Science.gov

Sample records for aerosol source functions

  1. 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

  2. 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

  3. Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles.

    PubMed

    Russell, Lynn M; Bahadur, Ranjit; Ziemann, Paul J

    2011-03-01

    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.

  4. Size distributions and source function of sea spray aerosol over the South China Sea

    NASA Astrophysics Data System (ADS)

    Chu, Yingjia; Sheng, Lifang; Liu, Qian; Zhao, Dongliang; Jia, Nan; Kong, Yawen

    2016-08-01

    The number concentrations in the radius range of 0.06-5 μm of aerosol particles and meteorological parameters were measured on board during a cruise in the South China Sea from August 25 to October 12, 2012. Effective fluxes in the reference height of 10 m were estimated by steady state dry deposition method based on the observed data, and the influences of different air masses on flux were discussed in this paper. The number size distribution was characterized by a bimodal mode, with the average total number concentration of (1.50 ± 0.76)×103 cm-3. The two mode radii were 0.099 µm and 0.886 µm, both of which were within the scope of accumulation mode. A typical daily average size distribution was compared with that measured in the Bay of Bengal. In the whole radius range, the number concentrations were in agreement with each other; the modes were more distinct in this study than that abtained in the Bay of Bengal. The size distribution of the fluxes was fitted with the sum of log-normal and power-law distribution. The impact of different air masses was mainly on flux magnitude, rather than the shape of spectral distribution. A semiempirical source function that is applicable in the radius range of 0.06 µm< r 80<0.3 µm with the wind speed varying from 1.00 m s-1 to 10.00 m s-1 was derived.

  5. A sea-state based source function for size and composition resolved marine aerosol

    SciTech Connect

    Long, Michael S; Keene, William C; Erickson III, David J

    2011-01-01

    A parameterization for the size- and composition-resolved production fluxes of nascent marine aerosol was developed from prior experimental observations and extrapolated to ambient conditions based on estimates of air entrainment by the breaking of wind-driven ocean waves. Production of particulate organic carbon (OC{sub aer}) was parameterized based on Langmuir equilibrium-type association of organic matter to bubble plumes in seawater and resulting aerosol as constrained by measurements of aerosol produced from productive and oligotrophic seawater. This novel approach is the first to parameterize size- and composition-resolved aerosol production based on explicit evaluation of wind-driven air entrainment/detrainment fluxes and chlorophyll-a as a proxy for surfactants in surface seawater. Production fluxes were simulated globally with an eight aerosol-size-bin version of the NCAR Community Atmosphere Model (CAM v3.5.07). Simulated production fluxes fell within the range of published estimates based on observationally constrained parameterizations. Because the parameterization does not consider contributions from spume drops, the simulated global mass flux (1.5 x 10{sup 3} Tg y{sup -1}) is near the lower end of published estimates. The simulated production of aerosol number (1.4 x 10{sup 6} m{sup -2} s{sup -1}) and OC{sub aer} (29 Tg C y{sup -1}) fall near the upper end of published estimates and suggest that primary marine aerosols may have greater influences on the physicochemical evolution of the troposphere, radiative transfer and climate, and associated feedbacks on the surface ocean than suggested by previous model studies.

  6. Atmospheric aerosol over Finnish Arctic: source analysis by the multilinear engine and the potential source contribution function

    NASA Astrophysics Data System (ADS)

    Yli-Tuomi, Tarja; Hopke, Philip K.; Paatero, Pentti; Basunia, M. Shamsuzzoha; Landsberger, Sheldon; Viisanen, Yrjö; Paatero, Jussi

    Week-long samples of total suspended particles were collected between 1964 and 1978 from Kevo at the Finnish Arctic and analyzed for a number of chemical species. The chemical composition data was analyzed using a mixed 2-way/3-way model. The results of receptor modeling were connected with the back trajectory data in a Potential Source Contribution Function analysis to determine the likely source areas. Nine sources, namely silver emissions, coal/oil shale combustion, biomass burning, non-ferrous smelters (two sources), crustal elements from remote sources, excess silicon from local sources, sea salt particles and biogenic sulfur emissions from marine algae were found. Although the emissions from industrial areas in the Kola Peninsula had an effect on the concentration of anthropogenic pollutants at Kevo, the highest concentrations during winter were transported from the sources in the mid-latitudes. The yearly strength of the biogenic sulfur emissions showed no dependence on the Northern Hemisphere temperature anomaly and thus, a climatic feedback loop could not be confirmed.

  7. Comparing momentum and mass (aerosol source function) fluxes for the North Atlantic and the European Arctic using different parameterizations

    NASA Astrophysics Data System (ADS)

    Wróbel, Iwona; Piskozub, Jacek

    2016-04-01

    Wind speed has a disproportionate role in the forming of the climate as well it is important part in calculate of the air-sea interaction thanks which we can study climate change. It influences on mass, momentum and energy fluxes and the standard way of parametrizing those fluxes is use this variable. However, the very functions used to calculate fluxes from winds have evolved over time and still have large differences (especially in the case of aerosol sources function). As we have shown last year at the EGU conference (PICO presentation EGU2015-11206-1) and in recent public article (OSD 12,C1262-C1264,2015) there is a lot of uncertainties in the case of air-sea CO2 fluxes. In this study we calculated regional and global mass and momentum fluxes based on several wind speed climatologies. To do this we use wind speed from satellite data in FluxEngine software created within OceanFlux GHG Evolution project. Our main area of interest is European Arctic because of the interesting air-sea interaction physics (six-monthly cycle, strong wind and ice cover) but because of better data coverage we have chosen the North Atlantic as a study region to make it possible to compare the calculated fluxes to measured ones. An additional reason was the importance of the area for the North Hemisphere climate, and especially for Europe. The study is related to an ESA funded OceanFlux GHG Evolution project and is meant to be part of a PhD thesis (of I.W) funded by Centre of Polar Studies "POLAR-KNOW" (a project of the Polish Ministry of Science). We have used a modified version FluxEngine, a tool created within an earlier ESA funded project (OceanFlux Greenhouse Gases) for calculating trace gas fluxes to derive two purely wind driven (at least in the simplified form used in their parameterizations) fluxes. The modifications included removing gas transfer velocity formula from the toolset and replacing it with the respective formulas for momentum transfer and mass (aerosol production

  8. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

    2014-11-01

    Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (-29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (-52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm < Da < 10 μm) at Amsterdam Island. This suggests that at least the high end of the previous estimates of sea spray mass emissions is unrealistic. On the other hand, the model clearly underestimated the observed concentrations of organic or total carbonaceous aerosol at Mace Head (-82%) and Amsterdam Island (-68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to

  9. Nanoelectrospray aerosols from microporous polymer wick sources

    NASA Astrophysics Data System (ADS)

    Tepper, Gary; Kessick, Royal

    2009-02-01

    Nanoelectrospray aerosols were formed from microporous polymer wick sources. Current-voltage characteristics were measured as a function of solution electrical conductivity and surface tension and two distinct electrospray modes were observed. In the first mode, when the maximum capillary flow rate through the wick exceeds the electrospray flow rate, a single electrospray forms from a droplet at the end of the wick. In the second mode, when the maximum capillary flow rate is less than the electrospray flow rate, a multitude of microscopic nanoelectrospray sources are formed from within the surface of the wick tip.

  10. 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

  11. Marine submicron aerosol gradients, sources and sinks

    NASA Astrophysics Data System (ADS)

    Ceburnis, Darius; Rinaldi, Matteo; Ovadnevaite, Jurgita; Martucci, Giovanni; Giulianelli, Lara; O'Dowd, Colin D.

    2016-10-01

    Aerosol principal sources and sinks over eastern North Atlantic waters were studied through the deployment of an aerosol chemistry gradient sampling system. The chemical gradients of primary and secondary aerosol components - specifically, sea salt (SS), water-insoluble organic matter (WIOM), water-soluble organic matter (WSOM), nitrate, ammonium, oxalate, amines, methanesulfonic acid (MSA) and water-soluble organic nitrogen (WSON) - were examined in great detail. Sea salt fluxes were estimated by the boundary layer box model and ranged from 0.3 to 3.5 ng m-2 s-1 over the wind speed range of 5-12 m s-1 and compared well with the derived fluxes from existing sea salt source parameterisations. The observed seasonal pattern of sea salt gradients was mainly driven by wind stress in addition to the yet unquantified effect of marine OM modifying fractional contributions of SS and OM in sea spray. WIOM gradients were a complex combination of rising and waning biological activity, especially in the flux footprint area, and wind-driven primary sea spray production supporting the coupling of recently developed sea spray and marine OM parameterisations.

  12. 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.

  13. 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.

  14. 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.

  15. 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

  16. Aerosol optical depths and their contributing sources in Taiwan

    NASA Astrophysics Data System (ADS)

    Chan, K. L.; Chan, K. L.

    2017-01-01

    In this paper, we present a quantitative investigation of the contributions of different aerosols to the aerosol optical depths (AODs) in Taiwan using a global chemical transport model (GEOS-Chem) and remote sensing measurements. The study focus is on the period from June 2012 to October 2013. Five different types of aerosols are investigated: sea salt, dust, sulfate, organic carbon and black carbon. Three of these aerosols, namely sulfate, organic carbon and black carbon, have significant anthropogenic sources. Model simulation results were compared with both ground based sun photometer measurements and MODerate resolution Imaging Spectroradiometer (MODIS) satellite observations. The model data shows good agreement with satellite observations (R = 0.72) and moderate correlation with sun photometer measurements (R = 0.52). Simulation results show the anthropogenic aerosols contribute ∼65% to the total AOD in Taipei, while natural originated aerosols only show a minor impact (∼35%). Among all the aerosols, sulfate is the dominating species, contributing 62.4% to the annual average total AOD. Organic carbon and black carbons respectively contribute 7.3% and 1.5% to the annual averaged total AOD. The annual average contributions of sea salt and dust aerosols to the total AOD are 26.4% and 2.4%, respectively. A sensitivity study was performed to identify the contributions of anthropogenic aerosol sources in each region to the AODs in Taipei. North-East Asia was identified as the major contributing source region of anthropogenic aerosols to Taipei, accounting for more than 50% of total sulfate, 32% of total organic carbon and 51% of total black carbon aerosols. South-East Asia is the second largest contributing source region, contributing 35%, 24% and 34% of total sulfate, organic carbon and black carbon aerosols, respectively. The aerosols from continents other than Asia only show minor impacts to the aerosol load in Taipei. In addition, a case study of a biomass

  17. 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

  18. Organic Mass Fragments and Organic Functional Groups in Aged Biomass Burning and Fossil Fuel Combustion Aerosol

    NASA Astrophysics Data System (ADS)

    Day, D. A.; Hawkins, L. N.; Russell, L. M.

    2009-12-01

    Organic functional group concentrations in submicron aerosol particles collected from 27 June to 17 September at the Scripps Pier in La Jolla, California as part of AeroSCOPE 2008 were quantified using Fourier Transform Infrared (FTIR) spectroscopy. Organic and inorganic non-refractory components in the same air masses were quantified using a Quadrupole Aerosol Mass Spectrometer (Q-AMS). Previous measurements at the Scripps pier indicate that a large fraction of submicron particle mass originates in Los Angeles and the port of Long Beach. Additional particle sources to the region include local urban emissions and periodic biomass burning during large wildfires. Three distinct types of organic aerosol components were identified from organic composition and elemental tracers, including biomass burning, fossil fuel combustion, and polluted marine components. Fossil fuel combustion organic aerosol was dominated by unsaturated alkane and was correlated with sulfur, vanadium, and nickel supporting ship and large trucks in and around the Los Angeles/Long Beach region as the dominant source. Biomass burning organic aerosol comprised a smaller unsaturated alkane fraction and larger fractions of non-acid carbonyl, amine, and carboxylic acid and was correlated with potassium and bromine. Polluted marine organic aerosol was dominated by organic hydroxyl and unsaturated alkane and was not correlated with any elemental tracers. Mass spectra of the organic aerosol support the aerosol sources determined by organic functional groups and elemental tracers and contain fragments commonly attributed to oxygenated organic aerosol (OOA), hydrocarbon-like organic aerosol (HOA), and biomass burning organic aerosol (BBOA). Comparisons of the PMF-derived Q-AMS source spectra with FTIR source spectra and functional group composition provide additional information on the relationship between commonly reported organic aerosol factors and organic functional groups in specific organic aerosol

  19. Transport characteristics of aerosol from urban point sources

    NASA Astrophysics Data System (ADS)

    Kunkel, Daniel; Lawrence, Mark G.; Kerkweg, Astrid; Tost, Holger; Jöckel, Patrick; Borrmann, Stephan

    2010-05-01

    Urban aerosols are an important source of regional and global air pollution. The local buildup, long-range transport, and dry and wet deposition of aerosols depend strongly on the aerosol size distribution and on the regional meteorological characteristics. We examine the characteristics of urban aerosol dispersion based on simulations of monodisperse passive aerosol tracers with sizes of 0.1, 1.0, 2.5, and 10.0 μm, performed with the global chemistry circulation model EMAC (ECHAM5-MESSy-Atmospheric-Chemistry). 39 point sources were selected for the analysis, originating from major population centers (MPCs) around the world. All tracers, one for each source and size, have the same total, constant emission flux, and undergo dry and wet aerosol deposition. Sensitivity simulations are performed in which either there is no activation of the aerosol as cloud condensation nuclei (CCN), or all aerosol is activated as CCN. Using the same constant emission rate for each MPC allows us to compare how different large point sources pollute the atmosphere and the surface on different horizontal scales. The transport and deposition of the aerosol tracers from each MPC are quantitatively compared by the application of metrics. The analysis focuses on: the efficiency of short- and long-range horizontal transport; the fraction of tracer transported to the upper troposphere; and the fractions which are dry or wet deposited. Smaller particles with longer lifetimes (two to 14 days) are more effective at polluting remote locations (horizontal and vertical) and are deposited mostly by scavenging, while larger particles, with shorter lifetimes (several hours to a couple of days) more effectively pollute the environment nearby their source, and are most strongly removed by dry deposition from the atmosphere. By means of considering the same emission for each city, the presentation provides a detailed view of how aerosol tracers disperse and deposit on different spatial scales, depending

  20. Aerosol Use in the Pulmonary Function Lab.

    PubMed

    Ruppel, Gregg L

    2015-06-01

    Aerosolized medications are frequently used in the pulmonary function laboratory. The 2 most common implementations are bronchodilators and bronchial challenge agents. Bronchodilator administration is not well standardized, largely because of the various methods of delivery available for clinical practice. Metered-dose inhalers used with spacer devices are the most common route for bronchodilator administration, but many laboratories use small-volume nebulizers. Interpretation of pre- and post-bronchodilator studies is confounded by the definitions of airway obstruction and bronchodilator responsiveness. Protocols for administering bronchial challenge aerosols (methacholine, mannitol, hypertonic saline) are well defined but are susceptible to some of the same problems that limit comparison of bronchodilator techniques. Bronchial challenges with inhaled aerosols are influenced not only by the delivery device but by the patient's breathing pattern, particularly in protocols that include deep inspiratory efforts.

