from typical decommissioning operations for each facility type have been determined. All wastes are also characterized by isotopic composition at time of generation and by general chemical composition. 70 references, 21 figures, 53 tables.

  3. Sea spray aerosol as a unique source of ice nucleating particles

    PubMed Central

    DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; Prather, Kimberly A.; Ruppel, Matthew J.; Mason, Ryan H.; Irish, Victoria E.; Lee, Taehyoung; Hwang, Chung Yeon; Snider, Jefferson R.; McMeeking, Gavin R.; Dhaniyala, Suresh; Lewis, Ernie R.; Wentzell, Jeremy J. B.; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M.; Ault, Andrew P.; Axson, Jessica L.; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M. Dale; Deane, Grant B.; Mayol-Bracero, Olga L.; Grassian, Vicki H.; Bertram, Timothy H.; Bertram, Allan K.; Moffett, Bruce F.; Franc, Gary D.

    2016-01-01

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

  4. Sea spray aerosol as a unique source of ice nucleating particles.

    PubMed

    DeMott, Paul J; Hill, Thomas C J; McCluskey, Christina S; Prather, Kimberly A; Collins, Douglas B; Sullivan, Ryan C; Ruppel, Matthew J; Mason, Ryan H; Irish, Victoria E; Lee, Taehyoung; Hwang, Chung Yeon; Rhee, Tae Siek; Snider, Jefferson R; McMeeking, Gavin R; Dhaniyala, Suresh; Lewis, Ernie R; Wentzell, Jeremy J B; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M; Ault, Andrew P; Axson, Jessica L; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M Dale; Deane, Grant B; Mayol-Bracero, Olga L; Grassian, Vicki H; Bertram, Timothy H; Bertram, Allan K; Moffett, Bruce F; Franc, Gary D

    2016-05-24

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

  5. Sea spray aerosol as a unique source of ice nucleating particles

    NASA Astrophysics Data System (ADS)

    DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; Prather, Kimberly A.; Collins, Douglas B.; Sullivan, Ryan C.; Ruppel, Matthew J.; Mason, Ryan H.; Irish, Victoria E.; Lee, Taehyoung; Hwang, Chung Yeon; Siek Rhee, Tae; Snider, Jefferson R.; McMeeking, Gavin R.; Dhaniyala, Suresh; Lewis, Ernie R.; Wentzell, Jeremy J. B.; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M.; Ault, Andrew P.; Axson, Jessica L.; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M. Dale; Deane, Grant B.; Mayol-Bracero, Olga L.; Grassian, Vicki H.; Bertram, Timothy H.; Bertram, Allan K.; Moffett, Bruce F.; Franc, Gary D.

    2016-05-01

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

  6. Elemental analysis of aerosols in Tehran's atmosphere using PIXE and identification of pollution sources.

    PubMed

    Esmaili, N; Khashman, S; Lamehi-Rachti, M; Agha Aligol, D; Shokouhi, F; Oliaiy, P; Farmahini Farahani, M

    2014-11-01

    In this study, the proton-induced X-ray emission (PIXE) technique has been applied to measure the elemental composition and concentrations of particulate matter of 220 samples of aerosols in Tehran's atmosphere within a 450-day time interval starting from March 2009 and ending in June 2010, covering all four seasons. PIXE analysis shows the samples are comprised of various elements including Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, and Pb. Also, to obtain more information about the sources of pollution and to identify the major sources of urban particulate matter, principal component analysis (PCA) was used. Furthermore, micro-PIXE was performed to study individual aerosols in some samples. Results revealed that the concentration of elements originating from vehicle emissions increases three times in winter; whereas the concentration of elements with soil origin remains constant. Based on wind rose maps, it is inferred that the high concentrations of the elements Al, Si, K, Ca, Ti, Mn, and Fe are associated with natural dust brought by winds into Tehran from the west. PMID:25027779

  7. Spallation Neutron Source Accident Terms for Environmental Impact Statement Input

    SciTech Connect

    Devore, J.R.; Harrington, R.M.

    1998-08-01

    This report is about accidents with the potential to release radioactive materials into the environment surrounding the Spallation Neutron Source (SNS). As shown in Chap. 2, the inventories of radioactivity at the SNS are dominated by the target facility. Source terms for a wide range of target facility accidents, from anticipated events to worst-case beyond-design-basis events, are provided in Chaps. 3 and 4. The most important criterion applied to these accident source terms is that they should not underestimate potential release. Therefore, conservative methodology was employed for the release estimates. Although the source terms are very conservative, excessive conservatism has been avoided by basing the releases on physical principles. Since it is envisioned that the SNS facility may eventually (after about 10 years) be expanded and modified to support a 4-MW proton beam operational capability, the source terms estimated in this report are applicable to a 4-MW operating proton beam power unless otherwise specified. This is bounding with regard to the 1-MW facility that will be built and operated initially. See further discussion below in Sect. 1.2.

  8. Common Calibration Source for Monitoring Long-term Ozone Trends

    NASA Technical Reports Server (NTRS)

    Kowalewski, Matthew

    2004-01-01

    Accurate long-term satellite measurements are crucial for monitoring the recovery of the ozone layer. The slow pace of the recovery and limited lifetimes of satellite monitoring instruments demands that datasets from multiple observation systems be combined to provide the long-term accuracy needed. A fundamental component of accurately monitoring long-term trends is the calibration of these various instruments. NASA s Radiometric Calibration and Development Facility at the Goddard Space Flight Center has provided resources to minimize calibration biases between multiple instruments through the use of a common calibration source and standardized procedures traceable to national standards. The Facility s 50 cm barium sulfate integrating sphere has been used as a common calibration source for both US and international satellite instruments, including the Total Ozone Mapping Spectrometer (TOMS), Solar Backscatter Ultraviolet 2 (SBUV/2) instruments, Shuttle SBUV (SSBUV), Ozone Mapping Instrument (OMI), Global Ozone Monitoring Experiment (GOME) (ESA), Scanning Imaging SpectroMeter for Atmospheric ChartographY (SCIAMACHY) (ESA), and others. We will discuss the advantages of using a common calibration source and its effects on long-term ozone data sets. In addition, sphere calibration results from various instruments will be presented to demonstrate the accuracy of the long-term characterization of the source itself.

  9. Long-term and seasonal variability of the aerosol optical depth at Mount Kasprowy Wierch (Poland)

    NASA Astrophysics Data System (ADS)

    Markowicz, Krzysztof M.; Uscka-Kowalkowska, Joanna

    2015-03-01

    This paper presents the results of long-term observations (1964-2003) of direct solar radiation, to determine aerosol optical depth (AOD), made with a Linke-Feussner actinometer at the Tatra Mountain Meteorological Observatory on Mount Kasprowy Wierch (1991 m above sea level, 49.233°N, 19.982°E). To this end, broadband direct solar flux (0.29-2.9 µm) and wideband solar radiation measured with OG530 and RG630 filters are used to estimate the broadband and wideband (0.53-0.63 µm) AOD. The inversion algorithm used is based on the MODTRAN (MODerate resolution atmospheric TRANsmission) radiative transfer model applied to estimate direct flux for aerosol-free atmosphere. Total water vapor content, which accounts for the largest extinction of clear-sky direct flux, was obtained by radio sounding from the Poprad-Ganovce station (33 km from Mount Kasprowy Wierch) and from water vapor pressure measurements at the Observatory. The almost 900 clear-sky observations, performed close to noon time, found a significant long-term reduction of AOD. AOD decadal trends were -0.006 (-8 ± 4% [2σ]) with a 95% confidence interval of ± 0.003 and -0.014 (-13 ± 4% [2σ]) with a 95% confidence interval of ± 0.004 for broadband and wideband, respectively. Similar trends, but for years with negligible contamination of volcanic aerosol, are -0.012 (-16 ± 6% [2σ]) and -0.018 (-17 ± 6% [2σ]) with a 95% confidence interval of ± 0.003 and ± 0.004. However, positive AOD trends (from 0 to 0.04 per decade) were found between 1964 and 1983 and negative AOD trends (from -0.016 to -0.035 per decade) were found between 1984 and 2003. Changes of the AOD trends between both periods are associated with global dimming and brightening phenomenon, which took place in the second half of the twentieth century and at the beginning of the 21st century. The long-term mean broadband and wideband AOD were 0.07 ± 0.01 and 0.11 ± 0.02, respectively. Both quantities show a significant annual cycle, with

  10. Long-term trends of aerosol carbon and nitrogen, their stable isotopic compositions, and water-soluble organic carbon in the western North Pacific

    NASA Astrophysics Data System (ADS)

    Kawamura, K.; Tachibana, E.; Umomoto, N.

    2009-12-01

    The western North Pacific is an outflow region of Asian dusts and pollutants. A rapid industrial development in China and East Asian countries for last two decades may have seriously altered the air quality of the North Pacific. However, long-term changes of atmospheric composition have not been studied in this region. To better understand long-term atmospheric changes in the western North Pacific, we collected marine aerosols on weekly basis in 2001-2009 at a remote island, Chichijima (27°04'E; 142°13'N) using high volume air sampler and pre-combusted quartz filter. The island is located in the boundary of westerly (winter and spring) and trade wind (summer and autumn) regimes. Here, the aerosol samples were analyzed for total carbon (TC) and nitrogen (TN) and their stable isotopic compositions as well as water-soluble organic carbon (WSOC). Concentrations of aerosol TC and TN were in a range of 0.21-4.58 (average 1.07) ug/m3 and 0.01-3.43 (av. 0.29) ng/m3. These values are ca. 20 times lower than the concentrations in urban Tokyo. C/N weight ratios ranged from 0.50 to 41 (av. 6.6) with summer maxima. Both TC and TN showed a gradual increase with winter/spring maxima probably due to the enhanced anthropogenic activities such as fossil fuel combustion and fertilizer usage in East Asia. On the other hand, stable carbon isotopic ratios (d13C) of TC ranged from -27.3 to -15.1‰; however, no systematic trend was detected. Nitrogen isotopic ratios of TN (d15N) ranged from +1.56 to +25.2‰ with lower values in winter and higher values in summer. Interestingly, d15N values showed a long-term trend of increase by 4‰ from 2001 to 2009. This may be caused by an increased emission of nitrogen species (NH3, NOx) from biomass burning sources in East Asia and other regions. WSOC (0.05-2.46 ug/m3, av. 0.40 ug/m3) also showed a long-term increase probably due to the increased emissions of organic aerosols and their precursors and subsequent oxidations in the atmosphere

  11. Elucidating carbonaceous aerosol sources by the stable carbon δ13CTC ratio in size-segregated particles

    NASA Astrophysics Data System (ADS)

    Masalaite, A.; Remeikis, V.; Garbaras, A.; Dudoitis, V.; Ulevicius, V.; Ceburnis, D.

    2015-05-01

    Carbonaceous aerosol sources were investigated by measuring the stable carbon isotope ratio (δ13CTC) in size-segregated aerosol particles. The samples were collected with a micro-orifice uniform deposit impactor (MOUDI) in 11 size intervals ranging from 0.056 μm to 18 μm. The aerosol particle size distribution obtained from combined measurements with a scanning mobility particle sizer (SMPS; TSI 3936) and an aerosol particle sizer (APS; TSI 3321) is presented for comparison with MOUDI data. The analysis of δ13CTC values revealed that the total carbonaceous matter in size-segregated aerosol particles significantly varied from - 23.4 ± 0.1‰ in a coarse mode to - 30.1 ± 0.5‰ in a fine mode. A wide range of the δ13CTC values of size-segregated aerosol particles suggested various sources of aerosol particles contributing to carbonaceous particulate matter. Therefore, the source mixing equation was applied to verify the idea of mixing of two sources: continental non-fossil and fossil fuel combustion. The obtained δ13CTC value of aerosol particles originating from fossil fuel combustion was - 28.0 to - 28.1‰, while the non-fossil source δ13CTC value was in the range of - 25.0 to - 25.5‰. The two source mixing model applied to the size-segregated samples revealed that the fossil fuel combustion source contributed from 100% to 60% to the carbonaceous particulate matter in the fine mode range (Dp < 1 μm). Meanwhile, the second source, continental non-fossil, was the main contributor in the coarse fraction (Dp > 2 μm). The particle range from 0.5 to 2.0 μm was identified as a transition region where two sources almost equally contributed to carbonaceous particulate matter. The proposed mixing model offers an alternative method for determining major carbonaceous matter sources where radiocarbon analysis may lack the sensitivity (as in size-segregated samples).

  12. SARNET: Integrating Severe Accident Research in Europe - Safety Issues in the Source Term Area

    SciTech Connect

    Haste, T.; Giordano, P.; Micaelli, J.-C.; Herranz, L.

    2006-07-01

    conditions for new experiments. Regarding predictability of iodine species exiting the Reactor Coolant System (RCS), which affects the amount entering the containment, iodine behaviour in the circuit and silver-indium-cadmium (SIC) release have been reviewed. New experiments are being discussed and performed, and SIC degradation and release models are being improved. For the radioactive aerosol source term, work is conducted in the risk-relevant areas of steam generator (SG) tube rupture, transport through cracks in containment walls and revaporization from previous deposits in the RCS that could lead to a delayed source term. Models for aerosol retention in containment cracks and interpretation of data on retention in the SG secondary side are proposed. For radioactive iodine release to the environment, many physical and chemical processes affect the iodine concentration in the containment atmosphere; of these effects, mass transfer phenomena and radiolytic oxidation are being investigated first. (authors)

  13. Carbonaceous aerosols and pollutants over Delhi urban environment: Temporal evolution, source apportionment and radiative forcing.