  1. 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.

  2. Aerosol composition, sources and processes during wintertime in Beijing, China

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Wang, Z. F.; Fu, P. Q.; Yang, T.; Jiang, Q.; Dong, H. B.; Li, J.; Jia, J. J.

    2013-05-01

    Air pollution is a major environmental concern during all seasons in the megacity of Beijing, China. Here we present the results from a winter study that was conducted from 21 November 2011 to 20 January 2012 with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and various collocated instruments. The non-refractory submicron aerosol (NR-PM1) species vary dramatically with clean periods and pollution episodes alternating frequently. Compared to summer, wintertime submicron aerosols show much enhanced organics and chloride, which on average account for 52% and 5%, respectively, of the total NR-PM1 mass. All NR-PM1 species show quite different diurnal behaviors between summer and winter. For example, the wintertime nitrate presents a gradual increase during daytime and correlates well with secondary organic aerosol (OA), indicating a dominant role of photochemical production over gas-particle partitioning. Positive matrix factorization was performed on ACSM OA mass spectra, and identified three primary OA (POA) factors, i.e., hydrocarbon-like OA (HOA), cooking OA (COA), and coal combustion OA (CCOA), and one secondary factor, i.e., oxygenated OA (OOA). The POA dominates OA during wintertime, contributing 69%, with the other 31% being SOA. Further, all POA components show pronounced diurnal cycles with the highest concentrations occurring at nighttime. CCOA is the largest primary source during the heating season, on average accounting for 33% of OA and 17% of NR-PM1. CCOA also plays a significant role in chemically resolved particulate matter (PM) pollution as its mass contribution increases linearly as a function of NR-PM1 mass loadings. The SOA, however, presents a reverse trend, which might indicate the limited SOA formation during high PM pollution episodes in winter. The effects of meteorology on PM pollution and aerosol processing were also explored. In particular, the sulfate mass is largely enhanced during periods with high humidity because of fog

  3. 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.

  4. Linking Aerosol Source Activities to Present and Future Climate Effects

    NASA Astrophysics Data System (ADS)

    Koch, D.; Bond, T. C.; Streets, D.; Menon, S.; Unger, N.

    2007-05-01

    Aerosol source sectors (transport, power, industry, residential, biomass burning) generate distinct mixtures of aerosol species. These mixtures in turn have different effects on climate. As sectoral emissions change in coming decades, whether by regulation or not, it is helpful to link pollution from source types to climate consequences. We do so, using our global (GISS GCM) aerosol model for present and future IPCC SRES scenarios. According to our model, residential and transport sectors have net positive 1995 aerosol forcings (0.04 and 0.03 W m-2) due to their large black carbon contents. However, the sulfate-dominated power and industry sectors have net negative 1995 forcings (-0.10 and -0.09 W m-2). Due to the near-balance of absorbing and scattering components, biomass burning forcing is small. For the 2050 SRES A1B scenario, the net (negative) aerosol forcing is double 1995 due primarily to increased sulfur emissions in the industry and power sectors. For 2050 B1 the net (negative) forcing decreases relative to 1995, as sulfur emissions are reduced. Both future scenarios project decreasing residential emissions. Yet transport emissions are expected to remain significant and thus become the dominant source of warming aerosols in the future. Aerosol pollution is projected to shift southward relative to the present, as the current industrialized regions generally reduce emissions and tropical and southern hemispheric regions continue to develop. Similar to these SRES scenarios, IIASA scenarios project a decline in residential emissions; however IIASA is more optimistic about transport sector emissions reductions. We will conduct present-day climate experiments, including aerosol direct and indirect effects, to study impacts of power and transport sectors on climate features such as air temperature and hydrologic cycle.

  5. 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.

  6. 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.

  7. 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

  8. Concentration, sources, and degradation of organic aerosol at Summit, Greenland

    NASA Astrophysics Data System (ADS)

    von Schneidemesser, Erika

    Characterization and understanding of the carbonaceous portion of the aerosol in the Arctic is limited. The objective of the research presented in this thesis was to improve the scope of knowledge pertaining to carbonaceous aerosols, in terms of atmospheric and snow concentrations, sources, and post-depositional processing. An extraction technique was developed to quantitatively identify a suite of organic compounds, typically observed in aerosol samples, at trace level concentrations in snow melt water samples. A field campaign of sampling and exposure experiments was carried out at Summit, Greenland. A 3-meter snow pit, sampled at 20 cm intervals, was analyzed for organic compounds and total organic carbon (TOC). The average concentration of TOC for the entire pit was 64 mug C kg-1. The quantified organic compounds comprised 6 to 24% of TOC throughout the layers. Median concentrations of the water insoluble individual organic compounds ranged from 0.14 ng kg-1 (hopane) to 2200 ng kg-1 (alkanoic acid) at any one depth. High-volume aerosol samples were collected over a six month period and analyzed for organics. Median concentrations ranged from 0.00045 ng kg-1 (hopane) to 0.23 ng kg-1 (levoglucosan) in the air samples. Source apportionment results from the aerosol samples indicate anthropogenic influence at Summit from biomass burning, fossil fuels, and vegetative detritus. The majority (>90%) of the organic carbon in the aerosol was estimated to be secondary organic aerosol. To investigate the post-depositional processing of organic compounds in snow, contaminant labeled snow was produced and exposed for up to 72 hours on the surface of the Greenland ice sheet at Summit. Degradation of alkanes, acids, and PAHs to a threshold concentration was observed. The threshold concentration, at which no further degradation was observed, ranged from 10 to 60% of the original (non-exposed) snow concentrations, depending on the reaction rate. This would indicate that a

  9. 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.

  10. An analysis of AERONET aerosol absorption properties and classifications representative of aerosol source regions

    NASA Astrophysics Data System (ADS)

    Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Smirnov, A.; Slutsker, I.; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

    2012-09-01

    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 (τ) and single scattering albedo (ωo) from Aerosol Robotic Network (AERONET) measurements are used to form absorption (i.e., ωo and absorption Ångström exponent (αabs)) and size (i.e., extinction Ångström exponent (αext) and fine mode fraction of τ) 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 averageωo and αabs at each site (expanding upon previous work), (2) perform a sensitivity study on αabs by varying the spectral ωo, and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral ωo averages indicate slightly more aerosol absorption (i.e., a 0.0 < δωo ≤ 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 αabs show significant overlap among aerosol type categories, and at least 10% of the αabs retrievals in each category are below 1.0. Perturbing the spectral ωo by ±0.03 induces significant αabs changes from the unperturbed value by at least ˜±0.6 for Dust, ˜±0.2 for Mixed, and ˜±0.1 for Urban/Industrial and Biomass Burning. The ωo440nm and αext440-870nmrelationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

  11. 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.

  12. 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.

  13. 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.

  14. Source contributions to carbonaceous aerosol concentrations in Korea

    NASA Astrophysics Data System (ADS)

    Jeong, Jaein I.; Park, Rokjin J.; Woo, Jung-Hun; Han, Young-Ji; Yi, Seung-Muk

    2011-02-01

    We estimated the source contributions to carbonaceous aerosol concentration in Korea on the basis of Intercontinental Chemical Transport Experiment Phase B (INTEX-B) anthropogenic emissions and satellite-derived biomass burning emissions by using a nested version of GEOS-Chem with a spatial resolution of 0.5° × 0.667° for the period March 2006-February 2007. First, we evaluated the model by comparing the simulated and observed aerosol concentrations at East Asia Network (EANET) sites and at a site in Korea. The results indicate that the model reproduces the variability and magnitudes of the observed SO 42-, NO 3-, and NH 4+ concentrations in Korea and those of the observed PM 10 concentrations in East Asia. However, the organic carbon (OC) and black carbon (BC) aerosol concentrations estimated by the model are lower than those observed in Korea by a factor of 2, especially in winter. This underestimation is likely due to extremely low domestic anthropogenic emissions and lack in seasonal variation. Source adjustments using a simple fitting and the Emission Database for Global Atmospheric Research (EDGAR) monthly allocation factors for seasonal variation yield significantly improved model results ( R2 increased from 0.58 to 0.84), which can then be used to estimate the source contributions to the OC and BC concentrations in Korea. We found that domestic anthropogenic emissions are the most important factors, contributing 74% (9% from fossil fuels and 65% from biofuels) and 78% (42% from fossil fuels and 36% from biofuels) to the OC and BC concentrations, respectively, on an annual mean basis in Korea. The trans-boundary transport of Chinese sources is another important factor, contributing 13% and 20% to the OC and BC concentrations, respectively. The contributions of wildfires and biogenic sources to the annual mean carbonaceous aerosol concentration in Korea are relatively small (4% and 6%, respectively).

  15. Assessment of source-receptor relationships of aerosols: An integrated forward and backward modeling approach

    NASA Astrophysics Data System (ADS)

    Kulkarni, Sarika

    This dissertation presents a scientific framework that facilitates enhanced understanding of aerosol source -- receptor (S/R) relationships and their impact on the local, regional and global air quality by employing a complementary suite of modeling methods. The receptor -- oriented Positive Matrix Factorization (PMF) technique is combined with Potential Source Contribution Function (PSCF), a trajectory ensemble model, to characterize sources influencing the aerosols measured at Gosan, Korea during spring 2001. It is found that the episodic dust events originating from desert regions in East Asia (EA) that mix with pollution along the transit path, have a significant and pervasive impact on the air quality of Gosan. The intercontinental and hemispheric transport of aerosols is analyzed by a series of emission perturbation simulations with the Sulfur Transport and dEposition Model (STEM), a regional scale Chemical Transport Model (CTM), evaluated with observations from the 2008 NASA ARCTAS field campaign. This modeling study shows that pollution transport from regions outside North America (NA) contributed ˜ 30 and 20% to NA sulfate and BC surface concentration. This study also identifies aerosols transported from Europe, NA and EA regions as significant contributors to springtime Arctic sulfate and BC. Trajectory ensemble models are combined with source region tagged tracer model output to identify the source regions and possible instances of quasi-lagrangian sampled air masses during the 2006 NASA INTEX-B field campaign. The impact of specific emission sectors from Asia during the INTEX-B period is studied with the STEM model, identifying residential sector as potential target for emission reduction to combat global warming. The output from the STEM model constrained with satellite derived aerosol optical depth and ground based measurements of single scattering albedo via an optimal interpolation assimilation scheme is combined with the PMF technique to

  16. 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

  17. 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

  18. Source contributions to black carbon mass fractions in aerosol particles over the northwestern Pacific

    NASA Astrophysics Data System (ADS)

    Koga, Seizi; Maeda, Takahisa; Kaneyasu, Naoki

    Aerosol particle number size distributions above 0.3 μm in diameter and black carbon mass concentrations in aerosols were observed on Chichi-jima of the Ogasawara Islands in the northwestern Pacific from January 2000 to December 2002. Chichi-jima is suitable to observe polluted air masses from East Asia in winter and clean air masses over the western North Pacific in summer. In winter, aerosols over Chichi-jima were strongly affected by anthropogenic emissions in East Asia. The form of energy consumption in East Asia varies in various regions. Hence, each source region is expected to be characterized by an individual black carbon mass fraction. A three-dimensional Eulerian transport model was used to estimate contribution rates to air pollutants from each source region in East Asia. Because the Miyake-jima eruption began at the end of June 2000, the influence of smokes from Miyake-jima was also considered in the model calculation. The results of model calculations represent what must be noticed about smokes from volcanoes including Miyake-jima to interpret temporal variations of sulfur compounds over the northwestern Pacific. To evaluate black carbon mass fractions in anthropogenic aerosols as a function of source region, the relationships between the volume concentration of aerosol particles and the black carbon mass concentration in the winter were classified under each source region in East Asia. Consequently, the black carbon mass fractions in aerosols from China, Japan and the Korean Peninsula, and other regions were estimated to be 9-13%, 5-7%, and 4-5%, respectively.

  19. 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

  20. Light source effects on aerosol photoacoustic spectroscopy measurements

    NASA Astrophysics Data System (ADS)

    Radney, James G.; Zangmeister, Christopher D.

    2017-01-01

    Photoacoustic spectroscopy measurements of flame-generated soot aerosol coated with small amounts of water yielded absorption enhancements that were dependent on the laser used: quasi-continuous wave (Q-CW, ≈650 ps pulse duration and 78 MHz repetition rate) versus continuous wave (CW). Water coating thickness was controlled by exposing the aerosol to a set relative humidity (RH). At ≈85% RH, the mass of the soot particles increased by an amount comparable to a monolayer of water being deposited and enhanced the measured absorption by 36% and 15% for the Q-CW and CW lasers, respectively. Extinction measurements were also performed using a cavity ring-down spectrometer (extinction equals the sum of absorption and scattering) with a CW laser and negligible enhancement was observed at all RH. These findings demonstrate that source choice can impact measurements of aerosols with volatile coatings and that the absorption enhancements at high RH previously measured by Radney and Zangmeister [1] are the result of laser source used (Q-CW) and not from an increase in the particle absorption cross section.

  1. 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

  2. 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.

  3. 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

  4. Aerosol absorption over Bay of Bengal during winter: Variability and sources

    NASA Astrophysics Data System (ADS)

    Kedia, Sumita; Ramachandran, S.; Rajesh, T. A.; Srivastava, Rohit

    2012-07-01

    Measurements of black carbon (BC) mass concentration were made over the Bay of Bengal (BoB) during the period of 27 December 2008-29 January 2009. BC mass concentration is highest over the Coastal-BoB (5.1 ± 3.0 μg m-3) and is more than a factor of two higher than the South-BoB (2.5 ± 1.4 μg m-3). The source regions of BC over the study region is identified using the Total Potential Source Contribution Function (TPSCF) analysis. The probable source regions over the Coastal-BoB and North-BoB (India, Indo-Gangetic plain, Pakistan, Afghanistan) are found to be distinctly different than that over the East-BoB and South-BoB (mostly from southeast Asia). The spectral distribution of absorption coefficients suggested similar source types of BC present over the entire BoB, with significant contribution of absorbing aerosols from the sources other than fossil fuel burning. Our results suggest that the entire BoB remains dominantly influenced by aerosols emitted from biomass/biofuel burning during winter. Single scattering albedo (SSA) is found to vary in the range of 0.63-0.70 over different parts of BoB with the lowest value over Coastal-BoB and the highest value over South-BoB. SSA values observed in the present study are the lowest ever reported over the BoB in the last decade indicating highest concentration of absorbing aerosols over the BoB during winter. The present work and the results obtained will have strong implications while investigating the effect of anthropogenic aerosols over marine environment, and in estimating the spatiotemporal variation of aerosol radiative impact.

  5. Resources of the ionized atmosphere as an aerosol source

    NASA Astrophysics Data System (ADS)

    Smirnov, V. V.; Savchenko, A. V.

    2006-12-01

    The potential resources on the ion-stimulated syntheses effects of aerosol particles of lower troposphere in test sites in the arctic, mountain, arid and forest areas as the function of irradiation time and gas-precursor concentration were experimentally and theoretically evaluated. The dust-free outdoor air was irradiated with an ionization current of 10 - 6 A by α-rays from isotope 239Pu. The total output of radiolytic aerosols (RA) with a diameter of 3-1000 nm was found to be 0.05-0.1 molecules per 1 eV of absorbed radiation, while the physical upper limit is 0.25-0.4 molecules/eV. In an interval of exposition time from 6 to 800 s (adsorbed energy is 3 · 10 12-10 14 eV/cm 3) the RA mass concentration at different sites was increased from 1-10 to 50-500 μg/m 3. According to the liquid chromatography data the major RA material is the H 2O/HNO 3 solution with acid concentration ˜ 25%. The used physical model presents new aerosols as a product from small and intermediate ion association through formation of neutral clusters and describes adequately some of the peculiarities in field experiment data. Introducing SO 2, NH 3, and also hydrochloric, nitric and sulphuric acid vapours with concentration 0.1-1 mg/m 3 in the irradiated air stimulated an increase of mass aerosol concentration by a factor of 8-30. The mean size also decreased by a factor of 3-5. These facts allowed us to expect that the chemical composition of radiolytic aerosols generated in outdoor air would noticeably differ after addition of the gas-precursors.

  6. 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

  7. Nuclear magnetic resonance spectroscopy for determining the functional content of organic aerosols: a review.

    PubMed

    Chalbot, Marie-Cecile G; Kavouras, Ilias G

    2014-08-01

    The knowledge deficit of organic aerosol (OA) composition has been identified as the most important factor limiting our understanding of the atmospheric fate and implications of aerosol. The efforts to chemically characterize OA include the increasing utilization of nuclear magnetic resonance spectroscopy (NMR). Since 1998, the functional composition of different types, sizes and fractions of OA has been studied with one-dimensional, two-dimensional and solid state proton and carbon-13 NMR. This led to the use of functional group ratios to reconcile the most important sources of OA, including secondary organic aerosol and initial source apportionment using positive matrix factorization. Future research efforts may be directed towards the optimization of experimental parameters, detailed NMR experiments and analysis by pattern recognition methods to identify the chemical components, determination of the NMR fingerprints of OA sources and solid state NMR to study the content of OA as a whole.

  8. 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

  9. Source terms for plutonium aerosolization from nuclear weapon accidents

    SciTech Connect

    Stephens, D.R.

    1995-07-01

    The source term literature was reviewed to estimate aerosolized and respirable release fractions for accidents involving plutonium in high-explosive (HE) detonation and in fuel fires. For HE detonation, all estimates are based on the total amount of Pu. For fuel fires, all estimates are based on the amount of Pu oxidized. I based my estimates for HE detonation primarily upon the results from the Roller Coaster experiment. For hydrocarbon fuel fire oxidation of plutonium, I based lower bound values on laboratory experiments which represent accident scenarios with very little turbulence and updraft of a fire. Expected values for aerosolization were obtained from the Vixen A field tests, which represent a realistic case for modest turbulence and updraft, and for respirable fractions from some laboratory experiments involving large samples of Pu. Upper bound estimates for credible accidents are based on experiments involving combustion of molten plutonium droplets. In May of 1991 the DOE Pilot Safety Study Program established a group of experts to estimate the fractions of plutonium which would be aerosolized and respirable for certain nuclear weapon accident scenarios.

  10. Chemical composition of emissions from urban sources of fine organic aerosol

    SciTech Connect

    Hildemann, L.M.; Markowski, G.R.; Cass, G.R. )

    1991-04-01

    A dilution source sampling system was used to collect primary fine aerosol emissions from important sources of urban organic aerosol, including a boiler burning No. 2 fuel oil, a home fireplace, a fleet of catalyst-equipped and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat cooking operations. Alternative dilution sampling techniques were used to collect emissions from cigarette smoking and a roofing tar pot, and grab sample techniques were employed to characterize paved road dust, brake lining wear, and vegetative detritus. Organic aerosol constituted the majority of the fine aerosol mass emitted from many of the sources tested. Fine primary organic aerosol emissions within the heavily urbanized western portion of the Los Angeles Basin were determined to total 29.8 metric ton/day. Over 40% of these organic aerosol emissions are from anthropogenic pollution sources that are expected to emit contemporary (nonfossil) aerosol carbon, in good agreement with the available ambient monitoring data.

  11. 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

  12. 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.

  13. 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.

  14. 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

  15. 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

  16. Boundary layer aerosol chemistry during TexAQS/GoMACCS 2006: Insights into aerosol sources and transformation processes

    NASA Astrophysics Data System (ADS)

    Bates, T. S.; Quinn, P. K.; Coffman, D.; Schulz, K.; Covert, D. S.; Johnson, J. E.; Williams, E. J.; Lerner, B. M.; Angevine, W. M.; Tucker, S. C.; Brewer, W. A.; Stohl, A.

    2008-04-01

    The air quality and climate forcing impacts of atmospheric aerosols in a metropolitan region depend on the amount, composition, and size of the aerosol transported into the region; the input and removal of aerosols and aerosol precursors within the region; and the subsequent chemical processing in the atmosphere. These factors were studied in the Houston-Galveston-Gulf of Mexico region, aboard the NOAA R/V Ronald H. Brown during the Texas Air Quality Study and Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS/GoMACCS 2006). The aerosol measured in the Gulf of Mexico during onshore flow (low radon concentrations indicating no contact with land for several days) was highly impacted by Saharan dust and what appear to be ship emissions (acidic sulfate and nitrate). Mean (median) mass concentrations of the total submicrometer and supermicrometer aerosol were 6.5 (4.6) μg m-3 and 17.2 (8.7) μg m-3, respectively. These mass loadings of "background" aerosol are much higher than typically observed in the marine atmosphere and thus have a substantial impact on the radiative energy balance over the Gulf of Mexico and particulate matter (PM) loadings (air quality) in the Houston-Galveston area. As this background aerosol moved onshore, local urban and industrial sources added an organic rich submicrometer component (66% particulate organic matter (POM), 20% sulfate, 14% elemental carbon) but no significant supermicrometer aerosol. The resulting aerosol had mean (median) mass concentrations of the total submicrometer and supermicrometer aerosol of 10.0 (9.1) μg m-3 and 16.8 (11.2) μg m-3, respectively. These air masses, with minimal processing of urban emissions contained the highest SO2/(SO2 + SO4=) ratios and the highest hydrocarbon-like organic aerosol to total organic aerosol ratios (HOA/POM). In contrast, during periods of offshore flow, the aerosol was more processed and, therefore, much richer in oxygenated organic aerosol (OOA). Mean (median) mass

  17. 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.

  18. Source forensics of black carbon aerosols from China.

    PubMed

    Chen, Bing; Andersson, August; Lee, Meehye; Kirillova, Elena N; Xiao, Qianfen; Kruså, Martin; Shi, Meinan; Hu, Ke; Lu, Zifeng; Streets, David G; Du, Ke; Gustafsson, Örjan

    2013-08-20

    The limited understanding of black carbon (BC) aerosol emissions from incomplete combustion causes a poorly constrained anthropogenic climate warming that globally may be second only to CO2 and regionally, such as over East Asia, the dominant driver of climate change. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain as fossil BC is a stronger climate forcer. The source apportionment is the underpinning for targeted mitigation actions. However, technology-based "bottom-up" emission inventories are inconclusive, largely due to uncertain BC emission factors from small-scale/household combustion and open burning. We use "top-down" radiocarbon measurements of atmospheric BC from five sites including three city sites and two regional sites to determine that fossil fuel combustion produces 80 ± 6% 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 15 BC emission inventory models, including one with monthly resolution. Our results suggest that current climate modeling should refine both BC emission strength and consider the stronger radiative absorption associated with fossil-fuel-derived BC. To mitigate near-term climate effects and improve air quality in East Asia, activities such as residential coal combustion and city traffic should be targeted.

  19. 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

  20. 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.

  1. 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.

  2. A missing source of aerosols in Antarctica - beyond long-range transport, phytoplankton, and photochemistry

    NASA Astrophysics Data System (ADS)

    Giordano, Michael R.; Kalnajs, Lars E.; Avery, Anita; Goetz, J. Douglas; Davis, Sean M.; DeCarlo, Peter F.

    2017-01-01

    Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS - soot particle aerosol mass spectrometer - or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition

  3. 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

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

    SciTech Connect

    Mazurek, M.A. ); Hildemann, L.M. . Dept. of Civil Engineering); Cass, G.R.; Rogge, W.F. ); Simoneit, B.R.T. . Coll. of Oceanography)

    1990-10-01

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

  5. FTIR Analysis of Functional Groups in Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Shokri, S. M.; McKenzie, G.; Dransfield, T. J.

    2012-12-01

    Secondary organic aerosols (SOA) are suspensions of particulate matter composed of compounds formed from chemical reactions of organic species in the atmosphere. Atmospheric particulate matter can have impacts on climate, the environment and human health. Standardized techniques to analyze the characteristics and composition of complex secondary organic aerosols are necessary to further investigate the formation of SOA and provide a better understanding of the reaction pathways of organic species in the atmosphere. While Aerosol Mass Spectrometry (AMS) can provide detailed information about the elemental composition of a sample, it reveals little about the chemical moieties which make up the particles. This work probes aerosol particles deposited on Teflon filters using FTIR, based on the protocols of Russell, et al. (Journal of Geophysical Research - Atmospheres, 114, 2009) and the spectral fitting algorithm of Takahama, et al (submitted, 2012). To validate the necessary calibration curves for the analysis of complex samples, primary aerosols of key compounds (e.g., citric acid, ammonium sulfate, sodium benzoate) were generated, and the accumulated masses of the aerosol samples were related to their IR absorption intensity. These validated calibration curves were then used to classify and quantify functional groups in SOA samples generated in chamber studies by MIT's Kroll group. The fitting algorithm currently quantifies the following functionalities: alcohols, alkanes, alkenes, amines, aromatics, carbonyls and carboxylic acids.

  6. Quantification of aerosol type, and sources of aerosols over the Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Kedia, Sumita; Ramachandran, S.; Holben, B. N.; Tripathi, S. N.

    2014-12-01

    Differences and similarities in aerosol characteristics, for the first time, over two environmentally distinct locations in Indo-Gangetic plain (IGP) - Kanpur (KPR) (urban location) and Gandhi College (GC) (rural site) are examined. Aerosol optical depths (AODs) exhibit pronounced seasonal variability with higher values during winter and premonsoon. Aerosol fine mode fraction (FMF) and Ångström exponent (α) are higher over GC than KPR indicating relatively higher fine mode aerosol concentration over GC. Higher FMF over GC is attributed to local biomass burning activities. Analysis of AOD spectra revealed that aerosol size distribution is dominated by wide range of fine mode fractions or mixture of modes during winter and postmonsoon, while during premonsoon and monsoon coarse mode aerosols are more abundant. Single scattering albedo (SSA) is lower over GC than KPR. SSA spectra reveals the abundance of fine mode (coarse mode) absorbing (scattering) aerosols during winter and postmonsoon (premonsoon and monsoon). Spectral SSA features reveal that OC contribution to enhanced absorption is negligible. Analysis shows that absorbing aerosols can be classified as Mostly Black Carbon (BC), and Mixed BC and Dust over IGP. Mixed BC and dust is always higher over KPR, while Mostly BC is higher over GC throughout the year. The amount of long range transported dust exhibits a gradient between KPR (higher) and GC (lower). Results on seasonally varying aerosol types, and absorbing aerosol types and their gradients over an aerosol hotspot are important to tune models and to reduce the uncertainty in radiative and climate impact of aerosols.

  7. Measurement of the emission rate of an aerosol source--comparison of aerosol and gas transport coefficients.

    PubMed

    Bémer, D; Callé, S; Godinot, S; Régnier, R; Dessagne, J M

    2000-12-01

    A measuring method of the emission rate of an atmospheric pollutant source, based on the use of a tracer gas (helium) and developed in the case of a gaseous source, was tested for an aerosol source. The influence of both particle sedimentation and wall depositions was studied. The transport coefficients of the tracer gas and of alumina particles of various particle sizes (MMAD from 8 to 36 microns) were measured on a vertical axis close to the source, in a 71 m3 room swept by a piston flow. The measurements clearly demonstrated the predominant influence of sedimentation in the case of particles with aerodynamic diameters greater than 10 microns. Particle wall deposition was determined by measuring the gas and particle concentration decay in the ventilated room. To do this, a new tracing method using a fluorescent aerosol was developed. The measured aerosol deposition rates are much higher than those calculated from the formula of Corner for a cubical volume. Aerosol sedimentation and wall deposition are two phenomena limiting the use of a tracer gas to measure the aerosol emission rate. The chemical substances and materials used in work premises are likely to be released into the atmosphere and lead to the formation of pollutants. These emissions stem from either physical or chemical processes (evaporation of a solvent) or from mechanical processes (dispersion of oil droplets at the source of mists).