    PubMed

    Bisht, D S; Dumka, U C; Kaskaoutis, D G; Pipal, A S; Srivastava, A K; Soni, V K; Attri, S D; Sateesh, M; Tiwari, S

    2015-07-15

    Particulate matter (PM2.5) samples were collected over Delhi, India during January to December 2012 and analysed for carbonaceous aerosols and inorganic ions (SO4(2-) and NO3(-)) in order to examine variations in atmospheric chemistry, combustion sources and influence of long-range transport. The PM2.5 samples are measured (offline) via medium volume air samplers and analysed gravimetrically for carbonaceous (organic carbon, OC; elemental carbon, EC) aerosols and inorganic ions (SO4(2-) and NO3(-)). Furthermore, continuous (online) measurements of PM2.5 (via Beta-attenuation analyser), black carbon (BC) mass concentration (via Magee scientific Aethalometer) and carbon monoxide (via CO-analyser) are carried out. PM2.5 (online) range from 18.2 to 500.6μgm(-3) (annual mean of 124.6±87.9μgm(-3)) exhibiting higher night-time (129.4μgm(-3)) than daytime (103.8μgm(-3)) concentrations. The online concentrations are 38% and 28% lower than the offline during night and day, respectively. In general, larger night-time concentrations are found for the BC, OC, NO3(-)and SO4(2-), which are seasonally dependent with larger differences during late post-monsoon and winter. The high correlation (R(2)=0.74) between OC and EC along with the OC/EC of 7.09 (day time) and 4.55 (night-time), suggest significant influence of biomass-burning emissions (burning of wood and agricultural waste) as well as secondary organic aerosol formation during daytime. Concentrated weighted trajectory (CWT) analysis reveals that the potential sources for the carbonaceous aerosols and pollutants are local emissions within the urban environment and transported smoke from agricultural burning in northwest India during post-monsoon. BC radiative forcing estimates result in very high atmospheric heating rates (~1.8-2.0Kday(-1)) due to agricultural burning effects during the 2012 post-monsoon season. PMID:25864155

  14. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

    NASA Astrophysics Data System (ADS)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-08-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine

  15. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

    NASA Astrophysics Data System (ADS)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-11-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play

  16. Improved source term estimation using blind outlier detection

    NASA Astrophysics Data System (ADS)

    Martinez-Camara, Marta; Bejar Haro, Benjamin; Vetterli, Martin; Stohl, Andreas

    2014-05-01

    Emissions of substances into the atmosphere are produced in situations such as volcano eruptions, nuclear accidents or pollutant releases. It is necessary to know the source term - how the magnitude of these emissions changes with time - in order to predict the consequences of the emissions, such as high radioactivity levels in a populated area or high concentration of volcanic ash in an aircraft flight corridor. However, in general, we know neither how much material was released in total, nor the relative variation of emission strength with time. Hence, estimating the source term is a crucial task. Estimating the source term generally involves solving an ill-posed linear inverse problem using datasets of sensor measurements. Several so-called inversion methods have been developed for this task. Unfortunately, objective quantitative evaluation of the performance of inversion methods is difficult due to the fact that the ground truth is unknown for practically all the available measurement datasets. In this work we use the European Tracer Experiment (ETEX) - a rare example of an experiment where the ground truth is available - to develop and to test new source estimation algorithms. Knowledge of the ground truth grants us access to the additive error term. We show that the distribution of this error is heavy-tailed, which means that some measurements are outliers. We also show that precisely these outliers severely degrade the performance of traditional inversion methods. Therefore, we develop blind outlier detection algorithms specifically suited to the source estimation problem. Then, we propose new inversion methods that combine traditional regularization techniques with blind outlier detection. Such hybrid methods reduce the error of reconstruction of the source term up to 45% with respect to previously proposed methods.

  17. Sources of submicron aerosol during fog-dominated wintertime at Kanpur.

    PubMed

    Gupta, Tarun; Mandariya, Anil

    2013-08-01

    The main objective of this atmospheric study was to determine the major sources of PM1 (particles having aerodynamic diameter <1.0 μm) within and near the city of Kanpur, in the Indo-Gangetic Plain. Day and night, 10 h long each, filter-based aerosol samples were collected for 4 months (November 2009 to February 2010) throughout the winter season. These samples were subjected to gravimetric and quantitative chemical analyses for determining water-soluble ions (NH4 (+), F(-), Cl(-), NO3 (-), and SO4 (2-)) using an ion chromatograph and trace elements using an inductively coupled plasma-optical emission spectrometer. The mean PM1 mass concentrations were recorded as 114 ± 71 μg/m(3) (day) and 143 ± 86 μg/m(3) (night), respectively. A significantly higher diurnal contribution of ions (NH4 (+), F(-), Cl(-), NO3 (-), and SO4 (2-)) in PM1 mass was observed during the fog-affected days and nights throughout the winter season, for which the average values were recorded as 38.09 ± 13.39 % (day) and 34.98 ± 12.59 % (night), respectively, of the total PM1 mass. This chemical dataset was then used in a source-receptor model, UNMIX, and the model results are described in detail. UNMIX provided a maximum number of five source factors, including crustal material, composite vehicle, secondary aerosol, coal combustion, and iron/steel production and metallurgical industries, as the dominant air pollution sources for this study. PMID:23443945

  18. Metals and Rare Earth Elements in polar aerosol as specific markers of natural and anthropogenic aerosol sources areas and atmospheric transport processes

    NASA Astrophysics Data System (ADS)

    Giardi, Fabio; Becagli, Silvia; Caiazzo, Laura; Cappelletti, David; Grotti, Marco; Malandrino, Mery; Salzano, Roberto; Severi, Mirko; Traversi, Rita; Udisti, Roberto

    2016-04-01

    Metals and Rare Earth Elements (REEs) in the aerosol have conservative properties from the formation to the deposition and can be useful to identify and quantify their natural and anthropic sources and to study the atmospheric transport processes. In spite of their importance relatively little is known about metals and especially REEs in the Artic atmosphere due to their low concentration in such environment. The present work reports the first attempt to determine and interpret the behaviour of metals and REEs in polar aerosol at high temporal resolution. Daily PM10 samples of arctic atmospheric particulate were collected on Teflon filters, during six spring-summer campaigns, since 2010, in the laboratory of Gruvebadet in Ny Ålesund (78°56' N, 11°56' E, Svalbard Islands, Norway). Chemical analyses were carried out through Inductively Coupled Plasma Mass Spectrometer provided with a desolvation nebulizer inlet system, allowing to reduce isobaric interferences and thus to quantify trace and ultra-trace metals in very low concentration in the Arctic aerosol samples. The results are useful in order to study sources areas, transport processes and depositional effects of natural and anthropic atmospheric particulate reaching the Arctic from southern industrialized areas; moreover, the observed seasonal trends give information about the different impact of natural and anthropic emissions driven by phenomena such as the Arctic Haze and the melting of the snow. In particular Rare Earth Elements (often in the ppt range) can be considered as soil's fingerprints of the particulate source areas and their determination, together with air-mass backtrajectory analysis, allow to identify dust source areas for the arctic mineral aerosol.

  19. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    NASA Astrophysics Data System (ADS)

    Woody, M. C.; Baker, K. R.; Hayes, P. L.; Jimenez, J. L.; Koo, B.; Pye, H. O. T.

    2015-10-01

    Community Multiscale Air Quality (CMAQ) model simulations utilizing the volatility basis set (VBS) treatment for organic aerosols (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of organic aerosol (OA) in southern California. CMAQ-VBS (OA lumped by volatility, semivolatile POA) underpredicted total organic carbon (OC) at CSN (-25.5 % Normalized Median Bias (NMdnB)) and IMPROVE (-63.9 % NMdnB) locations and total OC was underpredicted to a greater degree compared to the CMAQ-AE6 (9.9 and -55.7 % NMdnB, respectively; semi-explicit OA treatment, SOA lumped by parent hydrocarbon, nonvolatile POA). However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA indicated that CMAQ-VBS better represented the diurnal profile and the primary/secondary split of OA. CMAQ-VBS secondary organic aerosol (SOA) underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate of SOA) concentration by a factor of 5.2 (4.7 μg m-3 measured vs. 0.9 μg m-3 modeled), a considerable improvement to CMAQ-AE6 SOA predictions, which were approximately 24× lower than the average AMS OOA concentration. We use two new methods, based on species ratios and on a simplified SOA parameterization from the observations, to apportion the SOA underprediction for CMAQ-VBS to too slow photochemical oxidation (estimated as 1.5× lower than observed at Pasadena using - log (NOx: NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2× for Pasadena), and too low emissions or too high dispersion for the Pasadena site (estimated to be 1.6 to 2.3× too low/high). The first and third factors will be similar for CMAQ-AE6, while the intrinsic SOA formation

  20. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    DOE PAGESBeta

    Woody, Matthew C.; Baker, Kirk R.; Hayes, Patrick L.; Jimenez, Jose L.; Koo, Bonyoung; Pye, Havala O. T.

    2016-03-29

    In this paper, Community Multiscale Air Quality (CMAQ) model simulations utilizing the traditional organic aerosol (OA) treatment (CMAQ-AE6) and a volatility basis set (VBS) treatment for OA (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of OA in southern California. Traditionally, CMAQ treats primary organic aerosol (POA) as nonvolatile and uses a two-product framework to represent secondary organic aerosol (SOA) formation. CMAQ-VBS insteadmore » treats POA as semivolatile and lumps OA using volatility bins spaced an order of magnitude apart. The CMAQ-VBS approach underpredicted organic carbon (OC) at IMPROVE and CSN sites to a greater degree than CMAQ-AE6 due to the semivolatile POA treatment. However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA, indicated that CMAQ-VBS better represented the diurnal profile and primary/secondary split of OA. CMAQ-VBS SOA underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate for SOA) concentration by a factor of 5.2, representing a considerable improvement to CMAQ-AE6 SOA predictions (factor of 24 lower than AMS). We use two new methods, one based on species ratios (SOA/ΔCO and SOA/Ox) and another on a simplified SOA parameterization, to apportion the SOA underprediction for CMAQ-VBS to slow photochemical oxidation (estimated as 1.5 × lower than observed at Pasadena using -log(NOx:NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2 × for Pasadena), and low emissions or excessive dispersion for the Pasadena site (estimated to be 1.6 to 2.3 × too low/excessive). The first and third factors are common to CMAQ-AE6, while the intrinsic SOA formation

  1. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    NASA Astrophysics Data System (ADS)

    Woody, Matthew C.; Baker, Kirk R.; Hayes, Patrick L.; Jimenez, Jose L.; Koo, Bonyoung; Pye, Havala O. T.

    2016-03-01

    Community Multiscale Air Quality (CMAQ) model simulations utilizing the traditional organic aerosol (OA) treatment (CMAQ-AE6) and a volatility basis set (VBS) treatment for OA (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of OA in southern California. Traditionally, CMAQ treats primary organic aerosol (POA) as nonvolatile and uses a two-product framework to represent secondary organic aerosol (SOA) formation. CMAQ-VBS instead treats POA as semivolatile and lumps OA using volatility bins spaced an order of magnitude apart. The CMAQ-VBS approach underpredicted organic carbon (OC) at IMPROVE and CSN sites to a greater degree than CMAQ-AE6 due to the semivolatile POA treatment. However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA, indicated that CMAQ-VBS better represented the diurnal profile and primary/secondary split of OA. CMAQ-VBS SOA underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate for SOA) concentration by a factor of 5.2, representing a considerable improvement to CMAQ-AE6 SOA predictions (factor of 24 lower than AMS). We use two new methods, one based on species ratios (SOA/ΔCO and SOA/Ox) and another on a simplified SOA parameterization, to apportion the SOA underprediction for CMAQ-VBS to slow photochemical oxidation (estimated as 1.5 × lower than observed at Pasadena using -log(NOx : NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2 × for Pasadena), and low emissions or excessive dispersion for the Pasadena site (estimated to be 1.6 to 2.3 × too low/excessive). The first and third factors are common to CMAQ-AE6, while the intrinsic SOA formation efficiency for that model is

  2. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    DOE PAGESBeta

    Woody, Matthew C.; Baker, Kirk R.; Hayes, Patrick L.; Jimenez, Jose L.; Koo, Bonyoung; Pye, Havala O. T.

    2016-03-29

    Community Multiscale Air Quality (CMAQ) model simulations utilizing the traditional organic aerosol (OA) treatment (CMAQ-AE6) and a volatility basis set (VBS) treatment for OA (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of OA in southern California. Traditionally, CMAQ treats primary organic aerosol (POA) as nonvolatile and uses a two-product framework to represent secondary organic aerosol (SOA) formation. CMAQ-VBS instead treats POA asmore » semivolatile and lumps OA using volatility bins spaced an order of magnitude apart. The CMAQ-VBS approach underpredicted organic carbon (OC) at IMPROVE and CSN sites to a greater degree than CMAQ-AE6 due to the semivolatile POA treatment. However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA, indicated that CMAQ-VBS better represented the diurnal profile and primary/secondary split of OA. CMAQ-VBS SOA underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate for SOA) concentration by a factor of 5.2, representing a considerable improvement to CMAQ-AE6 SOA predictions (factor of 24 lower than AMS). We use two new methods, one based on species ratios (SOA/ΔCO and SOA/Ox) and another on a simplified SOA parameterization, to apportion the SOA underprediction for CMAQ-VBS to slow photochemical oxidation (estimated as 1.5 ×  lower than observed at Pasadena using −log(NOx : NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2 ×  for Pasadena), and low emissions or excessive dispersion for the Pasadena site (estimated to be 1.6 to 2.3 ×  too low/excessive). The first and third factors are common to CMAQ-AE6, while the intrinsic SOA formation

  3. STACE: Source Term Analyses for Containment Evaluations of transport casks

    SciTech Connect

    Seager, K. D.; Gianoulakis, S. E.; Barrett, P. R.; Rashid, Y. R.; Reardon, P. C.

    1992-01-01

    Following the guidance of ANSI N14.5, the STACE methodology provides a technically defensible means for estimating maximum permissible leakage rates. These containment criteria attempt to reflect the true radiological hazard by performing a detailed examination of the spent fuel, CRUD, and residual contamination contributions to the releasable source term. The evaluation of the spent fuel contribution to the source term has been modeled fairly accurately using the STACE methodology. The structural model predicts the cask drop load history, the mechanical response of the fuel assembly, and the probability of cladding breach. These data are then used to predict the amount of fission gas, volatile species, and fuel fines that are releasable from the cask. There are some areas where data are sparse or lacking (e.g., the quantity and size distribution of fuel rod breaches) in which experimental validation is planned. The CRUD spallation fraction is the major area where no quantitative data has been found; therefore, this also requires experimental validation. In the interim, STACE conservatively assumes a 100% spallation fraction for computing the releasable activity. The source term methodology also conservatively assumes that there is 1 Ci of residual contamination available for release in the transport cask. However, residual contamination is still by far the smallest contributor to the source term activity.

  4. Source Term Code Package: a user's guide (Mod 1)

    SciTech Connect

    Gieseke, J.A.; Cybulskis, P.; Jordan, H.; Lee, K.W.; Schumacher, P.M.; Curtis, L.A.; Wooton, R.O.; Quayle, S.F.; Kogan, V.