  8. Scattering Functions Near the Sun by Large Aerosols

    DTIC Science & Technology

    1993-05-20

    Reprint S FLN ;NG N U M 1E q5 I Scattering Functions Near the Sun by Large Aerosols !E 61102F !PR 2310 TA G1 j6. AUTHCR(S) WU 18 iFrederic E. Volz 7...98 ’~ PL-TR-93-2129 a reprint from Applied Optics Scattering functions near the Sun by large aerosols 93-13947 Frederic E. Volz Ill 11111 hil; liill...Introduction no glare (ND = 0) 2°-4’ from the Sun , persistent Over most of the globe, the sky brightness close to the values of ND of - 2.0 (and

  9. 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

  10. Organic Composition and Morphology of Sea Spray Aerosols as a Function of Biological Life during IMPACTS

    NASA Astrophysics Data System (ADS)

    Pham, D.; Moffet, R.; Fraund, M. W.; O'Brien, R.; Laskina, O.; Prather, K. A.; Grassian, V. H.; Beall, C.; Wang, X.; Forestieri, S.; Cappa, C. D.

    2015-12-01

    Aerosols influence climate by directly reflecting or absorbing sunlight, or indirectly by affecting clouds. A major source of aerosols is from oceanic wave breaking. Due to their complexity, the effects of marine aerosol on climate are uncertain. To provide more detailed measurements of the chemical composition of marine aerosols, Scanning Transmission X-Ray Microscopy coupled with Near Edge X-Ray Absorption Fine Structure (SXTM-NEXAFS) was used to give spatially resolved molecular information for carbon and oxygen. Application of STXM/NEXAFS to particles collected during a mesocosm study using a unique wave channel facility to generate aerosols shows that the organic volume fraction of aerosols at the aerodynamic diameter size range of 0.18-0.32 μm are a direct function of the biological activity in the sea water. Aerosol organic volume fraction increased from 0.32 for particles generated from seawater containing low biolife to 0.49 and 0.40 for particles produced during phytoplankton blooms. However, the organic volume fraction of aerosols at the aerodynamic diameter size range of 0.56-1 μm did not change with biological activity. Measurements also show that different types of organics can concentrate into aerosols depending on the enzyme activity expressed at the time. Enhanced spectral signatures for aliphatic hydrocarbons were observed during the first phytoplankton bloom compared to a second phytoplankton bloom occurring directly thereafter. The decreased signature of aliphatic organics in the second phytoplankton bloom was correlated with increased lipase activity from heterobacteria. Organic aggregates having similar morphology also differ in composition from their carbon spectra from the two blooms. For July 17, organic aggregates were much richer in hydrocarbons, which showed a remarkably intense C-H absorbance and a broad C-C absorbance. Organic aggregates observed for July 26-27, did not have the C-H and C-C signatures, but contained more polar

  11. 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.

  12. Aerosols

    Atmospheric Science Data Center

    2013-04-17

    ... article title:  Aerosols over Central and Eastern Europe     View Larger Image ... last weeks of March 2003, widespread aerosol pollution over Europe was detected by several satellite-borne instruments. The Multi-angle ...

  13. 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.

  14. Modeling of secondary organic aerosols from mobile sources in Mexico City

    NASA Astrophysics Data System (ADS)

    Zavala, M.; Lei, W.; Bei, N.; Li, G.; Tsimpidi, A. P.; Karydis, V. A.; Pandis, S.; Molina, L. T.

    2009-04-01

    Mobile sources are significant contributors of emissions of CO, NOx, hydrocarbons and particle matter (PM) that constitute critical precursors of ozone as well as secondary organic and inorganic particles that decisively impact the photochemical levels and aerosol loadings in the atmosphere. Currently there are large uncertainties in regional air quality models during the treatment of aerosol formation from aerosol precursors via the production of condensable organic gases. As a result, the modeling of the concentrations and properties of aerosols resulted from mobile emissions sources is an important challenge. In this study we compare aerosol simulations using the PM-CAMx air quality model linked to the SAPRC99 chemical mechanism with measured aerosol data obtained during the MILAGRO/MCMA-2006 field campaign in Mexico City. The PM-CAMx modeling framework is based on the volatility-basis approach: both primary and secondary organic components are assumed to be photochemically reactive and are logarithmically distributed in volatility bins. The distinction of the volatility properties of aerosols precursors is particularly important for diesel and gasoline emission sources due to their different organic carbon speciation emissions profiles. Using this volatility-basis technique, we will present results on the relative contributions from both gasoline and diesel vehicle fleet emission sources to the formation of secondary organic aerosols in an urban area.

  15. 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...

  16. “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...

  17. Secondary organic aerosol formation and source apportionment in Southeast Texas

    NASA Astrophysics Data System (ADS)

    Zhang, Hongliang; Ying, Qi

    2011-06-01

    The latest version of US EPA's Community Multi-scale Air Quality (CMAQ v4.7) model with the most recent update on secondary organic aerosol (SOA) formation pathways was adapted into a source-oriented modeling framework to determine the contributions of different emission sources to SOA concentrations from a carbon source perspective in Southeast Texas during the 2000 Texas Air Quality Study (TexAQS 2000) from August 25 to September 5, 2000. A comparison of the VOC and SOA predictions with observations shows that anthropogenic emissions of long chain alkanes and aromatics are likely underestimated in the EPA's Clean Air Interstate Rule (CAIR) inventory and the current SOA mechanism in CMAQ still under-predicts SOA. The peak SOA concentrations measured at La Porte are more accurately predicted by increasing the emissions of the anthropogenic SOA precursors by a factor of 5 although the overall precursor concentrations are better predicted by increasing the emissions by a factor of 2. A linear correlation between SOA and odd oxygen (ΔSOA/ΔOx = 23.0-28.4 μg m-3/ppm Ox) can be found when they are formed simultaneously in the air masses passing the urban Houston area on high SOA days. Based on the adjusted emissions (a factor of 2 increase in the alkane and aromatics precursor emissions), approximately 20% of the total SOA in the Houston-Galveston Bay area is due to anthropogenic sources. Solvent utilization and gasoline engines are the main anthropogenic sources. SOA from alkanes and aromatics accounts for approximately 2-4% and 5-9% of total SOA, respectively. The predicted overall anthropogenic SOA concentrations are not sensitive to the half-life time used to calculate the conversion rate of semi-volatile organic compounds to non-volatile oligomers in the particle phase. The main precursors of biogenic SOA are sesquiterpenes, which contribute to approximately 12-35% of total SOA. Monoterpenes contribute to 3-14% and isoprene accounts for approximately 6-9% of the

  18. 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

  19. 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

  20. A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

    NASA Astrophysics Data System (ADS)

    Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.

    2016-11-01

    We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography-mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on

  1. Aerosol black carbon quantification in the central Indo-Gangetic Plain: Seasonal heterogeneity and source apportionment

    NASA Astrophysics Data System (ADS)

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

    2017-03-01

    Two years of aerosol spectral light absorption measurements, using filter based technique, from the central Indo-Gangetic plain (IGP), Gorakhpur (26.75°N, 83.38°E, 85 m amsl), are analyzed to study their seasonal behavior and to quantify their magnitude in terms of absorbing aerosols loading and source speciation. Spectral absorption analysis reveals a four-fold enhancement in absorption in winter (W) and post-monsoon (PoM) seasons at UV wavelengths as compared to IR wavelengths on account of increased biomass burning aerosol contribution to total absorbing aerosol load. Aerosols from the biomass sources contribute 28% during W and PoM seasons as against 16% in pre-monsoon (PM) and monsoon (M) seasons to the total absorbing aerosol content. A Mode shift in the distribution of the Absorption Ångström exponent (α) from 1.3 to 1.6 from PM-M seasons to PoM-W seasons signifies change in source type of absorbing aerosols from fossil fuel to biomass burning and their relative source strength. Due to near stagnant wind conditions combined with shallow boundary layer height, where air masses travelling to the central IGP are confined to a smaller volume, in W and PoM seasons, local sources assume more prominence rather than long-range transport of aerosols. Long-term measurements of aerosols physicochemical and radiative properties from this measurement location will enhance our understanding of the complex aerosol system over the IGP and its climatic implications.

  2. Contaminated aerosol recovery from pulmonary function testing equipment.

    PubMed

    Hiebert, T; Miles, J; Okeson, G C

    1999-02-01

    Clinically, the spread of infectious agents between subjects undergoing spirometry is quite uncommon. There is almost no documentation in the medical literature on this subject. We studied the retrieval of nonpathogenic Escherichia coli after aerosolizing organisms into standard pulmonary function tubing of a type that is frequently used by volume-sensing spirometers. The arrival of the aerosol at the distal end of the tubing was documented by culture. After delays of 0, 1, 5, and 10 min, respectively, air was forcibly withdrawn from the proximal end of the tubing through a special petri plate assembly. The plates were cultured and the colonies were counted. Immediately after insufflation of organisms, air withdrawn from the proximal tubing had counts similar to the air sampled at the distal end. After a 1-min delay, the proximal samples contained only rare organisms. No organisms were recovered from proximal air samples after a delay of 5 or 10 min after insufflation of organisms. The absence of detectable aerosolized E. coli after delays of 5 and 10 min after insufflation of organisms into spirometry tubing supports the hypothesis that a significant transfer of aerosolized organisms does not occur during routine pulmonary function testing as long as an interval of 5 min or more is allowed between tests.

  3. 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.

  4. Chemical composition, main sources and temporal variability of PM1 aerosols in southern African grassland

    NASA Astrophysics Data System (ADS)

    Tiitta, P.; Vakkari, V.; Josipovic, M.; Croteau, P.; Beukes, J. P.; van Zyl, P. G.; Venter, A. D.; Jaars, K.; Pienaar, J. J.; Ng, N. L.; Canagaratna, M. R.; Jayne, J. T.; Kerminen, V.-M.; Kulmala, M.; Laaksonen, A.; Worsnop, D. R.; Laakso, L.

    2013-06-01

    Southern Africa is a significant source region of atmospheric pollution, yet long-term data on pollutant concentrations and properties from this region are rather limited. A recently established atmospheric measurement station in South Africa, Welgegund, is strategically situated to capture regional background emissions, as well as emissions from the major source regions in the interior of South Africa. We measured non-refractive submicron aerosols (NR-PM1) and black carbon over a one year period in Welgegund, and investigated the seasonal and diurnal patterns of aerosol concentration levels, chemical composition, acidity and oxidation level. Based on air mass back trajectories, four distinct source regions were determined for NR-PM1. Supporting data utilized in our analysis included particle number size distributions, aerosol absorption, trace gas concentrations, meteorological variables and the flux of carbon dioxide. The dominant submicron aerosol constituent during the dry season was organic aerosol, reflecting high contribution from savannah fires and other combustion sources. Organic aerosol concentrations were lower during the wet season, presumably due to wet deposition as well as reduced emissions from combustion sources. Sulfate concentrations were usually high and exceeded organic aerosol concentrations when air-masses were transported over regions containing major point sources. Sulfate and nitrate concentrations peaked when air masses passed over the industrial Highveld (iHV) area. In contrast, concentrations were much lower when air masses passed over the cleaner background (BG) areas. Air masses associated with the anti-cyclonic recirculation (ACBIC) source region contained largely aged OA. Positive Matrix Factorization (PMF) analysis of aerosol mass spectra was used to characterize the organic aerosol (OA) properties. The factors identified were oxidized organic aerosols (OOA) and biomass burning organic aerosols (BBOA) in the dry season and low

  5. Sources and composition of submicron organic mass in marine aerosol particles

    DOE PAGES

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; ...

    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

  6. 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

  7. 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...

  8. 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

  9. ATR-FTIR characterization of organic functional groups and inorganic ions in ambient aerosols at a rural site

    NASA Astrophysics Data System (ADS)

    Coury, Charity; Dillner, Ann M.

    An Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) spectroscopic method was used to measure organic functional groups and inorganic ions at Tonto National Monument (TNM), an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampling site in a rural area near Phoenix, Arizona. Functional groups and ions from common aerosol compound classes such as aliphatic and aromatic CH, methylene, methyl, aldehydes/ketones, carboxylic acids, ammonium sulfate and nitrate as well as functional groups from difficult to measure compound classes such as esters/lactones, acid anhydrides, carbohydrate hydroxyl and ethers, amino acids, and amines were quantified. On average, ˜33% of the PM 1.0 mass was composed of organic aerosol. The average (standard deviation) composition of the organic aerosol at TNM was 34% (6%) biogenic functional groups, 21% (5%) oxygenated functional groups, 28% (7%) aliphatic hydrocarbon functional groups (aliphatic CH, methylene and methyl) and 17% (1%) aromatic hydrocarbon functional groups. Compositional analysis, functional group correlations, and back trajectories were used to identify three types of events with source signatures: primary biogenic-influenced, urban-influenced, and regional background. The biogenic-influenced event had high concentrations of amino acids and carbohydrate hydroxyl and ether, as well as aliphatic CH and aromatic CH functional groups and qualitatively high levels of silicate. The urban-influenced events had back trajectories traveling directly from the Phoenix area and high concentrations of hydrocarbons, oxygenated functional groups, and inorganic ions. This aerosol characterization suggests that both primary emissions in Phoenix and secondary formation of aerosols from Phoenix emissions had a major impact on the aerosol composition and concentration at TNM. The regional background source had low concentrations of all functional groups, but had higher concentrations of biogenic functional

  10. Source Strength and Scattering Properties of Organic Marine Aerosols

    DTIC Science & Technology

    1999-09-20

    aerosol LONG-TERM GOAL My long term goal is to quantify the role played by sea salt in radiative scattering in the marine environment. This project studies...the number of aerosol particles produced from sea salt under different marine conditions. Studying the chemical composition of those particles...provides important information about their behavior in the atmosphere. OBJECTIVES I would like to see whether the number of sea salt particles observed in

  11. 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

  12. 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.

  13. 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...

  14. A source of experimental underestimation of aerosol bolus deposition

    NASA Technical Reports Server (NTRS)

    Verbanck, S.; Darquenne, C.; Prisk, G. K.; Vincken, W.; Paiva, M.