    1986-07-01

    As part of a major reassessment of the release of radioactive materials to the environment (source terms) in severe reactor accidents, a group of state-of-the-art computer codes was utilized to perform extensive analyses. A major product of this source term reassessment effort was a demonstrated methodology for analyzing specific accident situations to provide source term predictions. The computer codes forming this methodology have been upgraded and modified for release and further use. This system of codes has been named the Source Term Code Package (STCP) and is the subject of this user's guide. The guide is intended to provide an understanding of the STCP structure and to facilitate STCP use. The STCP was prepared for operation on a CDC system but is written in FORTRAN-77 to permit transportability. In the current version (Mod 1) of the STCP, the various calculational elements fall into four major categories represented by the codes MARCH3, TRAP-MELT3, VANESA, and NAUA/SPARC/ICEDF. The MARCH3 code is a combination of the MARCH2, CORSOR-M, and CORCON-Mod 2 codes. The TRAP-MELT3 code is a combination of the TRAP-MELT2.0 and MERGE codes.

  5. Disposal Unit Source Term (DUST) data input guide

    SciTech Connect

    Sullivan, T.M.

    1993-05-01

    Performance assessment of a low-level waste (LLW) disposal facility begins with an estimation of the rate at which radionuclides migrate out of the facility (i.e., the source term). The focus of this work is to develop a methodology for calculating the source term. In general, the source term is influenced by the radionuclide inventory, the wasteforms and containers used to dispose of the inventory, and the physical processes that lead to release from the facility (fluid flow, container degradation, wasteform leaching, and radionuclide transport). The computer code DUST (Disposal Unit Source Term) has been developed to model these processes. This document presents the models used to calculate release from a disposal facility, verification of the model, and instructions on the use of the DUST code. In addition to DUST, a preprocessor, DUSTIN, which helps the code user create input decks for DUST and a post-processor, GRAFXT, which takes selected output files and plots them on the computer terminal have been written. Use of these codes is also described.

  6. BWR ASSEMBLY SOURCE TERMS FOR WASTE PACKAGE DESIGN

    SciTech Connect

    T.L. Lotz

    1997-02-15

    This analysis is prepared by the Mined Geologic Disposal System (MGDS) Waste Package Development Department (WPDD) to provide boiling water reactor (BWR) assembly radiation source term data for use during Waste Package (WP) design. The BWR assembly radiation source terms are to be used for evaluation of radiolysis effects at the WP surface, and for personnel shielding requirements during assembly or WP handling operations. The objectives of this evaluation are to generate BWR assembly radiation source terms that bound selected groupings of BWR assemblies, with regard to assembly average burnup and cooling time, which comprise the anticipated MGDS BWR commercial spent nuclear fuel (SNF) waste stream. The source term data is to be provided in a form which can easily be utilized in subsequent shielding/radiation dose calculations. Since these calculations may also be used for Total System Performance Assessment (TSPA), with appropriate justification provided by TSPA, or radionuclide release rate analysis, the grams of each element and additional cooling times out to 25 years will also be calculated and the data included in the output files.

  7. Organic aerosol components derived from 25 AMS datasets across Europe using a newly developed ME-2 based source apportionment strategy

    NASA Astrophysics Data System (ADS)

    Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Di Marco, C. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J.-L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

    2013-09-01

    Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of EUCAARI and the intensive campaigns of EMEP during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we propose a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 datasets accounting for urban, rural, remote and high altitude sites and therefore it is likely suitable for the treatment of AMS-related ambient datasets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling evaluation purposes.

  8. Atmospheric Aerosol Source-Receptor Relationships: The Role of Coal-Fired Power Plants

    SciTech Connect

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2005-12-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of March 2005 through August 2005. Significant progress was made this project period on the source characterization, source apportionment, and deterministic modeling activities. This report highlights new data on road dust, vegetative detritus and motor vehicle emissions. For example, the results show significant differences in the composition in urban and rural road dust. A comparison of the organic of the fine particulate matter in the tunnel with the ambient provides clear evidence of the significant contribution of vehicle emissions to ambient PM. The source profiles developed from this work are being used by the source-receptor modeling activities. The report presents results on the spatial distribution of PMF-factors. The results can be grouped into three different categories: regional sources, local sources, or potentially both regional and local sources. Examples of the regional sources are the sulfate and selenium PMF-factors which most likely-represent coal fired power plants. Examples of local sources are the specialty steel and lead factors. There is reasonable correspondence between these apportionments and data from the EPA TRI and AIRS emission inventories. Detailed comparisons between PMCAMx predictions and measurements by the STN and IMPROVE measurements in the Eastern US are presented. Comparisons were made for the major aerosol components and PM{sub 2.5} mass in July 2001, October 2001, January 2002, and April 2002. The results are encouraging with average fraction biases for most species less than 0.25. The improvement of the model performance during the last two years was mainly due to the comparison of the model predictions with the continuous measurements in the Pittsburgh Supersite. Major improvements have included the descriptions: of ammonia emissions (CMU inventory), night time nitrate chemistry, EC emissions and their diurnal

  9. Molecular marker analysis as a guide to the sources of fine organic aerosols

    SciTech Connect

    Rogge, W.F.; Cass, G.R.; Hildemann, L.M.; Mazurek, M.A.; Simoneit, B.R.T.

    1992-07-01

    The molecular composition of fine particulate (D{sub p} {ge} 2 {mu}m) organic aerosol emissions from the most important sources in the Los Angeles area has been determined. Likewise, ambient concentration patterns for more than 80 single organic compounds have been measured at four urban sites (West Los Angeles, Downtown Los Angeles, Pasadena, and Rubidoux) and at one remote offshore site (San Nicolas Island). It has been found that cholesterol serves as a marker compound for emissions from charbroilers and other meat cooking operations. Vehicular exhaust being emitted from diesel and gasoline powered engines can be traced in the Los Angeles atmosphere using fossil petroleum marker compounds such as steranes and pentacyclic triterpanes (e.g., hopanes). Biogenic fine particle emission sources such as plant fragments abraded from leaf surfaces by wind and weather can be traced in the urban atmosphere. Using distinct and specific source organic tracers or assemblages of organic compounds characteristic for the sources considered it is possible to estimate the influence of different source types at any urban site where atmospheric data are available.

  10. Molecular marker analysis as a guide to the sources of fine organic aerosols

    SciTech Connect

    Rogge, W.F.; Cass, G.R. ); Hildemann, L.M. . Dept. of Civil Engineering); Mazurek, M.A. ); Simoneit, B.R.T. Environmental Geochemistry Group)

    1992-07-01

    The molecular composition of fine particulate (D[sub p] [ge] 2 [mu]m) organic aerosol emissions from the most important sources in the Los Angeles area has been determined. Likewise, ambient concentration patterns for more than 80 single organic compounds have been measured at four urban sites (West Los Angeles, Downtown Los Angeles, Pasadena, and Rubidoux) and at one remote offshore site (San Nicolas Island). It has been found that cholesterol serves as a marker compound for emissions from charbroilers and other meat cooking operations. Vehicular exhaust being emitted from diesel and gasoline powered engines can be traced in the Los Angeles atmosphere using fossil petroleum marker compounds such as steranes and pentacyclic triterpanes (e.g., hopanes). Biogenic fine particle emission sources such as plant fragments abraded from leaf surfaces by wind and weather can be traced in the urban atmosphere. Using distinct and specific source organic tracers or assemblages of organic compounds characteristic for the sources considered it is possible to estimate the influence of different source types at any urban site where atmospheric data are available.

  11. Tropospheric ozone and aerosol long-term trends over the Indo-Gangetic Plain (IGP), India

    NASA Astrophysics Data System (ADS)

    Lal, D. M.; Ghude, Sachin D.; Patil, S. D.; Kulkarni, Santosh H.; Jena, Chinmay; Tiwari, S.; Srivastava, Manoj K.

    2012-10-01

    We investigate, for the first time, long-term trends in tropospheric ozone and its association with the industrial growth in large part of India. A multifunction regression model has been used to estimate the trends in tropospheric ozone between 1979 and 1992 over the Indian region. Increasing trends in tropospheric ozone are observed over most of the regions of India. Recent year's (2005-2010) data also shows the similar features. It is quite consistent with the observed trends in coal (9.2%/year) and petroleum (8.3%/year) consumption, and NOx and CO emissions in India during the study period. The regressed Tropospheric Ozone Residual (TOR) pattern during monsoon season shows large trend over the entire Indo-Gangetic region and is largest, 6-7.2% per decade, over the northeastern Gangetic plain of India. Annually, trend of about 0.4 ± 0.25 (1σ) % per year has been seen over the northeastern Gangetic region. Similar positive trend in aerosol index (AI) (1.7 ± 1.2 (1σ) % per year) is also detected over this region. The quality of correlation between TOR and AI suggested that tropospheric ozone appeared to be influenced by the increased anthropogenic activities in this region.

  12. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA): Introduction and overview

    PubMed Central

    Godleski, John J.; Rohr, Annette C.; Kang, Choong M.; Diaz, Edgar A.; Ruiz, Pablo A.; Koutrakis, Petros

    2013-01-01

    Determining the health impacts of sources and components of fine particulate matter (PM2.5) is an important scientific goal. PM2.5 is a complex mixture of inorganic and organic constituents that are likely to differ in their potential to cause adverse health outcomes. The Toxicological Evaluation of Realistic Emissions of Source Aerosols (TERESA) study focused on two PM sources—coal-fired power plants and mobile sources—and sought to investigate the toxicological effects of exposure to emissions from these sources. The set of papers published here document the power plant experiments. TERESA attempted to delineate health effects of primary particles, secondary (aged) particles, and mixtures of these with common atmospheric constituents. TERESA involved withdrawal of emissions from the stacks of three coal-fired power plants in the United States. The emissions were aged and atmospherically transformed in a mobile laboratory simulating downwind power plant plume processing. Toxicological evaluations were carried out in laboratory rats exposed to different emission scenarios with extensive exposure characterization. The approach employed in TERESA was ambitious and innovative. Technical challenges included the development of stack sampling technology that prevented condensation of water vapor from the power plant exhaust during sampling and transfer, while minimizing losses of primary particles; development and optimization of a photochemical chamber to provide an aged aerosol for animal exposures; development and evaluation of a denuder system to remove excess gaseous components; and development of a mobile toxicology laboratory. This paper provides an overview of the conceptual framework, design, and methods employed in the study. PMID:21639692

  13. Carbonaceous aerosols recorded in a Southeastern Tibetan glacier: variations, sources and radiative forcing

    NASA Astrophysics Data System (ADS)

    Wang, M.; Xu, B.; Cao, J.; Tie, X.; Wang, H.; Zhang, R.; Qian, Y.; Rasch, P. J.; Zhao, S.; Wu, G.; Zhao, H.; Joswiak, D. R.; Li, J.; Xie, Y.

    2014-07-01

    High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956-2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of OC / BC ratio with higher values in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source-receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia is a primary contributor during the non-monsoon season (October to May) (81%) and on an annual basis (74%), followed by East Asia (14% and 21%, respectively). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia as the primary contributor. Moreover, the increasing trend of OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice core record.

  14. Atmospheric chemistry of nitrogenous aerosols in northeastern Asia: biological sources and secondary formation

    NASA Astrophysics Data System (ADS)

    Pavuluri, C. M.; Kawamura, K.; Fu, P. Q.

    2015-09-01

    To better understand the sources of nitrogenous aerosols, particularly water-soluble organic nitrogen (WSON) and water-insoluble organic nitrogen (WION), in northeastern Asia, we measured total nitrogen (TN) and water-soluble total nitrogen (WSTN) as well as nitrogen isotope ratios (δ15N) of TN (δ15NTN) and WSTN (δ15NWSTN) in the total suspended particulate (TSP) samples collected from Sapporo, northern Japan, for a 1-year period. In general, WION was more abundant (126 ± 117 ng m-3), whereas WSON was 89.7 ± 80.6 ng m-3, accounting for 14 ± 11 % and 9.2 ± 7.3 % of TN, respectively. WSON peaked in late autumn to winter (maximum 288 ng m-3) and WION peaked in mid-spring to early summer (454 ng m-3). δ15NTN (21.9 ± 4.1 ‰) and δ15NWSTN (25.8 ± 8.2 ‰) showed peaks in summer with relatively high ratios in late autumn. Based on the seasonal variations in WSON and WION together with organic tracers, fossil fuel combustion and biomass burning are found to be two major sources of WSON, whereas emissions of biological particles and secondary formation by reactions of biogenic secondary organic species (carbonyls) with NH3 are suggested as an important source of WION. The seasonality of δ15NTN and δ15NWSTN, together with the comparisons to literature values, implies that chemical aging (including gas-particle partitioning) and biomass burning are the causes of the enhanced values in summer and autumn, respectively. This study demonstrates that contributions of aerosol N from fossil fuel combustion and biomass burning dominate in autumn and/or winter, whereas emission of terrestrial biological particles and secondary formation from biogenic hydrocarbons and subsequent chemical aging in the atmosphere are important in spring and/or summer in northeastern Asia.

  15. Atmospheric chemistry of nitrogenous aerosols in Northeast Asia: biological sources and secondary formation

    NASA Astrophysics Data System (ADS)

    Pavuluri, C. M.; Kawamura, K.; Fu, P. Q.

    2015-04-01

    To better understand the sources of nitrogenous aerosols, particularly water-soluble organic nitrogen (WSON) and water-insoluble organic nitrogen (WION), in Northeast Asia, we measured total nitrogen (TN) and water-soluble total nitrogen (WSTN) as well as nitrogen isotope ratios (δ15N) of TN (δ15NTN) and WSTN (δ15NWSTN) in the total suspended particles (TSP) collected from Sapporo, northern Japan for one-year period. In general, WION was more abundant (126 ± 117 ng m-3) whereas WSON (89.7 ± 80.6 ng m-3), accounting for 14 ± 11% and 9.2 ± 7.3% of TN, respectively. WSON peaked in late autumn to winter (maximum 288 ng m-3) and WION peaked in mid spring to early summer (454 ng m-3). δ15NTN (21.9 ± 4.1‰) and δ15NWSTN (25.8 ± 8.2‰) showed peaks in summer with relatively high ratios in late autumn. Based on the seasonal variations of WSON and WION together with organic tracers, fossil fuel combustion and biomass burning are found to be two major sources of WSON whereas emissions of biological particles and secondary formation by reactions of biogenic secondary organic species (carbonyls) with NH3 are suggested as important source of WION. The seasonality of δ15NTN and δ15NWSTN, together with the comparisons to literature values, implies that chemical aging (including gas/particle partitioning) and biomass burning are the causes of the enhanced values in summer and autumn, respectively. This study demonstrates that contributions of aerosol N from fossil fuel combustion and biomass burning dominate in autumn/winter whereas emission of terrestrial biological particles and secondary formation from biogenic hydrocarbons and subsequent chemical aging in the atmosphere are important in spring/summer in Northeast Asia.

  16. Insights Into Water-Soluble Organic Aerosol Sources From Carbon-13 Ratios of Size Exclusion Chromatography Fractions

    NASA Astrophysics Data System (ADS)

    Ruehl, C. R.; Chuang, P. Y.; McCarthy, M. D.

    2008-12-01

    Many sources of organic aerosols have been identified and quantified, and much of this work has used individual (mosty water-insoluble) compounds as tracers of primary sources. However, most organic aerosol cannot be molecularly characterized, and the water-soluble organic carbon (WSOC) in many aerosols is thought to originate from gaseous precursors (i.e., it is secondary in nature). It can therefore be difficult to infer aerosol sources, particularly of background (i.e., aged) aerosols, and of the relatively high-MW component of aerosols. The stable isotope ratios (δ13C) of organic aerosols have been used to distinguish between sources, with lighter values (-30‰ to -25‰) interpreted as having originated from fossil fuel combustion and C4 biogenic emission, and heavier values (-25‰ to - 20‰) indicating a marine or C3 biogenic source. Most published measurements were of either total suspended particulates or PM2.5, however, and it is unknown to what extent these fractions differ from submicron WSOC. We report δ13C for submicron WSOC collected at a variety of sites, ranging from marine to polluted to background continental. Bulk marine organic δ13C ranged from -30.4 to - 27.6‰, slightly lighter than previously published results. This could be due to the elimination of supermicron cellular material or other biogenic primary emissions from the sample. Continental WSOC δ13C ranged from -19.1 to -29.8‰, with heavier values (-19.8 ± 1.0‰) in Oklahoma and lighter values at Great Smoky Mountain National Park in Tennessee (-25.8 ± 2.6‰) and Illinois (-24.5 ± 1.0‰). This likely results from the greater proportional of C3 plant material in the Oklahoma samples. In addition to bulk samples, we used size exclusion chromatography (SEC) to report δ13C of organic aerosols as a function of hydrodynamic diameter. Variability and magnitude of hydrodynamic diameter was greatest at low SEC pH, indicative of the acidic character of submicron WSOC. Tennessee

  17. Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

    NASA Astrophysics Data System (ADS)

    Hapsari Budisulistiorini, Sri; Baumann, Karsten; Edgerton, Eric S.; Bairai, Solomon T.; Mueller, Stephen; Shaw, Stephanie L.; Knipping, Eladio M.; Gold, Avram; Surratt, Jason D.

    2016-04-01

    A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA) and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 %) and sulfate (up to 31 %). Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), semi-volatile oxygenated OA (SV-OOA), low-volatility oxygenated OA (LV-OOA), isoprene-derived epoxydiols (IEPOX) OA (IEPOX-OA) and 91Fac (a factor dominated by a distinct ion at m/z 91 fragment ion previously observed in biogenic influenced areas). LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass). BBOA (15-33 % of OA mass) was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ˜ 27 %), it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27-41 %) of OA at both sites, particularly in spring and summer. An ion fragment at m/z 75 is well correlated with the m/z 82 ion associated with the aerosol mass spectrum of IEPOX-derived secondary organic aerosol (SOA). The

  18. Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles

    PubMed Central

    Russell, Lynn M.; Bahadur, Ranjit; Ziemann, Paul J.

    2011-01-01

    Measurements of submicron particles by Fourier transform infrared spectroscopy in 14 campaigns in North America, Asia, South America, and Europe were used to identify characteristic organic functional group compositions of fuel combustion, terrestrial vegetation, and ocean bubble bursting sources, each of which often accounts for more than a third of organic mass (OM), and some of which is secondary organic aerosol (SOA) from gas-phase precursors. The majority of the OM consists of alkane, carboxylic acid, hydroxyl, and carbonyl groups. The organic functional groups formed from combustion and vegetation emissions are similar to the secondary products identified in chamber studies. The near absence of carbonyl groups in the observed SOA associated with combustion is consistent with alkane rather than aromatic precursors, and the absence of organonitrate groups can be explained by their hydrolysis in humid ambient conditions. The remote forest observations have ratios of carboxylic acid, organic hydroxyl, and nonacid carbonyl groups similar to those observed for isoprene and monoterpene chamber studies, but in biogenic aerosols transported downwind of urban areas the formation of esters replaces the acid and hydroxyl groups and leaves only nonacid carbonyl groups. The carbonyl groups in SOA associated with vegetation emissions provides striking evidence for the mechanism of esterification as the pathway for possible oligomerization reactions in the atmosphere. Forest fires include biogenic emissions that produce SOA with organic components similar to isoprene and monoterpene chamber studies, also resulting in nonacid carbonyl groups in SOA. PMID:21317360

  19. Sources and composition of submicron organic mass in marine aerosol particles

    SciTech Connect

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak

  20. Sources and composition of submicron organic mass in marine aerosol particles

    DOE PAGESBeta

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

  1. Source and composition of size fractionated aerosols collected in the Central Valley

    NASA Astrophysics Data System (ADS)

    Allen, G.; Kelly, P. B.; Buchholz, B. A.; Clifford, A.

    2013-12-01

    The Central Valley in California has historically had high levels of atmospheric particulate matter (PM), resulting in significant adverse health effects. The three sources of atmospheric PM in the Central Valley are vehicle exhaust emissions, agricultural activity and residential wood burning. Ambient PM was collected during the winter of 2011 and 2012 in Davis, CA using a DRUM impact analyzer to determine the contributions of the various sources to the size fractionated aerosols. Laser desorption ionization time-of-flight mass spectrometry (LDI-TOF MS) and radiocarbon accelerator mass spectrometry (AMS) were performed on size fractionated atmospheric PM. The results show that as particle size decreases the amount of organic carbon increases. In the smallest size fraction (0.09 - 1.2 μm) the organic carbon encompasses approximately 70% of the LDI-TOF signal intensity. A comparison of the size fraction PM LDI-TOF spectra showed that there was a significant difference in the chemical composition with particle size. Three distinct chemical composition modes were observed in the LDI-TOF analysis: 0.09 to 0.34 μm, 0.34 to 0.56 μm and >0.56 μm. The particles <0.34 μm were found to be statistically different than those >0.5 μm. The chemical difference in the PM is driven by the large amount of secondary organic aerosol. Dicarboxylic acids, aromatic acids and nitrated aromatics were predominately found in particles <0.34 μm. The effect on human health of these compounds needs to be further explored. The difference in the chemical composition between the respirable and larger PM needs to be considered when associating health effects with PM exposure. The radiocarbon AMS analysis showed that the size fractionated total carbonaceous particulate matter was mainly biogenic in origin, having an average fraction modern (F14C) = 0.753 × 0.006. The F14C from both sample collections were similar and there wasn't a significant change in fraction modern as particle size

  2. Source contributions to 2012 summertime aerosols in the Euro-Mediterranean region

    NASA Astrophysics Data System (ADS)

    Rea, G.; Turquety, S.; Menut, L.; Briant, R.; Mailler, S.; Siour, G.

    2015-07-01

    In the Mediterranean area, aerosols may originate from anthropogenic or natural emissions (biogenic, mineral dust, fire and sea salt) before undergoing complex chemistry. In case of a huge pollution event, it is important to know whether European pollution limits are exceeded and, if so, whether the pollution is due to anthropogenic or natural sources. In this study, the relative contribution of emissions to surface PM10, surface PM2.5 and total aerosol optical depth (AOD) is quantified. For Europe and the Mediterranean regions and during the summer of 2012, the WRF and CHIMERE models are used to perform a sensitivity analysis on a 50 km resolution domain (from -10° W to 40° E and from 30° N to 55° N): one simulation with all sources (reference) and all others with one source removed. The reference simulation is compared to data from the AirBase network and two ChArMEx stations, and from the AERONET network and the MODIS satellite instrument, to quantify the ability of the model to reproduce the observations. It is shown that the correlation ranges from 0.19 to 0.57 for surface particulate matter and from 0.35 to 0.75 for AOD. For the summer of 2012, the model shows that the region is mainly influenced by aerosols due to mineral dust and anthropogenic emissions (62 and 19 %, respectively, of total surface PM10 and 17 and 52 % of total surface PM2.5). The western part of the Mediterranean is strongly influenced by mineral dust emissions (86 % for surface PM10 and 44 % for PM2.5), while anthropogenic emissions dominate in the northern Mediterranean basin (up to 75 % for PM2.5). Fire emissions are more sporadic but may represent 20 % of surface PM2.5, on average, during the period near local sources. Sea salt mainly contributes for coastal sites (up to 29 %) and biogenic emissions mainly in central Europe (up to 20 %). The same analysis was undertaken for the number of daily exceedances of the European Union limit of 50 μg m-3 for PM10 (over the stations), and

  3. Long-term trends in aerosol optical characteristics in the Po Valley, Italy

    NASA Astrophysics Data System (ADS)

    Putaud, J. P.; Cavalli, F.; Martins dos Santos, S.; Dell'Acqua, A.

    2014-09-01

    Aerosol properties have been monitored by ground-based in situ and remote sensing measurements at the station for atmospheric research located in Ispra, on the edge of the Po Valley, for almost one decade. In situ measurements are performed according to Global Atmosphere Watch recommendations, and quality is assured through the participation in regular inter-laboratory comparisons. Sun-photometer data are produced by the Aerosol Robotic Network (AERONET). Data show significant decreasing trends over the 2004-2010 period for a number of variables, including particulate matter (PM) mass concentration, aerosol scattering, backscattering and absorption coefficients, and aerosol optical thickness (AOT). In situ measurement data show no significant trends in the aerosol backscatter ratio, but they do show a significant decreasing trend of about -0.7 ± 0.3% yr-1 in the aerosol single scattering albedo (SSA) in the visible light range. Similar trends are observed in the SSA retrieved from sun-photometer measurements. Correlations appear between in situ PM mass concentration and aerosol scattering coefficient, on the one hand, and elemental carbon (EC) concentration and aerosol absorption coefficient, on the other hand. However, no increase in the EC / PM ratio was observed, which could have explained the decrease in SSA. The application of a simple approximation to calculate the direct radiative forcing by aerosols suggests a significant diminution in their cooling effect, mainly due to the decrease in AOT. Applying the methodology we present to those sites, where the necessary suite of measurements is available, would provide important information to inform future policies for air-quality enhancement and fast climate change mitigation.

  4. Radiocarbon-based source apportionment of black carbon (BC) in PM 10 aerosols from residential area of suburban Tokyo

    NASA Astrophysics Data System (ADS)

    Uchida, Masao; Kumata, Hidetoshi; Koike, Yasuyo; Tsuzuki, Mikio; Uchida, Tatsuya; Fujiwara, Kitao; Shibata, Yasuyuki

    2010-04-01

    The AMS technique was applied to analyse black carbon (BC), total organic carbon (TOC), and previously reported polycyclic aromatic hydrocarbons (PAHs) in PM 10 aerosols from a residential area, suburban Tokyo, to determine natural abundance of radiocarbon ( 14C), an ideal tracer to distinguish fossil fuel ( 14C-free) from modern biomass combustion sources of pyrolytic products. The 14C concentrations in BC, isolated using the CTO-375 method, were 42% and 30% pMC (in terms of percent Modern Carbon: pMC) in summer and winter, respectively. The 14C concentrations in BC were also compared with those of compound-class specific 14C content of PAHs previously reported for the same samples: they were 45% and 33% pMC in summer and winter, respectively. The 14C signals of BC were identical to those of high molecular weight (MW ⩾ 226, 5-6 rings) PAHs. The resemblance between 14C signals of BC and PAHs can be referred as a 'certificate' for the validity of the BC isolation method employed in this study. Also, it suggests that 14C-BC approach can be a surrogate for PAHs specific 14C analyses to monitor seasonal source variation of combustion-derived pyrolytic products. On the other hand, 14C contents of total organic carbon in 2004 were 61% and 42% pMC in summer and winter, respectively. This is likely attributed to higher contribution of plant activity in summer.

  5. IMPACTS OF SOURCE TERM HETEROGENEITIES ON WATER PATHWAY DOSE.

    SciTech Connect

    SULLIVAN, T.; GUSKOV, A.; POSKAS, P.; RUPERTI, N.; HANUSIK, V.; ET AL.

    2004-09-15

    and for which a solution has to be found in term of long-term disposal. Together with their casing and packaging, they are one form of heterogeneous waste; many other forms of waste with heterogeneous properties exist. They may arise in very small quantities and with very specific characteristics in the case of small producers, or in larger streams with standard characteristics in others. This wide variety of waste induces three main different levels of waste heterogeneity: (1) hot spot (e.g. disused sealed sources); (2) large item inside a package (e.g. metal components); and (3) very large items to be disposed of directly in the disposal unit (e.g. irradiated pipes, vessels). Safety assessments generally assume a certain level of waste homogeneity in most of the existing or proposed disposal facilities. There is a need to evaluate the appropriateness of such an assumption and the influence on the results of safety assessment. This need is especially acute in the case of sealed sources. There are many cases where are storage conditions are poor, or there is improper management leading to a radiological accident, some with significant or detrimental impacts. Disposal in a near surface disposal facility has been used in the past for some disused sealed sources. This option is currently in use for others sealed sources, or is being studied for the rest of them. The regulatory framework differs greatly between countries. In some countries, large quantities of disused sealed sources have been disposed of without any restriction, in others their disposal is forbidden by law. In any case, evaluation of the acceptability of disposal of disused sealed sources in near surface disposal facility is of utmost importance.