    1999-01-01

    We examined the measurement error in inhaled and exhaled aerosol concentration resulting from the bolus delivery system when small volumes of monodisperse aerosols are inspired to different lung depths. A laser photometer that illuminated approximately 75% of the breathing path cross section recorded low inhaled bolus half-widths (42 ml) and negative deposition values for shallow bolus inhalation when the inhalation path of a 60-ml aerosol was straight and unobstructed. We attributed these results to incomplete mixing of the inhaled aerosol bolus over the breathing path cross section, on the basis of simultaneous recordings of the photometer with a particle-counter sampling from either the center or the edge of the breathing path. Inserting a 90 degrees bend into the inhaled bolus path increased the photometer measurement of inhaled bolus half-width to 57 ml and yielded positive deposition values. Dispersion, which is predominantly affected by exhaled bolus half-width, was not significantly altered by the 90 degrees bend. We conclude that aerosol bolus-delivery systems should ensure adequate mixing of the inhaled bolus to avoid error in measurement of bolus deposition.

  15. 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

  16. 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

  17. Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

    PubMed

    Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

    2009-03-01

    During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

  18. 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 presented as a function of aerosol type. In general, the highest f(RH) values were measured in clean marine environments, with pollution having a major influence on f(RH). Dust aerosol tended to have the lowest reported hygroscopicity of any of the aerosol types studied. Major open questions and suggestions for future research priorities are outlined.

  19. 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.

  20. 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

  1. Characteristics, sources and evolution of fine aerosol (PM1) at urban, coastal and forest background sites in Lithuania

    NASA Astrophysics Data System (ADS)

    Masalaite, A.; Holzinger, R.; Remeikis, V.; Röckmann, T.; Dusek, U.

    2017-01-01

    The chemical and isotopic composition of organic aerosol (OA) samples collected on PM1 filters was determined as a function of desorption temperature to investigate the main sources of organic carbon and the effects of photochemical processing on atmospheric aerosol. The filter samples were collected at an urban (54°38‧ N, 25°18‧ E), coastal (55°55‧ N, 21°00‧ E) and forest (55°27‧ N, 26°00' E) site in Lithuania in March 2013. They can be interpreted as winter-time samples because the monthly averaged temperature was -4 °C. The detailed chemical composition of organic compounds was analysed with a thermal desorption PTR-MS. The mass concentration of organic aerosol at the forest site was roughly by a factor of 30 lower than at the urban and coastal site. This fact could be an indication that in this cold month the biogenic secondary organic aerosol (SOA) formation was very low. Moreover, the organic aerosol collected at the forest site was more refractory and contained a larger fraction of heavy molecules with m/z > 200. The isotopic composition of the aerosol was used to differentiate the two main sources of organic aerosol in winter, i.e. biomass burning (BB) and fossil fuel (FF) combustion. Organic aerosol from biomass burning is enriched in 13C compared to OA from fossil fuel emissions. δ13COC values of the OA samples showed a positive correlation with the mass fraction of several individual organic compounds. Most of these organic compounds contained nitrogen indicating that organic nitrogen compounds formed during the combustion of biomass may be indicative of BB. Other compounds that showed negative correlations with δ13COC were possibly indicative of FF. These compounds included heavy hydrocarbons and were on the average less oxidized than the bulk organic carbon. The correlation of δ13COC and the O/C ratio was positive at low but negative at high desorption temperatures at the forest site. We propose that this might be due to

  2. The contribution of different aerosol sources to the Aerosol Optical Depth in Hong Kong

    NASA Astrophysics Data System (ADS)

    Zhang, Zhenxi; Wenig, Mark; Zhou, Wen; Diehl, Thomas; Chan, Ka-Lok; Wang, Lingna

    2014-02-01

    The contribution of major aerosol components emitted from local and remote regions to Hong Kong's Aerosol Optical Depth (AOD) in 2007 is quantitatively determined using the chemical transport model GOCART (Global Ozone Chemistry Aerosol Radiation and Transport). Of the major aerosol components, sulphur has the largest influence (68%) on Hong Kong, followed by organic carbon (OC, 13%) and dust (11%), and the influences of black carbon (BC, 5%) and sea salt (3%) are the lowest. The highest AOD is seen in September 2007 and is composed mainly of sulphur aerosols (85%). The high AOD values in March and April 2007 are caused by sulphur and OC. OC has a relative contribution of 39% in March and 30% in April. The anthropogenic sulphur, BC, and OC emitted from every continent, as well as from China and South China, are considered respectively. In summer, South China's contribution of sulphur aerosols from anthropogenic SO2 emissions to the total sulphur AOD in Hong Kong is more than 20%. In other seasons, sulphur aerosols from anthropogenic SO2 emissions in Rest China (all of China except South China) accounts for more than 25%. Anthropogenic BC from South China accounts for more than 20% of total BC AOD in Hong Kong in summer. The contribution of anthropogenic BC from Rest China exceeds 40% in autumn and winter. Anthropogenic BC from Rest Asia (all of Asia except China) accounts for more than 30% in summer and autumn. The contribution of anthropogenic OC from Rest China is more than 35% in autumn and winter. The contribution of anthropogenic OC from Rest Asia exceeds 20% in summer. Gobi dust accounts for more than 40% of the total dust AOD in winter, and its impact appears mainly in the Atmospheric Boundary Layer (ABL), where it is responsible for 50% of the dust concentration. The contribution of Sahara dust to the dust AOD in spring exceeds 35%, and its contribution to the dust concentration in the free atmosphere (40%) is larger than that in the ABL (10%). More than 35

  3. Organic aerosol sources an partitioning in CMAQv5.2

    EPA Science Inventory

    We describe a major CMAQ update, available in version 5.2, which explicitly treats the semivolatile mass transfer of primary organic aerosol compounds, in agreement with available field and laboratory observations. Until this model release, CMAQ has considered these compounds to ...

  4. 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.

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

    SciTech Connect

    Mazurek, M.A. ); Hildemann, L.M. . Dept. of Civil Engineering); Cass, G.R.; Rogge, W.F. . Dept. of Environmental Engineering Science); Simoneit, B.R.T. . Coll. of Oceanography)

    1990-04-01

    Extractable organic compounds having between 6 to 40 carbon atoms comprise an important mass fraction of the fine particulate matter samples from major urban emission sources. Depending on the emission source type, this solvent-soluble fraction accounts for <20% to 100% of the total organic aerosol mass, as measured by quantitative high-resolution has chromatography (HRGC) with flame ionization detection. In addition to total extract quantitation, HRGC can be applied to further analyses of the mass distributions of elutable organics present in the complex aerosol extract mixtures, thus generating profiles that serve as fingerprints'' for the sources of interest. This HRGC analytical method is applied to emission source samples that contain between 7 to 12,000 {mu}g/filter organic carbon. It is shown to be a sensitive technique for analysis of carbonaceous aerosol extract mixtures having diverse mass loadings and species distributions. This study describes the analytical chemical methods that have been applied to: the construction of chemical mass balances based on the mass of fine organic aerosol emitted for major urban sources of particulate carbon; and the generation of discrete emission source chemical profiles derived from chromatographic characteristics of the organic aerosol components. 21 refs., 1 fig., 2 tabs.

  6. 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.

  7. 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.

  8. Sources and characteristics of sub-micron aerosols in the San Joaquin Valley, CA

    NASA Astrophysics Data System (ADS)

    Bahreini, R.; Middlebrook, A. M.; Brioude, J.; Brock, C. A.; de Gouw, J. A.; Hall, K.; Holloway, J. S.; Neuman, J.; Nowak, J. B.; Pollack, I. B.; Ryerson, T. B.; Warneke, C.; Parrish, D. D.

    2010-12-01

    The NOAA WP-3D aircraft performed several flights in the San Joaquin Valley (SJV), California during the CalNex-2010 (California Research at the Nexus of Air Quality and Climate Change) field project in May-June 2010. SJV is generally a rural valley, with a high concentration of feedlots and agricultural sites as well as urbanized centers such as Fresno and Bakersfield. Preliminary results on size-resolved chemical composition of sub-micron aerosols measured using a compact time-of-flight aerosol mass spectrometer, measurements of trace gases affecting secondary production of aerosols, and FLEXPART back trajectory analyses are presented in order to identify sources of aerosols transported to or produced in the valley. Observed enhancements in various trace gases and aerosol species indicate a mixed influence from urban, industrial, and animal feedlots in the SJV. Three distinct observations suggest a complex transport pattern of pollutants with different origins to and within the valley: 1) CO and NOx mixing ratios were prominent downwind of the urban areas in the valley; 2) SO2, aerosol organics and sulfate were higher closer to the foothills of the Sierra Nevada Mountains on the east of the valley; 3) high concentration of aerosol phase ammonium and nitrate were observed in NH3-rich air masses, directly downwind of the feedlots in the central part of the valley. Aerosol enhancements in each of these air mass categories relative to the background determine the relative contribution and significance of different sources to aerosol loadings in the valley. Differences in VOC measurements and meteorology will be explored to investigate the observed variation in characteristics of organics on different days.

  9. 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...

  10. Comparison of sources and nature of the tropical aerosol with the summer high Arctic aerosol

    NASA Astrophysics Data System (ADS)

    Leck, Caroline; Bigg, E. Keith

    2008-02-01

    Marine aerosol was collected in September 1998 and July 2005 on the upwind coast of an island at latitude 15°S, about 15 km downwind from the outer edge of the Great Barrier Reef, Australia, and examined by electron microscopy. Exopolymer gels, aggregates of organic particles, marine micro-organisms and fragments of marine life formed a substantial part of the accumulation mode aerosol. Differences in transparency, firmness of outlines and shape of gels and the influence of organic vapours on them, suggested progressive physical and chemical changes with atmospheric residence time. The organic aggregate components had a size distribution remarkably close to that found in similar particles over the central Arctic Ocean peaking at diameters of 30-40 nm. Single components or small groups of these aggregates were found within at least 75% of particles resembling ammonium sulphate in appearance, indicating that aggregates fragmented in the atmosphere. Sea salt was not detected in particles <200 nm diameter unlike many observations showing it to be a major component, a result that was entirely consistent with the Arctic findings. The deduced sequence of changes to particles entering the atmosphere from the ocean is also very similar to that found in the Arctic, suggesting that it is a common pattern over the oceans. That conclusion would require modification of the parametrization of the marine aerosol used in climate models and of possible climate feedback effects.

  11. 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

  12. Evaluating the impact of improvements to the FLAMBE smoke source model on forecasts of aerosol distribution from NAAPS

    NASA Astrophysics Data System (ADS)

    Hyer, E. J.; Reid, J. S.

    2006-12-01

    As more forecast models aim to include aerosol and chemical species, there is a need for source functions for biomass burning emissions that are accurate, robust, and operable in real-time. NAAPS is a global aerosol forecast model running every six hours and forecasting distributions of biomass burning, industrial sulfate, dust, and sea salt aerosols. This model is run operationally by the U.S. Navy as an aid to planning. The smoke emissions used as input to the model are calculated from the data collected by the FLAMBE system, driven by near-real-time active fire data from GOES WF_ABBA and MODIS Rapid Response. The smoke source function uses land cover data to predict properties of detected fires based on literature data from experimental burns. This scheme is very sensitive to the choice of land cover data sets. In areas of rapid land cover change, the use of static land cover data can produce artifactual changes in emissions unrelated to real changes in fire patterns. In South America, this change may be as large as 40% over five years. We demonstrate the impact of a modified land cover scheme on FLAMBE emissions and NAAPS forecasts, including a fire size algorithm developed using MODIS burned area data. We also describe the effects of corrections to emissions estimates for cloud and satellite coverage. We outline areas where existing data sources are incomplete and improvements are required to achieve accurate modeling of biomass burning emissions in real time.

  13. 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 Astrophysics Data System (ADS)

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

    2013-09-01

    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 savannah at Mongu (Zambia), with average SSA ∼0.85 in the midvisible. These can serve as candidate sets of aerosol microphysical/optical 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.

  14. 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.

  15. 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

  16. 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

  17. Atmospheric acidification of mineral aerosols: a source of bioavailable phosphorus for the oceans

    NASA Astrophysics Data System (ADS)

    Nenes, A.; Krom, M. D.; Mihalopoulos, N.; van Cappellen, P.; Shi, Z.; Bougiatioti, A.; Zarmpas, P.; Herut, B.

    2011-07-01

    Primary productivity of continental and marine ecosystems is often limited or co-limited by phosphorus. Deposition of atmospheric aerosols provides the major external source of phosphorus to marine surface waters. However, only a fraction of deposited aerosol phosphorus is water soluble and available for uptake by phytoplankton. We propose that atmospheric acidification of aerosols is a prime mechanism producing soluble phosphorus from soil-derived minerals. Acid mobilization is expected to be pronounced where polluted and dust-laden air masses mix. Our hypothesis is supported by the soluble compositions and reconstructed pH values for atmospheric particulate matter samples collected over a 5-yr period at Finokalia, Crete. In addition, at least tenfold increase in soluble phosphorus was observed when Saharan soil and dust were acidified in laboratory experiments which simulate atmospheric conditions. Aerosol acidification links bioavailable phosphorus supply to anthropogenic and natural acidic gas emissions, and may be a key regulator of ocean biogeochemistry.

  18. Atmospheric acidification of mineral aerosols: a source of bioavailable phosphorus for the oceans

    NASA Astrophysics Data System (ADS)

    Nenes, A.; Krom, M. D.; Mihalopoulos, N.; van Cappellen, P.; Shi, Z.; Bougiatioti, A.; Zarmpas, P.; Herut, B.

    2011-02-01

    Primary productivity of continental and marine ecosystems is often limited or co-limited by phosphorus. Deposition of atmospheric aerosols provides the major external source of phosphorus to surface waters. However, only a fraction of deposited aerosol phosphorus is water soluble and available for uptake by phytoplankton. We propose that atmospheric acidification of aerosols is a prime mechanism producing soluble phosphorus from soil-derived minerals. Acid mobilization is expected to be pronounced where polluted and dust-laden air masses mix. Our hypothesis is supported by the soluble compositions and reconstructed pH values for atmospheric particulate matter samples collected over a 5-year period at Finokalia, Crete. At least tenfold increase in soluble phosphorus is observed when Saharan soil and dust were acidified in laboratory experiments which simulate atmospheric conditions. Aerosol acidification links bioavailable phosphorus supply to anthropogenic and natural acidic gas emissions, and may be a key regulator of ocean biogeochemistry.