  6. Tracing of industrial aerosol sources in an urban environment using Pb, Sr, and Nd isotopes.

    PubMed

    Geagea, Majdi Lahd; Stille, Peter; Gauthier-Lafaye, François; Millet, Maurice

    2008-02-01

    A comprehensive Pb-Sr-Nd isotope tracer study of atmospheric trace metal pollution has been performed in the urban environment of Strasbourg-Kehl. Filter dust of the principal pollutant sources (waste incinerators, thermal power plant and steel plant) and soot of car and ship exhausts have been analyzed. In addition tree barks (as biomonitors) and PM10 have been analyzed to trace and determine the distribution of the pollution in the environment. The industrial sources have highly variable epsilonNd values (-9.7 and -12.5 for incinerators and -17.5 for steel plant). Much higher epsilonNd values have been found for soot of car exhausts (-6 and -6.9). These high values make the Nd isotope system a powerful tool for the discrimination of traffic emissions but especially for the identification of diesel derived particles in the urban environment. The 206Pb/207Pb isotope ratios of gasoline are low (1.089) compared to diesel soot (1.159). The 26Pb/207Pb ratios of 1.151-1.152 for the steel plant and 1.152 for the solid waste incinerator are close to the Pb isotope ratio of diesel. The 87Sr/ 8Sr isotope ratios of the principal industrial sources vary significantly: 0.7095 for the domestic solid waste incinerator, 0.709 for the steel plant, and 0.7087 for car exhaust soot. PM10 aerosols collected in the urban center of Strasbourg show the influence of the pollutant sources at 3-7 km distance from the center. Most of the aerosols Pb isotopic compositions suggest Pb admixtures from at least three sources: a natural background and in function of the wind direction the domestic waste incinerator (S-wind) or the steel plant and the chemical waste incinerator (NE-wind). The traffic contribution can only be estimated with help of Nd isotopes. Therefore the clear identification of different pollutant sources in the urban environment is only possible by combining the three different isotope systems and is based on the fact that significant differences exist between the Pb, Sr, and

  7. Source apportionment of aerosol particles near a steel plant by electron microscopy.

    PubMed

    Ebert, Martin; Müller-Ebert, Dörthe; Benker, Nathalie; Weinbruch, Stephan

    2012-12-01

    The size, morphology and chemical composition of 37,715 individual particles collected over 22 sampling days in the vicinity of a large integrated steel production were studied by scanning and transmission electron microscopy. Based on the morphology, chemistry and beam stability the particles were classified into the following fourteen groups: silicates, sea salt, calcium sulfates, calcium carbonates, carbonate-silicate mixtures, sulfate-silicate mixtures, iron oxides, iron mixtures, metal oxide-metals, complex secondary particles, soot, Cl-rich particles, P-rich particles, and other particles. The majority of iron oxide (≈85%) and metal oxide-metal (≈70%) particles as well as ≈20% of the silicate particles are fly ashes from high temperature processes. The emissions from the steel work are dominated by iron oxide particles. For source apportionment, seven source categories and two sectors of local wind direction (industrial and urban background) were distinguished. In both sectors PM₁₀ consists of four major source categories: 35% secondary, 20% industrial, 17% soil and 16% soot in the urban background sector compared to 45% industrial, 20% secondary, 13% soil, and 9% soot in the industrial sector. As the secondary and the soot components are higher in the urban background sector than in the industrial sector, it is concluded that both components predominantly originate from urban background sources (traffic, coal burning, and domestic heating). Abatement measures should not only focus on the steel work but should also include the urban background aerosol. PMID:23149950

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

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

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

  9. Bayesian Estimation of Prior Variance in Source Term Determination

    NASA Astrophysics Data System (ADS)

    Smidl, Vaclav; Hofman, Radek

    2015-04-01

    The problem of determination of source term of an atmospheric release is studied. We assume that the observations y are obtained as linear combination of the source term, x, and source-receptor sensitivities, which can be written in matrix notation as y = Mx with source receptor sensitivity matrix M. Direct estimation of the source term vector x is not possible since the system is often ill-conditioned. The solution is thus found by minimization of a cost function with regularization terms. A typical cost function is: C (x) = (y - M x)TR-1(y- M x) + αxTDT Dx, (1) where the first term minimizes the error of the measurements with covariance matrix R, and the second term is the regularization with weight α. Various types of regularization arise for different choices of matrix D. For example, Tikhonov regularization arises for D in the form of identity matrix, and smoothing regularization for D in the form of a tri-diagonal matrix (Laplacian operator). Typically, the form of matrix D is assumed to be known, and the weight α is optimized manually by a trial and error procedure. In this contribution, we use the probabilistic formulation of the problem, where term (αDTD)-1 is interpreted as a covariance matrix of the prior distribution of x. Following the Bayesian approach, we relax the assumption of known α and D and assume that these are unknown and estimated from the data. The general problem is not analytically tractable and approximate estimation techniques has to be used. We present Variational Bayesian solution of two special cases of the prior covariance matrix. First, the structure of D is assumed to be known and only the weight α is estimated. Application of the Variational Bayes method to this case yields an iterative estimation algorithm. In the first step, the usual optimization problem is solved for an estimate of α. In the next step, the value of α is re-estimated and the procedure returns to the first step. Positivity of the solution is guaranteed

  10. Applications of optical spectroscopy and stable isotope analyses to organic aerosol source discrimination in an urban area

    NASA Astrophysics Data System (ADS)

    Mladenov, N.; Alados-Arboledas, L.; Olmo, F. J.; Lyamani, H.; Delgado, A.; Molina, A.; Reche, I.

    2011-02-01

    Understanding the chemical character of organic aerosols is extremely important for evaluating their role in climate forcing and human respiratory health. Aerosol columnar properties retrieved by sun photometry represent a large dataset of information about the physical and light absorbing and scattering properties of the total aerosol, but lack more detailed chemical information about the organic fraction of atmospheric particulate matter. To obtain additional information about relationships between organic aerosol sources and columnar properties, we simultaneously examined stable isotope properties of PM 10 aerosols from urban (Granada, Spain) and remote (Sierra Nevada, Spain) sites and diesel exhaust, spectroscopic properties of water soluble organic carbon (WSOC) of PM 10 aerosols, and sun photometry measurements. We demonstrated that C and N stable isotopes and parameters from UV-vis and fluorescence spectroscopy are able to discriminate between aerosols receiving substantial fossil fuel pollution and those influenced by Saharan dust in an urban area. More depleted δ 13C was associated with low asymmetry parameter, g λ, and high values of the spectral slope ratio, S R, were associated with high effective radius, typical of pollution situations. The humification index (HIX), used predominantly to evaluate the degree of organic matter humification, was significantly related to g λ and the radius of fine mode particles, r f, and may reflect aging of the Saharan dust-influenced aerosols. Parallel factor analysis (PARAFAC) modeling identified a fluorescent component (C3) with a spectrum similar to that of naphthalene, which was significantly related to g λ and r f. The diesel exhaust sample represented a pollution end-member, with the lightest δ 13C value (-26.4‰), lowest S R (0.95), lowest HIX (2.77) and highest %C3 (20%) of all samples.

  11. Evaluation of aerosol sources at European high altitude background sites with trajectory statistical methods

    NASA Astrophysics Data System (ADS)

    Salvador, P.; Artíñano, B.; Pio, C. A.; Afonso, J.; Puxbaum, H.; Legrand, M.; Hammer, S.; Kaiser, A.

    2009-04-01

    During the last years, the analysis of a great number of back-trajectories from receptor sites has turned out to be a valuable tool to identify sources and sinks areas of atmospheric particulate matter (PM) or to reconstruct their average spatial distribution. A number of works have applied different trajectory statistical methods (TSM), which allow working simultaneously with back-trajectories computed from one or several receptor points and PM concentration values registered there. In spite of these methods have many limitations, they are simple and effective methods to detect the relevant source regions and the air flow regimes which are connected with regional and large-scale air pollution transport. In this study 5-day backward air trajectories arriving over 3 monitoring sites, were utilised and analysed simultaneously with the PM levels and chemical composition values registered there. These sites are located in the centre of Europe and can be classified into natural continental background (Schauinsland-SIL in Germany (1205 m asl), Puy de Dôme-PDD in France (1450 m asl) and Sonnblick-SBO in Austria (3106 m asl)). In the framework of the CARBOSOL European project, weekly aerosol samples were collected with High Volume Samplers (DIGITEL DH77) and PM10 (SIL and PDD) or PM2.5 (SBO) inlets, on quartz fibre filters. Filter samples were treated and analyzed for determining the levels of major organic fractions (OC, EC) and inorganic ions. Additionally, analyses for specific organic compounds were also carried out whenever was possible (Pio et al., 2007). For each day of the sampling period, four trajectories ending at 00:00, 06:00, 12:00 and 18:00 h UTC have been computed by the Norwegian Institute for Air Research NILU (SIL and PDD) and the Central Institute for Meteorology and Geophysics of Austria (SBO) using the FLEXTRA model (Stohl et al., 1995). In all, more than 8000 complete trajectories were available for analysis, each with 40 endpoints. Firstly air mass

  12. Photochemistry at interfaces: a source of radicals impacting on aerosol formation and properties

    NASA Astrophysics Data System (ADS)

    George, C.; D'anna, B.; Monge, M.; Dupart, Y.

    2011-12-01

    Recent findings confirm the presence of light absorbing organic material (HULIS, biomass burning particles, PAHs) in atmospheric aerosols... but also at the air/ocean interface. The presence of such light absorbing material allows photosensitised processes to occur. The latter may be sources of radicals in the troposphere that may alter its oxidation capacity (as for instance through the formation of HONO) or change the pathways leading to particle formation and ageing. We will exemplify such processes by presenting new data on the generation of radicals from dust particles or at the air/sea interface leading to particle formation in presence of SO2. These are recent findings that are questioning our current understanding of tropospheric photochemistry.

  13. Aerosol optical properties at a coastal site in Hong Kong, South China: temporal features, size dependencies and source analysis

    NASA Astrophysics Data System (ADS)

    Wang, Jiaping; Ding, Aijun; Virkkula, Aki; Lee, Shuncheng; Shen, Yicheng; Chi, Xuguang; Xu, Zheng

    2016-04-01

    Hong Kong is a typical coastal city adjacent to the Pearl River Delta (PRD) region in southern China, which is one of the regions suffering from severe air pollution. Atmospheric aerosols can affect the earth's radiative balance by scattering and absorbing incoming solar radiation. Black Carbon (BC) aerosol is a particularly emphasized component due to its strong light absorption. Aerosol transported from different source areas consists of distinct size distributions, leading to different optical properties. As the byproducts of the incomplete oxidation, BC and CO both have relatively long life time, their relationship is a good indicator for distinguishing different pollutant sources. In this study, temporal variations of aerosol optical properties and concentrations of BC and CO at a coastal background station in Hong Kong were investigated. Transport characteristics and origins of aerosol were elucidated by analyzing backward Lagrangian particle dispersion modeling (LPDM) results, together with related parameters including the relationships between optical properties and particle size, BC-CO correlations, ship location data and meteorological variables. From February 2012 to September 2013 and March 2014 to February 2015, continuous in-situ measurements of light scattering and absorption coefficients, particle size distribution and concentrations of BC and CO were conducted at Hok Tsui (HT), a coastal background station on the southeast tip of Hong Kong Island (22.22°N, 114.25°E, 60 m above the sea level) with few local anthropogenic activities. Affected by the Asian monsoon, this region is dominated by continental outflow in winter and by marine inflow from the South China Sea in summer, which is an ideal station for identifying the transport characteristics of aerosol and their effects on optical properties from different anthropogenic emission sources. 7-day backward Lagrangian particle dispersion modeling was performed for source identification. Three

  14. Recent Short Term Global Aerosol Trends over Land and Ocean Dominated by Biomass Burning

    NASA Technical Reports Server (NTRS)

    Remer, Lorraine A.; Koren, Ilan; Kleidman, RIchard G.; Levy, Robert C.; Martins, J. Vanderlei; Kim, Kyu-Myong; Tanre, Didier; Mattoo, Shana; Yu, Hongbin

    2007-01-01

    NASA's MODIS instrument on board the Terra satellite is one of the premier tools to assess aerosol over land and ocean because of its high quality calibration and consistency. We analyze Terra-MODIS's seven year record of aerosol optical depth (AOD) observations to determine whether global aerosol has increased or decreased during this period. This record shows that AOD has decreased over land and increased over ocean. Only the ocean trend is statistically significant and corresponds to an increase in AOD of 0.009, or a 15% increase from background conditions. The strongest increasing trends occur over regions and seasons noted for strong biomass burning. This suggests that biomass burning aerosol dominates the increasing trend over oceans and mitigates the otherwise mostly negative trend over the continents.

  15. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA)-power plant studies: assessment of cellular responses

    PubMed Central

    Godleski, John J.; Diaz, Edgar A.; Lemos, Miriam; Long, Mark; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Coull, Brent

    2013-01-01

    The Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA) project assessed primary and secondary particulate by simulating the chemical reactions that a plume from a source might undergo during atmospheric transport and added other atmospheric constituents that might interact with it. Three coal-fired power plants with different coal and different emission controls were used. Male Sprague-Dawley rats were exposed for 6 h to either filtered air or aged aerosol from the power plant. Four exposure scenarios were studied: primary particles (P); primary + secondary (oxidized) particles (PO); primary + secondary (oxidized) particles + SOA (POS); and primary + secondary (oxidized) particles neutralized + SOA (PONS). Exposure concentrations varied by scenario to a maximum concentration of 257.1 ± 10.0 µg/m3. Twenty-four hours after exposure, pulmonary cellular responses were assessed by bronchoalveolar lavage (BAL), complete blood count (CBC), and histopathology. Exposure to the PONS and POS scenarios produced significant increases in BAL total cells and macrophage numbers at two plants. The PONS and P scenarios were associated with significant increases in BAL neutrophils and the presence of occasional neutrophils and increased macrophages in the airways and alveoli of exposed animals. Univariate analyses and random forest analyses showed that increases in total cell count and macrophage cell count were significantly associated with neutralized sulfate and several correlated measurements. Increases in neutrophils in BAL were associated with zinc. There were no significant differences in CBC parameters or blood vessel wall thickness by histopathology. The association between neutrophils increases and zinc raises the possibility that metals play a role in this response. PMID:21466245

  16. ATMOSPHERIC AEROSOL SOURCE-RECEPTOR RELATIONSHIPS: THE ROLE OF COAL-FIRED POWER PLANTS

    SciTech Connect

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2004-04-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of September 2003 through February 2004. Significant progress was made this project period on the analysis of ambient data, source apportionment, and deterministic modeling activities. Results highlighted in this report include chemical fractionation of the organic fraction to quantify the ratio of organic mass to organic carbon (OM/OC). The average OM/OC ratio for the 31 samples analyzed so far is 1.89, ranging between 1.62 and 2.53, which is consistent with expectations for an atmospherically processed regional aerosol. Analysis of the single particle data reveals that a on a particles in Pittsburgh consist of complex mixture of primary and secondary components. Approximately 79% of all particles measured with the instrument containing some form of carbon, with Carbonaceous Ammonium Nitrate (54.43%) being the dominant particle class. PMCAMx predictions were compared with data from more than 50 sites of the STN network located throughout the Eastern United States for the July 2001 period. OC and sulfate concentrations predicted by PMCAMx are within {+-}30% of the observed concentration at most of these sites. Spherical Aluminum Silicate particle concentrations (SAS) were used to estimate the contribution of primary coal emissions to fine particle levels at the central monitoring site. Primary emissions from coal combustion contribute on average 0.44 {+-} 0.3 {micro}g/m{sup 3} to PM{sub 2.5} at the site or 1.4 {+-} 1.3% of the total PM{sub 2.5} mass. Chemical mass balance analysis was performed to apportion the primary organic aerosol. About 70% of the primary OC emissions are from vehicular sources, with the gasoline contribution being on average three times greater than the diesel emissions in the summer.

  17. Validating and Improving Long-Term Aerosol Data Records from SeaWiFS

    NASA Technical Reports Server (NTRS)

    Bettenhausen, Corey; Hsu, N. Christina; Sayer, Andrew; Huang, Jinhfeng; Gautam, Ritesh

    2011-01-01

    Natural and anthropogenic aerosols influence the radiative balance of the Earth through direct and indirect interactions with incoming solar radiation. However, the quantification of these interactions and their ultimate effect on the Earth's climate still have large uncertainties. This is partly due to the limitations of current satellite data records which include short satellite lifetimes, retrieval algorithm uncertainty, or insufficient calibration accuracy. We have taken the first steps in overcoming this hurdle with the production and public release of an aerosol data record using the radiances from the Sea-viewing Wide Field-of-View Sensor (Sea WiFS). Sea WiFS was launched in late 1997 and provided exceptionally well-calibrated top-of-atmosphere radiance data until December 2010, more than 13 years. We have partnered this data with an expanded Deep Blue aerosol retrieval algorithm. In accordance with Deep Blue's original focus, the latest algorithm retrieves aerosol properties not only over bright desert surfaces, but also over oceans and vegetated surfaces. With this combination of a long time series and global algorithm, we can finally identify the changing patterns of regional aerosol loading and provide insight into longterm variability and trends of aerosols on regional and global scales. In this work, we provide an introduction to Sea WiFS, the current algorithms, and our aerosol data records. We have validated the data over land and ocean with ground measurements from the Aerosol Robotic Network (AERONET) and compared them with other satellites such as MODIS and MISR. Looking ahead to the next data release, we will also provide details on the implemented and planned algorithm improvements, and subsequent validation results.

  18. Primary sources and secondary formation of organic aerosols in Beijing, China.

    PubMed

    Guo, Song; Hu, Min; Guo, Qingfeng; Zhang, Xin; Zheng, Mei; Zheng, Jun; Chang, Chih Chung; Schauer, James J; Zhang, Renyi

    2012-09-18

    Ambient aerosol samples were collected at an urban site and an upwind rural site of Beijing during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. Contributions of primary particles and secondary organic aerosols (SOA) were estimated by chemical mass balance (CMB) modeling and tracer-yield method. The apportioned primary and secondary sources explain 73.8% ± 9.7% and 79.6% ± 10.1% of the measured OC at the urban and rural sites, respectively. Secondary organic carbon (SOC) contributes to 32.5 ± 15.9% of the organic carbon (OC) at the urban site, with 17.4 ± 7.6% from toluene, 9.7 ± 5.4% from isoprene, 5.1 ± 2.0% from α-pinene, and 2.3 ± 1.7% from β-caryophyllene. At the rural site, the secondary sources are responsible for 38.4 ± 14.4% of the OC, with the contributions of 17.3 ± 6.9%, 13.9 ± 9.1%, 5.6 ± 1.9%, and 1.7 ± 1.0% from toluene, isoprene, α-pinene, and β-caryophyllene, respectively. Compared with other regions in the world, SOA in Beijing is less aged, but the concentrations are much higher; between the sites, SOA is more aged and affected by regional transport at the urban site. The high SOA loading in Beijing is probably attributed to the high regional SOC background (~2 μg m(-3)). The toluene SOC concentration is high and comparable at the two sites, implying that some anthropogenic components, at least toluene SOA, are widespread in Beijing and represents a major factor in affecting the regional air quality. The aerosol gaseous precursor concentrations and temperature correlate well with SOA, both affecting SOA formation. The significant SOA enhancement with increasing water uptake and acidification indicates that the aqueous-phase reactions are largely responsible SOA formation in Beijing. PMID:22486583

  19. Sources and composition of submicron organic mass in marine aerosol particles

    NASA Astrophysics Data System (ADS)

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-01

    The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of

  20. Spectral aerosol optical depths over Bay of Bengal and Chennai: II—sources, anthropogenic influence and model estimates

    NASA Astrophysics Data System (ADS)

    Ramachandran, S.; Jayaraman, A.

    A cruise experiment was conducted in February-March 2001 to study the aerosol optical characteristics over Bay of Bengal, identify the source regions of aerosols and to estimate the anthropogenic contribution to the measured aerosol optical depths. The aerosol optical depths (AODs) exhibit significant spatial differences. The observed variations are explained by 7-days back trajectory analyses performed at different heights. The higher AODs obtained on 21 February are found influenced by the air mass at different heights originating either from Bangladesh or mainland India, indicating the anthropogenic influence. The anthropogenic influence on AOD are estimated by comparing the AODs obtained over Bay of Bengal (i) with that measured over a clean oceanic region taking into account the wind speed dependence on sea-salt aerosols and (ii) using maritime clean aerosol. From the two methods the estimated mean contribution by the anthropogenic sources to the AODs measured over Bay of Bengal are found to be in the range of 74-92% at 0.5 μm. Over Chennai, an urban station located on the eastern coastline of India, the anthropogenic contribution is estimated by comparing the measured AOD values with that of clean continental aerosol model and is found to be about 89%. This percentage contribution is higher than the contributions measured over Kaashidhoo and the northern Indian Ocean during INDOEX. INDOEX expeditions were conducted over the Arabian Sea and Indian Ocean on the western side of the Indian subcontinent, while the Bay of Bengal experiment was conducted on the eastern side. The differences in percentage contributions could possibly be due to the differences in anthropogenic activities, changes in the meteorological conditions, wind patterns, production and subsequently the transport of aerosols. The measured AOD spectra are reconstructed using OPAC to find out the possible chemical species which make up the aerosols over Bay of Bengal and Chennai. The AODs are

  1. Phonatory sound sources in terms of Lagrangian Coherent Structures

    NASA Astrophysics Data System (ADS)

    McPhail, Michael; Krane, Michael

    2015-11-01

    Lagrangian Coherent Structures (LCS) are used to identify sound sources in phonation. Currently, it is difficult to causally relate changes in airflow topology from voice disorders to changes in voiced sound production. LCS reveals a flow's topology by decomposing the flow into regions of distinct dynamics. The aeroacoustic sources can be written in terms of the motion of these regions in terms of the motion of the boundaries of the distinct regions. Breaking down the flow into constituent parts shows how each distinct region contributes to sound production. This approach provides a framework to connect changes in anatomy from a voice disorder to measurable changes in the resulting sound. This approach is presented for simulations of some canonical cases of vortex sound generation, and a two-dimensional simulation of phonation. Acknowledge NIH grant 2R01 2R01DC005642.

  2. A nuclear source term analysis for spacecraft power systems

    SciTech Connect

    McCulloch, W.H.

    1998-12-01

    All US space missions involving on board nuclear material must be approved by the Office of the President. To be approved the mission and the hardware systems must undergo evaluations of the associated nuclear health and safety risk. One part of these evaluations is the characterization of the source terms, i.e., the estimate of the amount, physical form, and location of nuclear material, which might be released into the environment in the event of credible accidents. This paper presents a brief overview of the source term analysis by the Interagency Nuclear Safety Review Panel for the NASA Cassini Space Mission launched in October 1997. Included is a description of the Energy Interaction Model, an innovative approach to the analysis of potential releases from high velocity impacts resulting from launch aborts and reentries.

  3. Source Attribution of Light-absorbing Aerosols in Arctic Snow (Invited)

    NASA Astrophysics Data System (ADS)

    Hegg, D.; Warren, S. G.; Grenfell, T. C.; Doherty, S. J.; Larson, T. V.; Clarke, A. D.

    2010-12-01

    Light-absorbing aerosols (LAA) deposited on the arctic snow pack, in particular black carbon (BC), contribute appreciably to the arctic radiation budget and their reduction has been suggested as a means to attenuate warming in the arctic. Effective prediction and mitigation of Arctic snow LAA requires that the sources of the LAA be elucidated. To this end, receptor modeling in the form of Positive Matrix Factorization (PMF) has been exercised on a data set of chemical concentrations in snow of various species (including inorganic and organic acids, carbohydrates and selected other organics as well as LAA) derived from an extensive set of snow samples from locations in Russia (including Siberia), Canada, Greenland, the Arctic Ocean and Svalbard. The data were obtained in three distinct periods: spring of 2007, spring of 2008, and spring of 2009. Data from each period were analyzed separately (note that the Svalbard data were analyzed only recently and were not included in the published 2007 analysis). Aerosol light absorption was determined spectrophotometrically at multiple wavelengths on filters through which melted snow was filtered. Based on the Angstrom exponent of the light absorption, partitioning of the absorption between BC and other LAA species was estimated. Statistics of the LAA concentrations for the Arctic as a whole and the geographic distribution of BC and other LAA species are presented. PMF analysis of the filtrate and filters from the 2007 data set from western Siberia, the Canadian lower arctic and Greenland revealed four factors or sources: two distinct biomass burning sources, a pollution source and a marine source. The first three of these were responsible for essentially all of the black carbon, with the two biomass sources together accounting for > 90% of the black carbon. Geographically, the biomass sources were dominant for all regions except the Arctic Ocean near the North Pole. For the 2008 and 2009 data sets, from eastern Siberia and

  4. Primary sources of PM2.5 organic aerosol in an industrial Mediterranean city, Marseille

    NASA Astrophysics Data System (ADS)

    El Haddad, I.; Marchand, N.; Wortham, H.; Piot, C.; Besombes, J.-L.; Cozic, J.; Chauvel, C.; Armengaud, A.; Robin, D.; Jaffrezo, J.-L.

    2010-11-01

    Marseille, the most important port of the Mediterranean Sea, represents a challenging case study for source apportionment exercises, combining an active photochemistry and multiple emission sources, including fugitive emissions from industrial sources and shipping. This paper presents a Chemical Mass Balance (CMB) approach based on organic markers and metals to apportion the primary sources of organic aerosol in Marseille, with a special focus on industrial emissions. Overall, the CMB model accounts for the major primary anthropogenic sources including motor vehicles, biomass burning, and the aggregate emissions from three industrial processes (HFO combustion/shipping, coke production and steel manufacturing) as well as some primary biogenic emissions. This source apportionment exercise is well corroborated by 14C measurements. Primary OC estimated by the CMB accounts on average for 22% and is dominated by the vehicular emissions that contribute on average for 17% of OC mass concentration (17% of PM2.5). Even though, industrial emissions contribute for only 2.3% of the total OC (7% of PM2.5), they are associated with ultrafine particles (Dp<80 nm) and high concentrations of Polycyclic Aromatic Hydrocarbons (PAH) and heavy metals such as Pb, Ni and V. On one hand, given that industrial emissions governed key primary markers, their omission would lead to substantial uncertainties in the CMB analysis performed in areas heavily impacted by such sources, hindering accurate estimation of non-industrial primary sources and secondary sources. This result implies that CMB modelling should not be a straightforward exercise and one have to carefully investigate the marker behaviours and trends beforehand, especially in complex environments such as Marseille. On the other hand, being associated with bursts of submicron particles and carcinogenic and mutagenic components such as PAH, these emissions are most likely related with acute health outcomes and should be regulated

  5. Primary sources of PM2.5 organic aerosol in an industrial Mediterranean city, Marseille

    NASA Astrophysics Data System (ADS)

    El Haddad, I.; Marchand, N.; Wortham, H.; Piot, C.; Besombes, J.-L.; Cozic, J.; Chauvel, C.; Armengaud, A.; Robin, D.; Jaffrezo, J.-L.

    2011-03-01

    Marseille, the most important port of the Mediterranean Sea, represents a challenging case study for source apportionment exercises, combining an active photochemistry and multiple emission sources, including fugitive emissions from industrial sources and shipping. This paper presents a Chemical Mass Balance (CMB) approach based on organic markers and metals to apportion the primary sources of organic aerosol in Marseille, with a special focus on industrial emissions. Overall, the CMB model accounts for the major primary anthropogenic sources including motor vehicles, biomass burning and the aggregate emissions from three industrial processes (heavy fuel oil combustion/shipping, coke production and steel manufacturing) as well as some primary biogenic emissions. This source apportionment exercise is well corroborated by 14C measurements. Primary OC estimated by the CMB accounts on average for 22% of total OC and is dominated by the vehicular emissions that contribute on average for 17% of OC mass concentration (vehicular PM contributes for 17% of PM2.5). Even though industrial emissions contribute only 2.3% of the total OC (7% of PM2.5), they are associated with ultrafine particles (Dp<80 nm) and high concentrations of Polycyclic Aromatic Hydrocarbons (PAH) and heavy metals such as Pb, Ni and V. On one hand, given that industrial emissions governed key primary markers, their omission would lead to substantial uncertainties in the CMB analysis performed in areas heavily impacted by such sources, hindering accurate estimation of non-industrial primary sources and secondary sources. On the other hand, being associated with bursts of submicron particles and carcinogenic and mutagenic components such as PAH, these emissions are most likely related with acute ill-health outcomes and should be regulated despite their small contributions to OC. Another important result is the fact that 78% of OC mass cannot be attributed to the major primary sources and, thus, remains un

  6. Local and distant source contributions to secondary organic aerosol in the Beijing urban area in summer

    NASA Astrophysics Data System (ADS)

    Lin, Jian; An, Junling; Qu, Yu; Chen, Yong; Li, Ying; Tang, Yujia; Wang, Feng; Xiang, Weiling

    2016-01-01

    Quantification of local and distant source contributions to particulate matter is a key issue to improving air quality in large urban areas, but few studies have focused on secondary organic aerosol (SOA) source contributions in a large area, especially in China. In this study, we extended the Comprehensive Air Quality Model with Extensions (CAMX) version 5.4, replacing the two-product approach by the volatility basis-set (VBS) approach, with updated SOA yields based on smog chamber studies. The modules related to the computationally efficient particulate source apportionment technology (PSAT) used in CAMX v5.4 were extended based on the volatility basis set (VBS) approach. The updated version of the CAMX model was then used to calculate the local and distant source contributions to SOA in Beijing for the first time. The results indicated that the VBS approach substantially improved hourly, daily, and monthly SOA simulations, compared with the two-product approach and the observations. In August 2007, the local source contributions to anthropogenic and biogenic SOA in Beijing were 23.8% and 16.6%, respectively; distant sources dominated for both anthropogenic and biogenic SOA in Beijing: Northern Hebei, Middle Hebei, Northeast China, Inner Mongolia, Shandong, and Tianjin (including Xianghe) contributed 5.1%-18.2% to anthropogenic SOA in Beijing; whereas, Inner Mongolia, Northern Hebei, and Northeast China contributed 12.2%, 18.6%, and 10.1%, respectively, to biogenic SOA in Beijing. Additionally, other areas outside China respectively contributed 5.3% and 10.8% to anthropogenic and biogenic SOA in Beijing: this could be related to strong summer monsoon.