  19. A comparison of summertime secondary organic aerosol source contributions at contrasting urban locations.

    PubMed

    Stone, Elizabeth A; Zhou, Jiabin; Snyder, David C; Rutter, Andrew P; Mieritz, Mark; Schauer, James J

    2009-05-15

    Primary and secondary sources contributing to atmospheric organic aerosol during the months of July and August were quantitatively assessed in three North American urban areas: Cleveland, Ohio, and Detroit, Michigan, in the Midwest region and Riverside, California, in the Los Angeles Air Basin. Organic molecular marker species unique to primary aerosol sources and secondarytracers derived from isoprene, alpha-pinene, beta-caryophyllene, and toluene were measured using gas chromatography-mass spectrometry. Source contributions from motor vehicles, biomass burning, vegetative detritus, and secondary organic aerosol (SOA) were estimated using chemical mass balance (CMB) modeling. In Cleveland, primary sources accounted for 37 +/- 2% of ambient organic carbon, measured biogenic and anthropogenic secondary sources contributed 46 +/- 6%, and other unknown sources contributed 17 +/- 4%. Similarly, Detroit aerosol was determined to be 44 +/- 5% primary and 37 +/- 3% secondary, while 19 +/- 7% was unaccounted for by measured sources. In Riverside, 21 +/- 3% of organic carbon came from primary sources, 26 +/- 5% was attributed to measured secondary sources, and 53 +/- 3% came from other sources that were expected to be secondary in nature. The comparison of samples across these two regions demonstrated that summertime SOA in the Midwestern United States was substantially different from the summertime SOA in the Los Angeles Air Basin and indicated the need to exert caution when generalizing about the sources and nature of SOA across different urban areas. Furthermore, the results of this study suggestthatthe contemporary understanding of SOA sources and formation mechanisms is satisfactory to explainthe majority of SOA in the Midwest Additional SOA sources and mechanisms of formation are needed to explain the majority of SOA in the Los Angeles Air Basin.

  20. 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

  1. 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

  2. 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

  3. 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

  4. 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.

  5. Speciation and water soluble fraction of iron in aerosols from various sources

    NASA Astrophysics Data System (ADS)

    Takahashi, Y.; Kurisu, M.; Uematsu, M.

    2015-12-01

    Iron (Fe) is an essential micronutrient and has been identified as a limiting factor for phytoplankton growth in high-nitrate low-chlorophyll (HNLC) regions of the ocean. In the North Pacific, three sources of iron (Fe) transported via. atmosphere can be suggested: (i) mineral dust from East Asia, (ii) anthropogenic Fe, and (iii) aerosols from volcanic origin. Considering these different sources, Fe can be found and transported in a variety of chemical forms, both water-soluble and -insoluble. It is generally believed that only the soluble fraction of Fe can be considered as bioavailable for phytoplankton. To assess the biogeochemical impact of the atmospheric input, attempt was made to determine Fe species by X-ray absorption spectroscopy (XAS) and its water solubility, in particular to compare the three sources. Iron species, chemical composition, and soluble Fe concentration in aerosol collected at Tsukuba (Japan) through a year were investigated to compare the contributions of mineral dust and anthropogenic components. It was found that the concentration of soluble Fe in aerosol is correlated with those of sulfate and oxalate which originate from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. XAS analysis showed that main Fe species in aerosols in Tsukuba were illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, soluble Fe fraction is closely correlated with that of Fe(III) sulfate. In spite of supply of high concentrations of Fe in mineral dust from East Asia, it was found that anthropogenic fraction is important due to its high water solubility by the presence of Fe(III) sulfate. Marine aerosol samples originated from volcanic ash were collected in the western North Pacific during KH-08-2 cruise (August, 2008). XAS analysis suggested that Fe species of volcanic ashes changed during the long-range transport, while dissolution experiment showed that Fe solubility of the marine aerosol is larger than

  6. 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

  7. Retrieving Aerosol in a Cloudy Environment: Aerosol Availability as a Function of Spatial and Temporal Resolution

    NASA Technical Reports Server (NTRS)

    Remer, Lorraine A.; Mattoo, Shana; Levy, Robert C.; Heidinger, Andrew; Pierce, R. Bradley; Chin, Mian

    2011-01-01

    The challenge of using satellite observations to retrieve aerosol properties in a cloudy environment is to prevent contamination of the aerosol signal from clouds, while maintaining sufficient aerosol product yield to satisfy specific applications. We investigate aerosol retrieval availability at different instrument pixel resolutions, using the standard MODIS aerosol cloud mask applied to MODIS data and a new GOES-R cloud mask applied to GOES data for a domain covering North America and surrounding oceans. Aerosol availability is not the same as the cloud free fraction and takes into account the technqiues used in the MODIS algorithm to avoid clouds, reduce noise and maintain sufficient numbers of aerosol retrievals. The inherent spatial resolution of each instrument, 0.5x0.5 km for MODIS and 1x1 km for GOES, is systematically degraded to 1x1 km, 2x2 km, 4x4 km and 8x8 km resolutions and then analyzed as to how that degradation would affect the availability of an aerosol retrieval, assuming an aerosol product resolution at 8x8 km. The results show that as pixel size increases, availability decreases until at 8x8 km 70% to 85% of the retrievals available at 0.5 km have been lost. The diurnal pattern of aerosol retrieval availability examined for one day in the summer suggests that coarse resolution sensors (i.e., 4x4 km or 8x8 km) may be able to retrieve aerosol early in the morning that would otherwise be missed at the time of current polar orbiting satellites, but not the diurnal aerosol properties due to cloud cover developed during the day. In contrast finer resolution sensors (i.e., 1x1 km or 2x2 km) have much better opportunity to retrieve aerosols in the partly cloudy scenes and better chance of returning the diurnal aerosol properties. Large differences in the results of the two cloud masks designed for MODIS aerosol and GOES cloud products strongly reinforce that cloud masks must be developed with specific purposes in mind and that a generic cloud mask

  8. 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.

  9. Source attribution of climatically important aerosol properties measured at Paposo (Chile) during VOCALS

    NASA Astrophysics Data System (ADS)

    Chand, D.; Hegg, D. A.; Wood, R.; Shaw, G. E.; Wallace, D.; Covert, D. S.

    2010-11-01

    Measurements of submicron aerosol composition, light scattering, and size distribution were made from 17 October to 15 November 2008 at the elevated Paposo site (25° 0.4' S, 70° 27.01' W, 690 m a.s.l.) on the Chilean coast as part of the VOCALS* Regional Experiment (REx). Based on the chemical composition measurements, a receptor modeling analysis using Positive Matrix Factorization (PMF) was carried out, yielding four broad source categories of the aerosol mass, light scattering coefficient, and a proxy for cloud condensation nucleus (CCN) concentration at 0.4% supersaturation derived from the size distribution measurements assuming an observed soluble mass fraction of 0.53. The sources resolved were biomass burning, marine, an urban-biofuels mix and a somewhat ambiguous mix of smelter emissions and mineral dust. The urban-biofuels mix is the most dominant aerosol mass component (52%) followed by biomass burning (25%), smelter/soil dust (12%) and marine (9%) sources. The average (mean±std) submicron aerosol mass concentration, aerosol light scattering coefficient and proxy CCN concentration were, 8.77±5.40 μg m-3, 21.9±11.0 Mm-1 and 548±210 cm-3, respectively. Sulfate is the dominant identified submicron species constituting roughly 40% of the dry mass (3.64±2.30 μg m-3), although the indentified soluble species constitute only 53% of the mass. Much of the unidentified mass is likely organic in nature. The relative importance of each aerosol source category is different depending upon whether mass, light scattering, or CCN concentration is being considered, indicating that the mean size of aerosols associated with each source are different. Marine aerosols do not appear to contribute to more than 10% to either mass, light scattering, or CCN concentration at this site. Back trajectory cluster analysis proved consistent with the PMF source attribution. *VOCALS: VAMOS** Ocean-Cloud-Atmosphere-Land Study (VOCALS) **VAMOS: Variability of American Monsoon

  10. Source attribution of climatically important aerosol properties measured at Paposo (Chile) during VOCALS

    NASA Astrophysics Data System (ADS)

    Chand, D.; Hegg, D. A.; Wood, R.; Shaw, G. E.; Wallace, D.; Covert, D. S.

    2010-07-01

    Measurements of submicron aerosol composition, light scattering, and size distribution were made from 17 October to 15 November 2008 at the elevated Paposo site (25° 0.4' S, 70°27.01' W, 690 m a.s.l.) on the Chilean coast as part of the VOCALS1 Regional Experiment (REx). Based on the chemical composition measurements, a receptor modeling analysis using Positive Matrix Factorization (PMF) was carried out, yielding four broad source categories of the aerosol mass, light scattering coefficient, and a proxy for cloud condensation nucleus (CCN) concentration at 0.4% supersaturation derived from the size distribution measurements assuming an observed soluble mass fraction of 0.53. The sources resolved were biomass burning, marine, an urban-biofuels mix and a somewhat ambiguous mix of smelter emissions and mineral dust. The urban-biofuels mix is the most dominant aerosol mass component (52%) followed by biomass burning (25%), smelter/soil dust (12%) and marine (9%) sources. The average (mean±std) submicron aerosol mass concentration, aerosol light scattering coefficient and proxy CCN concentration were, 8.77±5.40 μg m-3, 21.9±11.0 Mm-1 and 548±210 cm-3, respectively. Sulfate is the dominant identified submicron species constituting roughly 40% of the dry mass (3.64±2.30 μg m-3, although the indentified soluble species constitute only 53% of the mass. Much of the unidentified mass is likely organic in nature. The relative importance of each aerosol source category is different depending upon whether mass, light scattering, or CCN concentration is being considered, indicating that the mean size of aerosols associated with each source are different. Marine aerosols do not appear to contribute to more than 10% to either mass, light scattering, or CCN concentration at this site. Back trajectory cluster analysis proved consistent with the PMF source attribution. 1 VOCALS: VAMOS Ocean-Cloud-Atmosphere-Land Study (VOCALS)VAMOS: Variability of American Monsoon System

  11. 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

  12. 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

  13. 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%.

  14. 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.

  15. 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

    countries). Secondary organic aerosol carbon formed by the photo-oxidation of biogenic emissions mainly from Germany, seems to be predominant in this season. This seasonal cycle is mainly driven by the winter/summer contrast of the regional-scale vertical mixing. During the warm season the vertical air mass exchange is enhanced by a more efficient upward transport from the boundary layer to the mountain sites. During the winter months, the vertical mixing intensity is reduced. In this season the mean levels obtained for OC and EC were lower than those recorded during the summer. Their spatiotemporal variability was mainly governed by air mass transport from distant regions, especially from Eastern Europe regions, where significant amounts of fossil fuels and biomass are currently consumed. Furthermore, emissions from desert regions in North Africa seemed to significantly influence the central European background mineral aerosol concentrations throughout the year. References: Pio C. A., M. Legrand, T. Oliveira, J. Afonso, C. Santos, A. Caseiro, P. Fialho, F. Barata, H. Puxbaum, A. Sanchez-Ochoa, A. Kasper-Giebl, A. Gelencsér, S. Preunkert, and M. Schock (2007), Climatology of aerosol composition (organic versus inorganic) at nonurban sites on a west-east transect across Europe. J. Geophys. Res., 112, D23S02, doi:10.1029/2006JD008038. Stohl A., G. Wotawa, P. Seibert and H. Kromp-Kolb (1995), Interpolation errors in wind fields as a function of spatial and temporal resolution and their impact on different types of kinematic trajectories. J. Appl. Meteorol., 34, 2149-2165. Stohl A. (1996), Trajectory statistics-a new method to establish source-receptor relationships of air pollutants and its application to the transport of particulate sulfate in Europe. Atmos. Environ., 30(4), 579-587.

  16. Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

    NASA Technical Reports Server (NTRS)

    Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E. (Editor); Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

    1994-01-01

    Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate

  17. Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

    NASA Astrophysics Data System (ADS)

    Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E.; Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

    1994-05-01

    Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120°, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20%±15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law size distribution, based on the spectral dependence of the optical thickness, a, cannot estimate accurately the phase function (up to 50% error for λ = 0.87 μm). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with α. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distributions before the injection of stratospheric aerosol consistently show two modes, sulfate particles with rm

  18. Anthropogenic aerosols as a source of ancient dissolved organic matter in glaciers

    USGS Publications Warehouse

    Stubbins, Aron; Hood, Eran; Raymond, Peter A.; Aiken, George R.; Sleighter, Rachel L.; Hernes, Peter J.; Butman, David; Hatcher, Patrick G.; Striegl, Rob; Schuster, Paul F.; Abdulla, Hussain A.N.; Vermilyea, Andrew W.; Scott, Durelle T.; Spencer, Robert G.M.

    2012-01-01

    Glacier-derived dissolved organic matter represents a quantitatively significant source of ancient, yet highly bioavailable carbon to downstream ecosystems. This finding runs counter to logical perceptions of age–reactivity relationships, in which the least reactive material withstands degradation the longest and is therefore the oldest. The remnants of ancient peatlands and forests overrun by glaciers have been invoked as the source of this organic matter. Here, we examine the radiocarbon age and chemical composition of dissolved organic matter in snow, glacier surface water, ice and glacier outflow samples from Alaska to determine the origin of the organic matter. Low levels of compounds derived from vascular plants indicate that the organic matter does not originate from forests or peatlands. Instead, we show that the organic matter on the surface of the glaciers is radiocarbon depleted, consistent with an anthropogenic aerosol source. Fluorescence spectrophotometry measurements reveal the presence of protein-like compounds of microbial or aerosol origin. In addition, ultrahigh-resolution mass spectrometry measurements document the presence of combustion products found in anthropogenic aerosols. Based on the presence of these compounds, we suggest that aerosols derived from fossil fuel burning are a source of pre-aged organic matter to glacier surfaces. Furthermore, we show that the molecular signature of the organic matter is conserved in snow, glacier water and outflow, suggesting that the anthropogenic carbon is exported relatively unchanged in glacier outflows.

  19. Contributions and source identification of biogenic and anthropogenic hydrocarbons to secondary organic aerosols at Mt. Tai in 2014.

    PubMed

    Zhu, Yanhong; Yang, Lingxiao; Kawamura, Kimitaka; Chen, Jianmin; Ono, Kaori; Wang, Xinfeng; Xue, Likun; Wang, Wenxing

    2017-01-01

    Ambient fine particulate matter (PM2.5) and volatile organic compounds (VOCs) collected at Mt. Tai in summer 2014 were analysed and the data were used to identify the contribution of biogenic and anthropogenic hydrocarbons to secondary organic aerosols (SOA) and their sources and potential source areas in high mountain regions. Compared with those in 2006, the 2014 anthropogenic SOA tracers in PM2.5 aerosols and VOC species related to vehicular emissions exhibited higher concentrations, whereas the levels of biogenic SOA tracers were lower, possibly due to decreased biomass burning. Using the SOA tracer and parameterisation method, we estimated the contributions from biogenic and anthropogenic VOCs, respectively. The results showed that the average concentration of biogenic SOA was 1.08 ± 0.51 μg m(-3), among which isoprene SOA tracers were dominant. The anthropogenic VOC-derived SOA were 7.03 ± 1.21 μg m(-3) and 1.92 ± 1.34 μg m(-3) under low- and high-NOx conditions, respectively, and aromatics made the greatest contribution. However, the sum of biogenic and anthropogenic SOA only contributed 18.1-49.1% of the total SOA. Source apportionment by positive matrix factorisation (PMF) revealed that secondary oxidation and biomass burning were the major sources of biogenic SOA tracers. Anthropogenic aromatics mainly came from solvent use, fuel and plastics combustion and vehicular emissions. However, for > C6 alkanes and cycloalkanes, vehicular emissions and fuel and plastics combustion were the most important contributors. The potential source contribution function (PSCF) identified the Bohai Sea Region (BSR) as the major source area for organic aerosol compounds and VOC species at Mt. Tai.

  20. 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

  1. Sea Salt Source Function over the Baltic Sea

    NASA Astrophysics Data System (ADS)

    Petelski, Tomasz; Makuch, Przemyslaw; Markuszewski, Piotr; Jankowski, Andrzej; Zieliński, Tymon

    2013-04-01

    Studies of production and transport of aerosol over the sea are very important for many areas of knowledge. Marine aerosol emitted from the sea surface helps to clean the boundary layer from other aerosol particles. The emitted droplets do not dry out in the highly humid surface layer air and because of their sizes most of them are deposited quickly at the sea surface. Therefore, marine aerosol has many features of rain i.e. the deposition in the marine boundary layer in high wind events is controlled not only by the "dry" processes but also by the "wet" scavenging. While many cruises conducted on board S/Y Oceania, we collected many data which were used to calculate sea salt source function over the Baltic Sea. Our cruises held between 2009 and 2012. Measurements were carried out using gradient method. For this method we used Laser Particle Counter (PMS model CSASP-100_HV) placed on one oft the mast of S/Y Oceania. Measurements were performed on five different levels around sea level: 8, 11, 14, 17 and 20 meters. Based on the averaged vertical concentration, profiles were calculated, using Monin-Obuchow theory, vertical sea spray fluxes in the near water layer. Based on fluxes calculated from vertical concentration profiles was calculated sea salt source function over the Baltic Sea. This function gives emission for different particle size, depending on environmental parameters. Emission of sea spray depends of the size of energy lost by the wind waves in process of collapse. Acknowledgements: The support for this study was provided by the project Satellite Monitoring of the Baltic Sea Environment - SatBałtyk founded by European Union through European Regional Development Fund contract No. POIG 01.01.02-22-011/09.

  2. Relevance of aerosol size spectrum analysis as support to qualitative source apportionment studies.

    PubMed

    Manigrasso, M; Febo, A; Guglielmi, F; Ciambottini, V; Avino, P

    2012-11-01

    This work presents a diagnostic methodology in support to source apportionment studies to identify remote and local pollution sources. It is based on the temporal analysis of both PM size distributions and PM size fraction correlation along with natural radioactivity measurements as index of Planetary Boundary Layer dynamic. A correlation drop is indicative of changing aerosol sources. When this observation is coupled with decreasing level of natural radioactivity and increasing aerosol concentration, be it coarse or fine, it is indicative of the inflow of remote polluted air masses. The methodology defines in which size range operates the contribution of remote pollution sources. It was applied to two PM10 pollution episodes: the first involved the advection of coarse PM, the second entailed the inflow of two air masses, one transporting coarse dust and the other fine PM. Dust models and backward trajectories analysis confirmed such results, indicating the air mass provenience.

  3. Atmospheric aerosols in Rome, Italy: sources, dynamics and spatial variations during two seasons

    NASA Astrophysics Data System (ADS)

    Struckmeier, Caroline; Drewnick, Frank; Fachinger, Friederike; Gobbi, Gian Paolo; Borrmann, Stephan

    2016-12-01

    Investigations on atmospheric aerosols and their sources were carried out in October/November 2013 and May/June 2014 consecutively in a suburban area of Rome (Tor Vergata) and in central Rome (near St Peter's Basilica). During both years a Saharan dust advection event temporarily increased PM10 concentrations at ground level by about 12-17 µg m-3. Generally, in October/November the ambient aerosol was more strongly influenced by primary emissions, whereas higher relative contributions of secondary particles (sulfate, aged organic aerosol) were found in May/June. Absolute concentrations of anthropogenic emission tracers (e.g. NOx, CO2, particulate polycyclic aromatic hydrocarbons, traffic-related organic aerosol) were generally higher at the urban location. Positive matrix factorization was applied to the PM1 organic aerosol (OA) fraction of aerosol mass spectrometer (HR-ToF-AMS) data to identify different sources of primary OA (POA): traffic, cooking, biomass burning and (local) cigarette smoking. While biomass burning OA was only found at the suburban site, where it accounted for the major fraction of POA (18-24 % of total OA), traffic and cooking were more dominant sources at the urban site. A particle type associated with cigarette smoke emissions, which is associated with a potential characteristic marker peak (m/z 84, C5H10N+, a nicotine fragment) in the mass spectrum, was only found in central Rome, where it was emitted in close vicinity to the measurement location. Regarding secondary OA, in October/November, only a very aged, regionally advected oxygenated OA was found, which contributed 42-53 % to the total OA. In May/June total oxygenated OA accounted for 56-76 % of the OA. Here a fraction (18-26 % of total OA) of a fresher, less oxygenated OA of more local origin was also observed. New particle formation events were identified from measured particle number concentrations and size distributions in May/June 2014 at both sites. While they were observed

  4. 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.

  5. Seasonal variations and sources of various elements in the atmospheric aerosols in Qingdao, China

    NASA Astrophysics Data System (ADS)

    Hao, Yunchao; Guo, Zhigang; Yang, Zuosheng; Fang, Ming; Feng, Jialiang

    2007-07-01

    Seasonal variations and sources of various elements in the atmospheric aerosols of the North China coast were investigated by analyzing aerosol samples collected in Qingdao, China. 23 total suspended particulate (TSP) samples were collected from June 2001 to May 2002, including three samples gathered during Asian dust episodes (20 March and 7-8 April 2002). The concentrations of ten elements including iron (Fe), titanium (Ti), manganese (Mn), vanadium (V), nickel (Ni), copper (Cu), lead (Pb), zinc (Zn), cadmium (Cd) and sulfur (S) were measured by 3000 ICP-OES. All elements measured in the aerosols of Qingdao displayed a strong seasonal variation: the concentrations of Fe, Ti, Mn, V, Ni, Cu, Pb, Zn, Cd were the lowest in summer, and the highest in winter. During the Asian dust episodes, the concentrations of Fe, Ti, Mn, V, Ni, Cu increased remarkably. The concentrations of Pb, Zn, Cu, S also increased greatly during the Asian dust episodes, but they were still lower than those in winter. The enrichment factors (EFs) of all elements (with reference to crustal Fe) indicate that Ti and Mn are mainly from soil sources. V in the Qingdao aerosols is mainly derived from the soil, with a minor contribution from ship emissions. The anthropogenic sources have a relatively higher contribution to Ni and Cu compared with Fe, Ti, and Mn. The S, Pb, Zn and Cd are mainly from anthropogenic sources even during Asian dust episodes. Principal component analysis (PCA), and cluster analysis (CA) indicated that the natural sources contributed about 60% to the sum of measured elements in all samples and anthropogenic sources contributed about 30%, and these elements can be classified into three categories as follow: Fe, Ti, Mn, V, and Ni represent the soil source factor; Cu represents the factor of mixed sources of soil and pollution; and Pb, Zn, Cd and S represents the pollution factor.

  6. Composition and major sources of organic compounds in urban aerosols

    NASA Astrophysics Data System (ADS)

    Bi, Xinhui; Simoneit, Bernd R. T.; Sheng, Guoying; Ma, Shexia; Fu, Jiamo

    Total suspended particles (TSP), collected during June 2002 to July 2003 in Guangzhou, a typical economically developed city in South China, were analyzed for the organic compound compositions using gas chromatography-mass spectrometry (GC/MS). Over 140 organic compounds were detected in the aerosols and grouped into different classes including n-alkanes, hopanoids, polycyclic aromatic hydrocarbons, alkanols, fatty acids, dicarboxylic acids excluding oxalic acid, polyols/polyacids, lignin products, phytosterols, phthalates and water-soluble sugars. The total amounts of the identified organic compounds including unresolved complex mixture (UCM) ranged from 3112 ng/m 3 in spring to 5116 ng/m 3 in winter, comprising on seasonal average 2.8% of TSP. Primary organic compounds peaked in winter although there are no heating systems burning fuels in Guangzhou. The highest saccharide levels occurred in fall due to agricultural activities. This study demonstrated that utilization of fossil fuels, biomass burning, soil resuspension and plastic/refuse burning are the major contributors to the identified organic compounds in the urban atmosphere of South China.

  7. Sources and Distributions of Secondary Aerosols over the Northeastern United States during the WINTER Aircraft Campaign.

    NASA Astrophysics Data System (ADS)

    Shah, V.; Jaegle, L.; Haskins, J.; Campuzano Jost, P.; Schroder, J. C.; Jimenez, J. L.; Sullivan, A.; Weber, R. J.; Dibb, J. E.; Green, J. R.; Fiddler, M. N.; Bililign, S.; Lopez-Hilfiker, F.; Lee, B. H.; Veres, P. R.; Thornton, J. A.

    2015-12-01

    Atmospheric aerosols harm public health, reduce visibility, and alter the Earth's climate. A significant fraction of the aerosol burden is composed of secondary aerosols formed from gas-phase precursors such as SO2, NOx, NH3, and VOC's. The formation and composition of secondary aerosols depends on precursor abundance, oxidant availability, and the thermodynamic properties of the semi-volatile species. The oxidation and thermodynamic processes are strongly dependent on the available sunlight, temperature, and humidity, and produce large seasonal shifts in the aerosol characteristics. While most previous aircraft campaigns have studied these processes during summer, the Wintertime INvestigation of Transport, Emissions, and Reactivity (WINTER) campaign focuses on the wintertime chemical processes over the northeastern United States. A comprehensive dataset of gas- and particle-phase species was collected during the campaign using the NSF/NCAR C-130 aircraft in February-March 2015. We interpret these observations using the GEOS-Chem chemical transport model with a 1/4 degree latitude by 5/16 degree longitude nested-grid over North America. We present a comparison of the model results with the aircraft measurements, and examine the sources of secondary inorganic and organic aerosols observed during the campaign. We use the model results to investigate the consistency between the aircraft, surface and satellite observations of aerosol concentrations and optical depths. Furthermore, we use multi-year model simulations to understand the effect of the unusually cold weather in 2015 over the northeastern United States on the chemical environment observed during the campaign.

  8. Size-resolved trace metal characterization of aerosols emitted by four important source types in Switzerland

    NASA Astrophysics Data System (ADS)

    Buerki, Peter R.; Gaelli, Brigitte C.; Nyffeler, Urs P.

    In central Switzerland five types of emission sources are mainly responsible for airborne trace metals: traffic, industrial plants burning heavy oil, resuspension of soil particles, residential heatings and refuse incineration plants. The particulate emissions of each of these source types except refuse incineration were sampled using Berner impactors and the mass and elemental size distributions of Cd, Cu, Mn, Pb, Zn, As and Na determined. Cd, Na and Zn are not characteristic for any of these source types. As and Cu, occurring in the fine particle fractions are characteristic for heavy oil combustion, Mn for soil dust and sometimes for heavy and fuel oil combustion and Pb for traffic aerosols. The mass size distributions of aerosols originating from erosion and abrasion processes show a maximum mass fraction in the coarse particle range larger than about 1 μm aerodynamic equivalent diameters (A.E.D.). Aerosols originating from combustion processes show a second maximum mass fraction in the fine particle range below about 0.5μm A.E.D. Scanning electron microscopy combined with an EDS analyzer was used for the morphological characterization of emission and ambient aerosols.

  9. 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

  10. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

    PubMed Central

    Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; He, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang

    2016-01-01

    Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m−3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. PMID:28028539

  11. 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.

  12. 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.

  13. 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.

  14. Assessment of pollution aerosols sources above the Straits of Dover using lead isotope geochemistry.

    PubMed

    Deboudt, K; Flament, P; Weis, D; Mennessier, J P; Maquinghen, P

    1999-09-15

    We assess the capability of lead isotopes to study the transport of pollution aerosols above the Straits of Dover by collecting atmospheric aerosols above the Eastern Channel and the Southern Bight of the North Sea. During the same period, we characterized the lead isotopic signature of the main industrial sources on the French coast near the Straits of Dover. Urban and automobile-derived aerosols were also collected. Due to the phasing out of lead in gasoline, the urban isotopic composition (206Pb/207Pb = 1.158 +/- 0.003) has become more radiogenic, although it is highly variable. On a regional scale, major industrial emissions have a well-defined isotopic composition (1.13 < 206Pb/207Pb < 1.22), more radiogenic than the petrol-lead signature (1.06 < 206Pb/207Pb < 1.12). These results together with those measured near the main coastal highway show that the automobile source has become a minor component of particulate lead in air. On a local scale, Dunkerque, the most urbanized and industrialized area along the Straits of Dover, may transiently control elevated lead concentrations. Except for the occurrence of local and regional range transport episodes, lead concentrations in the Straits of Dover can be related to remote or semi-remote pollution source emissions. Combining air mass retrospective trajectories and related lead abundances and isotopic compositions, it can be shown that lead aerosols originating from eastern Europe have an isotopic signature (1.145 < 206Pb/207Pb < 1.169) different from the isotopic composition of west-European lead aerosols (1.111 < 206Pb/207Pb < 1.142). The influence of remote North American sources is suggested, with caution, due to uncertainties in meteorological calculations.

  15. 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...