  7. Fossil and Nonfossil Sources of Organic and Elemental Carbon Aerosols in the Outflow from Northeast China.

    PubMed

    Zhang, Yan-Lin; Kawamura, Kimitaka; Agrios, Konstantinos; Lee, Meehye; Salazar, Gary; Szidat, Sönke

    2016-06-21

    Source quantification of carbonaceous aerosols in the Chinese outflow regions still remains uncertain despite their high mass concentrations. Here, we unambiguously quantified fossil and nonfossil contributions to elemental carbon (EC) and organic carbon (OC) of total suspended particles (TSP) from a regional receptor site in the outflow of Northeast China using radiocarbon measurement. OC and EC concentrations were lower in summer, representing mainly marine air, than in other seasons, when air masses mostly traveled over continental regions in Mongolia and northeast China. The annual-mean contribution from fossil-fuel combustion to EC was 76 ± 11% (0.1-1.3 μg m(-3)). The remaining 24 ± 11% (0.03-0.42 μg m(-3)) was attributed to biomass burning, with slightly higher contribution in the cold period (∼31%) compared to the warm period (∼21%) because of enhanced emissions from regional biomass combustion sources in China. OC was generally dominated by nonfossil sources, with an annual average of 66 ± 11% (0.5-2.8 μg m(-3)), approximately half of which was apportioned to primary biomass-burning sources (34 ± 6%). In winter, OC almost equally originated from primary OC (POC) emissions and secondary OC (SOC) formation from fossil fuel and biomass-burning sources. In contrast, summertime OC was dominated by primary biogenic emissions as well as secondary production from biogenic and biomass-burning sources, but fossil-derived SOC was the smallest contributor. Distinction of POC and SOC was performed using primary POC-to-EC emission ratios separated for fossil and nonfossil emissions. PMID:27203471

  8. Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China

    NASA Astrophysics Data System (ADS)

    Kirillova, E. N.; Andersson, A.; Han, J.; Lee, M.; Gustafsson, Ö.

    2014-02-01

    High loadings of anthropogenic carbonaceous aerosols in Chinese air influence the air quality for over one billion people and impact the regional climate. A large fraction (17-80%) of this aerosol carbon is water-soluble, promoting cloud formation and thus climate cooling. Recent findings, however, suggest that water-soluble carbonaceous aerosols also absorb sunlight, bringing additional direct and indirect climate warming effects, yet the extent and nature of light absorption by this water-soluble "brown carbon" and its relation to sources is poorly understood. Here, we combine source estimates constrained by dual carbon isotopes with light-absorption measurements of water-soluble organic carbon (WSOC) for a March 2011 campaign at the Korea Climate Observatory at Gosan (KCOG), a receptor station in SE Yellow Sea for the outflow from northern China. The mass absorption cross section at 365 nm (MAC365) of WSOC for air masses from N. China were in general higher (0.8-1.1 m2 g-1), than from other source regions (0.3-0.8 m2 g-1). However, this effect corresponds to only 2-10% of the radiative forcing caused by light absorption by elemental carbon. Radiocarbon constraints show that the WSOC in Chinese outflow had significantly higher fraction fossil sources (30-50%) compared to previous findings in S. Asia, N. America and Europe. Stable carbon (δ13C) measurements were consistent with aging during long-range air mass transport for this large fraction of carbonaceous aerosols.

  9. Actinide Source Term Program, position paper. Revision 1

    SciTech Connect

    Novak, C.F.; Papenguth, H.W.; Crafts, C.C.; Dhooge, N.J.

    1994-11-15

    The Actinide Source Term represents the quantity of actinides that could be mobilized within WIPP brines and could migrate with the brines away from the disposal room vicinity. This document presents the various proposed methods for estimating this source term, with a particular focus on defining these methods and evaluating the defensibility of the models for mobile actinide concentrations. The conclusions reached in this document are: the 92 PA {open_quotes}expert panel{close_quotes} model for mobile actinide concentrations is not defensible; and, although it is extremely conservative, the {open_quotes}inventory limits{close_quotes} model is the only existing defensible model for the actinide source term. The model effort in progress, {open_quotes}chemical modeling of mobile actinide concentrations{close_quotes}, supported by a laboratory effort that is also in progress, is designed to provide a reasonable description of the system and be scientifically realistic and supplant the {open_quotes}Inventory limits{close_quotes} model.

  10. Source quantification of size and season resolved aerosols in a semi-urban area of Indo-Gangetic plain, India

    NASA Astrophysics Data System (ADS)

    Hooda, R. K.; Hyvärinen, A.; Gilardoni, S.; Sharma, V.; Vestenius, M.; Kerminen, V.; Vignati, E.; Kulmala, M. T.; Lihavainen, H.

    2012-12-01

    This study describes a one year measurements of size-segregated aerosols at a semi-urban site in Indo-Gangetic plain (IGP), India, South Asia with focus on source quantification applied to organic and inorganic chemical species data using Positive Matrix Factorization (PMF), trajectory analysis and conditional probability function (CPF) methods. The campaign was planned in the framework of the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. In light of the above, Finnish Meteorological Institute (FMI), The Energy and Resources Institute (TERI) and Joint Research Centre (JRC) conducted aerosol mass measurements in Gual Pahari, India from April 2008 to March 2009. The average mass concentrations of fine (PM2.5) and coarse (PM2.5-10) aerosols are higher during the postmonsoon (October-November) and winter (December- February) compared to that during the summer season (March-May). Fine and coarse fraction concentrations observed are higher during the post-monsoon & winter months due to low and stable boundary layer. Concentrations decrease in March-June due to increasing temperatures and a higher boundary layer. The lowest concentrations are during the rainy months (June to August/Sept) due to wet removal. OC and EC fraction is higher in PM2.5. EC in in PM2.5 is 9%, and in PM2.5-10 size EC is 2%. OC contribution is about 36% of fine aerosol mass. High OC could be attributed to enhanced combustion sources and the meteorological conditions during winter period. High OC to EC ratio during postmonsoon and winter also supports higher secondary organic aerosol (SOA) formation in these seasons. Secondary organic carbon (SOC) calculated is 42% of the annual average of total OC in coarse fraction. SOC to total OC is highest in postmonsoon (53%), winter (34%) and followed by 29% in summer and monsoon seasons. 24-hr speciated fine and coarse aerosols annual data was used for source identification and quantification studies with

  11. Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

    PubMed Central

    Burkart, J.; Steiner, G.; Reischl, G.; Hitzenberger, R.

    2011-01-01

    During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22 nm and 929 nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160 cm−3 to 3600 cm−3 with a campaign average of 820 cm−3. Activation ratios were quite low (0.02–0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169 nm, range: (69–370) nm) than activation diameters for single-salt particles (around 50 nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations. PMID:21977003

  12. Characterization and source apportionment of aerosol light extinction with a coupled model of CMB-IMPROVE in Hangzhou, Yangtze River Delta of China

    NASA Astrophysics Data System (ADS)

    Wang, Jiao; Zhang, Yu-fen; Feng, Yin-chang; Zheng, Xian-jue; Jiao, Li; Hong, Sheng-mao; Shen, Jian-dong; Zhu, Tan; Ding, Jing; Zhang, Qi

    2016-09-01

    To investigate the characteristics and sources of aerosol light extinction in the Yangtze River Delta of China, a campaign was carried out in Hangzhou from December 2013 to November 2014. Hourly data for air pollutants including PM2.5, SO2, NO2, O3 and CO, and aerosol optical properties including aerosol scattering coefficient and aerosol absorbing coefficient was obtained in the environmental air quality automatic monitoring station. Meteorological parameters were measured synchronously in the automated meteorology monitoring station. Additionally, around seven sets of ambient PM2.5 samples per month were collected and analyzed during the campaign. The annual mean aerosol scattering coefficient, aerosol absorbing coefficient and aerosol single scattering albedo measured in this study was 514 ± 284 Mm- 1, 35 ± 20 Mm- 1 and 94% respectively. The aerosol extinction coefficient reconstructed using the modified IMPROVE (Interagency Monitoring of Protected Visual Environment) formula was compared to the measured extinction coefficient. Better correlations could be found between the measured and reconstructed extinction coefficient when RH was under 90%. A coupled model of CMB (chemical mass balance) and modified IMPROVE was used to apportion the sources of aerosol light extinction in Hangzhou. Vehicle exhaust, secondary nitrate and secondary sulfate were identified as the most significant sources for aerosol light extinction, accounted for 30.2%, 24.1% and 15.8% respectively.

  13. Yearly trend of dicarboxylic acids in organic aerosols from south of Sweden and source attribution

    NASA Astrophysics Data System (ADS)

    Hyder, Murtaza; Genberg, Johan; Sandahl, Margareta; Swietlicki, Erik; Jönsson, Jan Åke

    2012-09-01

    Seven aliphatic dicarboxylic acids (C3-C9) along with phthalic acid, pinic acid and pinonic acid were determined in 35 aerosol (PM10) samples collected over the year at Vavihill sampling station in south of Sweden. Mixture of dichloromethane and methanol (ratio 1:3) was preferred over water for extraction of samples and extraction was assisted by ultrasonic agitation. Analytes were derivatized using N,O-bis(trimethylsilyl)trifluoroacetamide (BSTFA) containing 1% trimethylsilyl chloride and analyzed using gas chromatography/mass spectrometry. Among studied analytes, azelaic acid was found maximum with an average concentration of 6.0 ± 3.6 ng m-3 and minimum concentration was found for pimelic acid (1.06 ± 0.63 ng m-3). A correlation coefficients analysis was used for defining the possible sources of analytes. Higher dicarboxylic acids (C7-C9) showed a strong correlation with each other (correlation coefficients (r) range, 0.96-0.97). Pinic and pinonic acids showed an increase in concentration during summer. Lower carbon number dicarboxylic acids (C3-C6) and phthalic acid were found strongly correlated, but showed a poor correlation with higher carbon number dicarboxylic acids (C7-C9), suggesting a different source for them. Biomass burning, vehicle exhaust, photo-oxidation of volatile organic compounds (natural and anthropogenic emissions) were possible sources for dicarboxylic acids.

  14. Sources of black carbon in aerosols: fossil fuel burning vs. biomass burning

    NASA Astrophysics Data System (ADS)

    Hsieh, Y.

    2013-12-01

    The uncertainty in black carbon (BC) analysis and our inability to directly quantify the BC sources in the atmosphere has led to the uncertainty in compiling a regional or global BC emission inventory attributed to biomass burnings. We initiate this study to demonstrate a new approach, which quantifies the source of BC in the atmosphere between biomass and fossil fuel burnings. We applied the newly developed multi-element scanning thermal analysis (MESTA) technology to quantify BC and organic carbon (OC), respectively, in aerosol samples. MESTA can also separate BC from OC for subsequent radiocarbon analyses. Because fossil fuel has been depleted of radiocarbon and biomass has radiocarbon of the modern atmospheric level, we can quantify the sources of BC between fossil fuel and biomass burnings. We sampled the PM2.5 in the ambient air of central Tallahassee and its rural areas during the May-June (prescribed burning) and Nov-Dec (non-burning) periods. The results indicate that biomass burning contributed 89×1% and 67×2% of BC, respectively, during May-June and Nov.-Dec. periods. The rest of PM2.5 BC was contributed from fossil fuel burning. The radiocarbon contents of the OC was 103.42×0.55 percent modern carbon (pmC), which is consistent with the current atmospheric level with a trace of the bomb radiocarbon remained from the open atmosphere nuclear testing.

  15. Composition and Sourcing of Aerosol in the Mexico City Metropolitan Area with PIXE/PESA/STIM and Multivariate Analysis

    NASA Astrophysics Data System (ADS)

    Zuberi, B.; Johnson, K. S.; de Foy, B.; Molina, L. T.; Molina, M. J.; Shutthanandan, V.; Xie, Y.; Disselkamp, R.; Jimenez, J.; Dzepina, K.; Salcedo, D.

    2004-12-01

    Particulate matter <2.5 μ m in diameter (PM2.5) is a serious concern in megacity air pollution for its possible effects on human health and climate, and potential role in heterogeneous chemical processes. Determining the chemical composition of PM2.5 is essential in assessing their effects, and the various aerosol emission sources must be identified in order to develop effective pollution control strategies. Samples of PM2.5 were collected in a southeastern site in the Mexico City Metropolitan Area (MCMA) during the MCMA-2003 campaign between April 3 - May 4, 2003 with a 3-stage IMPROVED Cascade DRUM Impactor in size ranges 0.07 - 0.34 μ m (Stage C), 0.34 - 1.15 μ m (Stage B), and 1.15 - 2.5 μ m (Stage A). Analyses by Proton-Induced X-ray Emission (PIXE), Proton-Elastic Scattering Analysis (PESA) and Scanning Transmission Ion Microscopy (STIM) were performed to provide 6-hr averaged concentrations of elements > Na, H, and total aerosol mass, respectively, for each size range. Multivariate analysis including Positive Matrix Factorization (PMF) was applied to group elements by common factors to identify possible aerosol emission sources within each size range. Sudden increases in elements characteristic of industrial emissions and fuel oil suggest manufacturing sources to the north of the city whereas soil aerosols originate from more rural areas to the south. Sulfur contributes to a significant fraction of PM2.5, in agreement with complementary aerosol measurements taken during the campaign. Additional trends and diurnal profiles observed for Mexico City aerosol are presented.

  16. Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

    NASA Astrophysics Data System (ADS)

    Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.

    2012-12-01

    137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

  17. Long-term (2007-2013) analysis of aerosol optical properties over four locations in the Indo-Gangetic plains.

    PubMed

    Bibi, Humera; Alam, Khan; Blaschke, Thomas; Bibi, Samina; Iqbal, Muhammad Jawed

    2016-08-10

    that the seasonal variation in aerosol types was influenced by a contribution of air masses from multiple source locations. PMID:27534460

  18. Spatial variability of carbonaceous aerosols and associated source tracers in two cites in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Snyder, David C.; Rutter, Andrew P.; Worley, Chris; Olson, Mike; Plourde, Anthony; Bader, Rebecca C.; Dallmann, Timothy; Schauer, James J.

    2010-05-01

    Semi-continuous and 24-h averaged measurements of fine carbonaceous aerosols were made concurrently at three sites within each of two U.S. Midwestern Cities; Detroit, Michigan and Cleveland, Ohio; during two, one-month intensive campaigns conducted in July of 2007 and January & February of 2008. A comparison of 24-h measurements revealed substantial intra-urban variability in carbonaceous aerosols consistent with the influence of local sources, and excesses in both PM 2.5 organic carbon (OC) and elemental carbon (EC) were identified at individual sites within each city. High time-resolved black carbon (BC) measurements indicated that elemental carbon concentrations were higher at sites adjacent to freeways and busy surface streets, and temporal patterns suggested that excess EC at sites adjacent to freeways was dominated by mobile source emissions while excesses in EC away from traffic corridors was dominated by point/area source emissions. The site-to-site variability in OC concentrations was approximately 7% within the neighborhood scale (0.5-4 km) and between 4 and 27% at the urban scale (4-100 km). In contrast, measurements of organic source tracers, in conjunction with a Chemical Mass Balance (CMB) source-apportionment model, indicated that the spatial variation in the contribution of both mobile and stationary sources to PM 2.5 OC often exceeded the variation in OC mass concentration by a factor of 3 or more. Markers for mobile sources, biomass smoke, natural gas, and coal combustion differed by as much as 60% within the neighborhood scale and by greater than 200% within the urban scale. The observations made during this study suggest that the urban excess of carbonaceous aerosols is much more complex than has been previously reported and that a more rigorous, source-oriented approach should be taken in order to assess the risk associated with exposure to carbonaceous aerosols within the industrialized environments of the Midwestern United States.

  19. Optical Properties of Aerosols from Long Term Ground-Based Aeronet Measurements

    NASA Technical Reports Server (NTRS)

    Holben, B. N.; Tanre, D.; Smirnov, A.; Eck, T. F.; Slutsker, I.; Dubovik, O.; Lavenu, F.; Abuhassen, N.; Chatenet, B.

    1999-01-01

    AERONET is an optical ground-based aerosol monitoring network and data archive supported by NASA's Earth Observing System and expanded by federation with many non-NASA institutions including AEROCAN (AERONET CANada) and PHOTON (PHOtometrie pour le Traiteinent Operatonnel de Normalisation Satellitaire). The network hardware consists of identical automatic sun-sky scanning spectral radiometers owned by national agencies and universities purchased for their own monitoring and research objectives. Data are transmitted hourly through the data collection system (DCS) on board the geostationary meteorological satellites GMS, GOES and METEOSAT and received in a common archive for daily processing utilizing a peer reviewed series of algorithms thus imposing a standardization and quality control of the product data base. Data from this collaboration provides globally distributed near real time observations of aerosol spectral optical depths, aerosol size distributions, and precipitable water in diverse aerosol regimes. Access to the AERONET data base has shifted from the interactive program 'demonstrat' (reserved for PI's) to the AERONET homepage allowing faster access and greater development for GIS object oriented retrievals and analysis with companion geocoded data sets from satellites, LIDAR and solar flux measurements for example. We feel that a significant yet under utilized component of the AERONET data base are inversion products made from hourly principal plane and almucanter measurements. The current inversions have been shown to retrieve aerosol volume size distributions. A significant enhancement to the inversion code has been developed and is presented in these proceedings.

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

    SciTech Connect

    Worsnop, Douglas R.

    2014-07-28

    This project funded the participation of scientists from seven research groups, running more than thirty instruments, in 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. The primary science questions for the ClearfLo Winter IOP were, 1) what is the urban increment of particulate matter (PM) and other pollutants in the greater London area, and, 2) what is the contribution of solid fuel use for home heating to wintertime PM? An additional motivation for the Detling measurements was the question of whether coatings on black carbon particles enhance absorption. The following four key accomplishments have been identified so far: 1) Chemical, physical and optical characterization of PM from local and regional sources (Figures 2, 4, 5 and 6). 2) Measurement of urban increment in particulate matter and gases in London (Figure 3). 3) Measurement of optical properties and chemical composition of coatings on black carbon containing particles indicates absorption enhancement. 4) First deployment of chemical ionization instrument (MOVI-CI-TOFMS) to measure both particle-phase and gas-phase organic acids. (See final report from Joel Thornton, University of Washington, for details.) Analysis of the large dataset acquired in Detling is ongoing and will yield further key accomplishments. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal. The measurement of absorption enhancement by coatings on black carbon will contribute to improved modeling of the direct radiative properties of PM.

  1. Chemically-resolved volatility measurements of organic aerosol fom different sources.

    PubMed

    Huffman, J A; Docherty, K S; Mohr, C; Cubison, M J; Ulbrich, I M; Ziemann, P J; Onasch, T B; Jimenez, J L

    2009-07-15

    A newly modified fast temperature-stepping thermodenuder (TD) was coupled to a High Resolution Time-of-Flight Aerosol Mass Spectrometer for rapid determination of chemically resolved volatility of organic aerosols (OA) emitted from individual sources. The TD-AMS system was used to characterize primary OA (POA) from biomass burning, trash burning surrogates (paper and plastic), and meat cooking as well as chamber-generated secondary OA (SOA) from alpha-pinene and gasoline vapor. Almost all atmospheric models represent POA as nonvolatile, with no allowance for evaporation upon heating or dilution, or condensation upon cooling. Our results indicate that all OAs observed show semivolatile behavior and that most POAs characterized here were at least as volatile as SOA measured in urban environments. Biomass-burning OA (BBOA) exhibited a wide range of volatilities, but more often showed volatility similar to urban OA. Paper-burning resembles some types of BBOA because of its relatively high volatility and intermediate atomic oxygen-to-carbon (O/C) ratio, while meat-cooking OAs (MCOA) have consistently lower volatility than ambient OA. Chamber-generated SOA under the relatively high concentrations used intraditional experiments was significantly more volatile than urban SOA, challenging extrapolation of traditional laboratory volatility measurements to the atmosphere. Most OAs sampled show increasing O/C ratio and decreasing H/C (hydrogen-to-carbon) ratio with temperature, further indicating that more oxygenated OA components are typically less volatile. Future experiments should systematically explore a wider range of mass concentrations to more fully characterize the volatility distributions of these OAs. PMID:19708365

  2. Marine biogenic aerosol sources simulated from below the global ocean-atmosphere interface

    NASA Astrophysics Data System (ADS)

    Elliott, S.; Burrows, S. M.; Cameron-Smith, P. J.; Deal, C.; Maltrud, M. E.; Ogunro, O. O.; Russell, L. M.; Wang, S.; Wingenter, O. W.

    2015-12-01

    Full understanding of biogenic aerosol emissions may require modeling of production, interconversion, phase changes and other processes influencing precursor distributions below the ocean surface. We describe a bottom-up, chemical oceanographic approach to the representation of marine sources now under development for Earth System Models in the U.S. Department of Energy. The motivation is to move beyond indirect bulk indicators such as chlorophyll or total dissolved organics. Dynamic mechanistic capabilities are sought for the relevant mixed layer materials and flux fields. The resulting fidelity and predictive capabilities may prove crucial during the era of global change. Reactive transport calculations are outlined for organosulfur, the suite of biomacromolecules, their degradation products plus both interphase or interfacial transitions. Volatile and polymeric substances are controlled on a compound by compound basis, driven by results from a global ecodynamics model of multiple phytotaxa and trophic levels. Surfactant behavior is considered simultaneously at the global bubble and atmospheric interfaces, and such two dimensional chemistry is extended beyond Langmuir monolayers to electrostatically supported films. Colloidal and gel sweeping-impaction by the wind-driven bubble field are considered as alternate means of vertical transport. At the top of the ocean within the microlayer, effects on sea spray number flux are estimated. Moving beyond aerosol emissions, our methods can also provide insight into the uncertainties traditionally inherent to sea-air gas transfer, since they are connected to macromolecular viscoelastics in the laminar barrier layer. We find that resolution of all these subsurface processes is possible at the level of the biogeographic marine province, including specialized treatments for the ice domain, sea ice edge and coastal regime.

  3. Long-term changes in the aerosol optical thickness in moscow and correction under strong atmospheric turbidity

    NASA Astrophysics Data System (ADS)

    Gorbarenko, E. V.; Rublev, A. N.

    2016-03-01

    We have estimated and compensated the error in long-term series of the aerosol optical thickness (AOT) calculated from the data on direct integral solar radiation measured by a standard actinometer at the Meteorological Observatory of the Moscow State University (MO MSU) for strong atmospheric turbidity conditions. The necessary corrections have been obtained by the Monte-Carlo simulation of the actinometry measurements for different atmospheric conditions, taking into account the angular size of the field of view of the instrument; and a special correctional formula has been obtained. This correction formula has been applied for all timed AOT values of above 0.5 observed at the MO MSU for the entire time period from 1955 to 2013. Changes in the long-term average AOT values in Moscow occurred only when the smoky haze from the forest and peat fires affected the aerosol turbidity of the atmosphere. Here, the significant decreasing trend of aerosol optical depth of the atmosphere from 1955 to 2013 has been retained with the same confidence level.

  4. Chemical composition and sources of organic aerosols over London from the ClearfLo 2012 campaigns

    NASA Astrophysics Data System (ADS)

    Finessi, Emanuela; Holmes, Rachel; Hopkins, James; Lee, James; Harrison, Roy; Hamilton, Jacqueline

    2014-05-01

    Air quality in urban areas represents a major public health issue with around one third of the European population concentrated in cities and numbers expected to increase at global scale, particularly in developing countries. Particulate matter (PM) represents a primary threat for human health as numerous studies have confirmed the association between increased levels of cardiovascular and respiratory diseases with the exposure to PM. Despite considerable efforts made in improving air quality and progressively stricter emissions regulations, the PM concentrations have not changed much over the past decades for reasons that remain unclear, and highlight that studies on PM source apportionment are required for the formulation of effective policy. We investigated the chemical composition of organic aerosol (OA) collected during two intensive field campaigns held in winter and summer 2012 in the frame of the project Clean air for London (http://www.clearflo.ac.uk/). PM samples were collected both at a city background site (North Kensington) and at a rural site 50 km southeast of London (Detling) with 8 to 24 hours sampling schedule and analysed using off-line methods. Thermal-optical analysis was used to quantify OC-EC components while a suite of soft ionization mass spectrometric techniques was deployed for detailed chemical characterization. Liquid chromatography mass Spectrometry (LC-MSn) was mostly used for the simultaneous detection and quantification of various tracers for both primary and secondary OA sources. Well-established markers for wood burning primary OA like levoglucosan and azelaic acid were quantified together with various classes of nitroaromatics including methyl-nitrocatechols that are potential tracers for wood burning secondary OA. In addition, oxidation products of biogenic VOCs such as isoprene and monoterpenes were also quantified for both seasons and sites. A non-negligible contribution from biogenic SOA to urban OA was found in summertime

  5. Reconstruction of long-term aerosol optical depth series with sunshine duration records

    NASA Astrophysics Data System (ADS)

    Sanchez-Romero, A.; Sanchez-Lorenzo, A.; González, J. A.; Calbó, J.

    2016-02-01

    We report the suitability of sunshine duration (SD) records as a proxy for the reconstruction of atmospheric aerosol content, for which little information exists, especially prior to the 1980s. Specifically, we have treated cloudless summer days in 16 stations throughout Spain. For almost all sites we find statistically significant relationships between aerosol optical depth (AOD) and daily SD. The correlation coefficient presents a mean value of -0.72, and slope values of the linear regressions are within the range [-0.11, -0.36]. The relationships are used to generate AOD series back to the 1960s (to the 1920s for Madrid). These reconstructed series show an increase in AOD from the mid-1960s to the 1980s, followed by a decrease until the present, in agreement with changes in anthropogenic aerosol emissions and with opposite trends of solar irradiance. The method can be used to reconstruct AOD from the late nineteenth century at many stations worldwide.

  6. Effect of hygroscopic growth on the aerosol light-scattering coefficient: A review of measurements, techniques and error sources

    NASA Astrophysics Data System (ADS)

    Titos, G.; Cazorla, A.; Zieger, P.; Andrews, E.; Lyamani, H.; Granados-Muñoz, M. J.; Olmo, F. J.; Alados-Arboledas, L.

    2016-09-01

    Knowledge of the scattering enhancement factor, f(RH), is important for an accurate description of direct aerosol radiative forcing. This factor is defined as the ratio between the scattering coefficient at enhanced relative humidity, RH, to a reference (dry) scattering coefficient. Here, we review the different experimental designs used to measure the scattering coefficient at dry and humidified conditions as well as the procedures followed to analyze the measurements. Several empirical parameterizations for the relationship between f(RH) and RH have been proposed in the literature. These parameterizations have been reviewed and tested using experimental data representative of different hygroscopic growth behavior and a new parameterization is presented. The potential sources of error in f(RH) are discussed. A Monte Carlo method is used to investigate the overall measurement uncertainty, which is found to be around 20-40% for moderately hygroscopic aerosols. The main factors contributing to this uncertainty are the uncertainty in RH measurement, the dry reference state and the nephelometer uncertainty. A literature survey of nephelometry-based f(RH) measurements is pres