  16. Evidence for a Significant Source of Sea Salt Aerosol from Blowing Snow Above Sea Ice in the Southern Ocean

    NASA Astrophysics Data System (ADS)

    Frey, M. M.; Brooks, I. M.; Anderson, P. A.; Nishimura, K.; Yang, X.; Jones, A. E.; Wolff, E. W.

    2014-12-01

    Over most of the Earth, sea salt aerosol (SSA) derives from sea spray and bubble bursting at the open ocean surface. SSA as the major component of marine aerosol contributes directly to the radiative balance and can act as cloud condensation nuclei. SSA can also significantly impact the lifetime of methane, ozone or mercury through the photochemical release of reactive halogens. A recent model study suggested that the sublimation of saline blowing snow above sea ice can generate more SSA than is produced from a similar area of open ocean. A winter cruise through the Weddell Sea during June - August 2013 provided unique access to a potential SSA source region in the Antarctic sea ice zone to test this hypothesis.Reported are first measurements of snow particle as well as aerosol concentrations, size distributions and chemical composition, during blowing snow events above sea ice. Snow particle spectra are found to be similar to those observed on the continent. Even though the salinity of surface and blowing snow was very low (<0.1 psu) a significant increase of aerosol in the SSA size range was observed during and after blowing snow events. This is consistent with model runs including a blowing snow parameterisation which suggest low sensitivity of SSA number densities to snow salinity within the observed range. First estimates of SSA flux from blowing snow using eddy correlation are significant, although falling below published values of the sea spray source function. We discuss the dependance of observed SSA production rates on ambient conditions as well as the significance to the Southern Ocean environment.

  17. 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

  18. Improved MODIS aerosol retrieval in urban areas using a land classification approach and empirical orthogonal functions

    NASA Astrophysics Data System (ADS)

    Levitan, Nathaniel; Gross, Barry

    2016-10-01

    New, high-resolution aerosol products are required in urban areas to improve the spatial coverage of the products, in terms of both resolution and retrieval frequency. These new products will improve our understanding of the spatial variability of aerosols in urban areas and will be useful in the detection of localized aerosol emissions. Urban aerosol retrieval is challenging for existing algorithms because of the high spatial variability of the surface reflectance, indicating the need for improved urban surface reflectance models. This problem can be stated in the language of novelty detection as the problem of selecting aerosol parameters whose effective surface reflectance spectrum is not an outlier in some space. In this paper, empirical orthogonal functions, a reconstruction-based novelty detection technique, is used to perform single-pixel aerosol retrieval using the single angular and temporal sample provided by the MODIS sensor. The empirical orthogonal basis functions are trained for different land classes using the MODIS BRDF MCD43 product. Existing land classification products are used in training and aerosol retrieval. The retrieval is compared against the existing operational MODIS 3 KM Dark Target (DT) aerosol product and co-located AERONET data. Based on the comparison, our method allows for a significant increase in retrieval frequency and a moderate decrease in the known biases of MODIS urban aerosol retrievals.

  19. 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.

  20. 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

  1. Potential sea salt aerosol sources from frost flowers in the pan-Arctic region

    SciTech Connect

    Xu, Li; Russell, Lynn M.; Burrows, Susannah M.

    2016-09-23

    In order to better represent observed wintertime aerosol concentrations at Barrow, Alaska, we implemented an observationally-based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM). In this work, we evaluate the potential influence of this sea salt source on the pan-Arctic (60ºN-90ºN) climate. Results show that frost flower salt emissions substantially increase the modeled surface sea salt aerosol concentration in the winter months when new sea ice and frost flowers are present. The parameterization reproduces both the magnitude and seasonal variation of the observed submicron sea salt aerosol concentration at surface in Barrow during winter much better than the standard CESM simulation without a frost-flower salt particle source. Adding these frost flower salt particle emissions increases aerosol optical depth by 10% and results in a small cooling at surface. The increase in salt particle mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration, as well as 10% increases in cloud droplet number and 40% increases in liquid water content near coastal regions adjacent to continents. These cloud changes reduce longwave cloud forcing by 3% and cause a small surface warming, increasing the downward longwave flux at the surface by 2 W m-2 in the pan-Arctic under the present-day climate.

  2. Aerosol fine fraction in the Venice Lagoon: Particle composition and sources

    NASA Astrophysics Data System (ADS)

    Prodi, F.; Belosi, F.; Contini, D.; Santachiara, G.; Di Matteo, L.; Gambaro, A.; Donateo, A.; Cesari, D.

    2009-04-01

    The work presents a characterisation of aerosol sampled during three campaigns conducted in the Venice Lagoon from 30 June to 21 July 2004, from 15 February to 10 March 2005 and from 8 May to 25 May 2006. The results yield information about the physical-chemical characteristics of fine aerosol, the possible sources and its fate. Sulphate (SO 42-), nitrate (NO 3-) and ammonium (NH 4+) are identified as the main water soluble components. The sum of these ions in the spring campaign 2006 varies from 51% to nearly 100% of PM2.5 fraction aerosol. NH 4+ is found to be significantly correlated to non-sea-salt sulphate (nss-SO 42-) and NO 3-, thus indicating the prevalent presence of ammonium nitrate and sulphate. The overall lack of a clear diurnal and seasonal cycle of sulphate suggests a transport from the Po Valley, while the diurnal and seasonal profile of nitrate concentrations suggests a prevalence of local generation. Sulphates from sea water through oxidation of dimethylsulfide (DMS) are not negligible (about 10% of the anthropogenic sulphate). The marine aerosol contribution to PM1 and PM2.5 fractions, calculated using Na + as a tracer of sea-salts, is low (range 1-6%). In some cases chlorine depletion is observed. The content of chlorine in the aerosol particle is mostly higher than expected for marine environments (considered on the basis of Cl -/Na + ratio). Therefore, specific sources for the element have been suggested. Oxalic acid anion, which accounts for 55% of the organic compounds examined, presents mean values 180 ng m - 3 and 161 ng m - 3 in the winter and spring campaigns, comparable with reported values in low polluted urban areas. In the winter campaign there is a high correlation between formate and acetate ( R2 = 0.93), suggesting that a common source makes a high contribution to the measured concentrations.

  3. Chemical characterization of PM1.0 aerosol in Delhi and source apportionment using positive matrix factorization.

    PubMed

    Jaiprakash; Singhai, Amrita; Habib, Gazala; Raman, Ramya Sunder; Gupta, Tarun

    2017-01-01

    Fine aerosol fraction (particulate matter with aerodynamic diameter <= 1.0 μm (PM)1.0) over the Indian Institute of Technology Delhi campus was monitored day and night (10 h each) at 30 m height from November 2009 to March 2010. The samples were analyzed for 5 ions (NH4(+), NO3(-), SO4(2-), F(-), and Cl(-)) and 12 trace elements (Na, K, Mg, Ca, Pb, Zn, Fe, Mn, Cu, Cd, Cr, and Ni). Importantly, secondary aerosol (sulfate and nitrate) formation was observed during dense foggy events, supporting the fog-smog-fog cycle. A total of 76 samples were used for source apportionment of PM mass. Six factors were resolved by PMF analyses and were identified as secondary aerosol, secondary chloride, biomass burning, soil dust, iron-rich source, and vehicular emission. The geographical location of the sources and/or preferred transport pathways was identified by conditional probability function (for local sources) and potential source contribution function (for regional sources) analyses. Medium- and small-scale metal processing (e.g. steel sheet rolling) industries in Haryana and National Capital Region (NCR) Delhi, coke and petroleum refining in Punjab, and thermal power plants in Pakistan, Punjab, and NCR Delhi were likely contributors to secondary sulfate, nitrate, and secondary chloride at the receptor site. The agricultural residue burning after harvesting season (Sept-Dec and Feb-Apr) in Punjab, and Haryana contributed to potassium at receptor site during November-December and March 2010. The soil dust from North and East Pakistan, and Rajasthan, North-East Punjab, and Haryana along with the local dust contributed to soil dust at the receptor site, during February and March 2010. A combination of temporal behavior and air parcel trajectory ensemble analyses indicated that the iron-rich source was most likely a local source attributed to emissions from metal processing facilities. Further, as expected, the vehicular emissions source did not show any seasonality and was

  4. 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.

  5. 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...

  6. 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.

  7. 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).

  8. 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

  9. 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.

  10. Source identification for fine aerosols in Mammoth Cave National Park

    NASA Astrophysics Data System (ADS)

    Zhao, Weixiang; Hopke, Philip K.

    2006-06-01

    In this study, positive matrix factorization (PMF) was applied to the chemical composition data of the ambient PM 2.5 collected at the Mammoth Cave National Park, an IMPROVE site in Kentucky. Eight individual carbon fractions, four organic carbons (OCs), pyrolyzed organic carbon (OP) and three elemental carbons (ECs), were provided to the analysis. Nine sources including the well-distinguished gasoline emission and diesel emission were identified. Also, the back trajectories indicated the crustal factor in this study were likely caused by Saharan dust storms in the summer. The apportionment of nine sources was: gasoline emission (6.7%), diesel emission (3.1%), summer secondary sulfate (49.0%), winter secondary sulfate (0.6%), OP-rich secondary sulfate (16.2%), secondary nitrate (2.8%), Intercontinental dust plus soil (4.9%), wood smoke (13.6%), and aged sea salt (3.2%). The results of this study will help regularize the pollution control strategies in rural areas of Kentucky and upper mid-western US while demonstrating the feasibility of applying carbon fractions to the source apportionment of rural upper-Midwestern areas.

  11. 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

    2016-06-02

    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.

  12. 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.

  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. Temporal variations in sources and concentrations of black and organic carbon aerosols in the LA Basin

    NASA Astrophysics Data System (ADS)

    Mouteva, G.; Kearney, J.; Fahrni, S.; Santos, G. M.; Czimczik, C. I.

    2012-12-01

    Temporal variations in sources and concentrations of black and organic carbon aerosols in the LA Basin Black carbon (BC), derived from incomplete combustion of fossil and biogenic fuels and vegetation fires, is a crucial component of the aerosol pool, but sources as well as atmospheric transport and lifetime remain poorly constrained by measurements. We characterized the composition of carbonaceous aerosols emitted from urban areas by quantifying the temporal variations in the concentrations and sources of BC and organic carbon (OC) in PM-10 and PM-2.5 from two locations in the Los Angeles basin. Using the radiocarbon signatures in BC and OC allowed us to apportion emissions into fossil and modern contributions. We separated and quantified BC and OC using a modified Sunset OC-EC analyzer coupled to a vacuum line and cryogenically trapped the evolving CO2 (Zhang et al. In Prep.). The instrument and method were tested with well-defined radiocarbon standards to determine background, accuracy and precision. The purified CO2 was converted to graphite and measured at the Keck-AMS facility on unknown samples as small as ≥5 μg C. Preliminary results suggest that radiocarbon content can be used to apportion BC into fossil and modern sources. BC concentrations are on the order of 6-31% total carbon, with 48 to 96% fossil contribution. In the OC fraction we detected several super-modern samples, suggesting local production of radiocarbon, e.g. from medical waste incinerators. Thus, the radiocarbon-based approach cannot be used to quantify sources of OC and bulk carbonaceous aerosols in urban areas. Our measurements contribute to a comprehensive quantification of temporal and spatial variations in urban BC, a key uncertainty in constraining BC sources and transport in North America. References: Zhang YL, Perron N, Zotter P, Minguillón MC, Wacker L, Prévôt ASH, Baltensperger U, Szidat S. In Prep. On the isolation of OC and EC and the optimal strategy of radiocarbon

  15. 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

  16. 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

  17. Toxicological evaluation of realistic emission source aerosols (TERESA): summary and conclusions

    PubMed Central

    Godleski, John J.; Rohr, Annette C.; Coull, Brent A.; Kang, Choong-Min; Diaz, Edgar A.; Koutrakis, Petros

    2013-01-01

    The toxicological evaluation of realistic emissions of source aerosols (TERESA) study seeks to delineate health effects of aerosols formed from emissions of particulate matter sources. This series of papers reports the findings of experiments using coal-fired power plants as the source of emissions and this paper summarizes the findings and knowledge acquired from these studies. Emissions were drawn directly from the stacks of three coal-fired power plants in the US, and photochemically aged in a mobile laboratory to simulate downwind power plant plume processing. The power plants used different sources of coal and had different emission controls. Exposure scenarios included primary particles, secondary particles and mixtures of these with common atmospheric constituents (α-pinene and ammonia). Extensive exposure characterization was carried out, and toxicological outcomes were evaluated in Sprague-Dawley rats exposed to different emission scenarios. Breathing pattern, pulmonary inflammatory responses, in vivo pulmonary and cardiac chemiluminescence and cardiac response in a model of acute myocardial infarction were assessed. The results showed no response or relatively mild responses to the inhaled aerosols studied; complex scenarios which included oxidized emissions and α-pinene to simulate biogenic secondary organic aerosol tended to induce more statistically significant responses than scenarios of oxidized and non-oxidized emissions alone. Relating adverse effects to specific components did not consistently identify a toxic constituent. These findings are consistent with most of the previously published studies using pure compounds to model secondary power plant emissions, but importantly add substantial complexity and thus have considerable merit in defining toxicological responses. PMID:21913822

  18. 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

  19. Experiments on liquid-metal fast breeder reactor aerosol source terms after severe accidents

    SciTech Connect

    Berthoud, G.; Longest, A.W.; Wright, A.L.; Schutz, W.P.

    1988-05-01

    In the extremely unlikely event of a liquid-metal fast breeder reactor core disruptive accident, expanding core material or sodium vapor inside the sodium pool may cause leaks in the vessel head and transport of radioactive material, mostly aerosols, in one large bubble or several smaller bubbles under energetic conditions to the cover gas and through leaks to the inner containment (''instantaneous source term''). Out-of-pile experiments on bubble expansion from a pressurized source inside a liquid (water or sodium) and related phenomena like heat transfer, condensation, entrainment, rise, and aerosol transport were carried out in France and the United States and are continuing in the Federal Republic of Germany. Parameters and results of these experiments are described and discussed, mainly concerning the aerosol problem. It appears that several mechanisms exist for a very efficient removal of particles from the bubble. Retention factors larger than 10,000 were found in most cases. In addition, a short survey is given of French and German experiments on fuel and fission product release from evaporating or burning sodium pools (delayed source term).

  20. [Tracing Sources of Sulfate Aerosol in Nanjing Northern Suburb Using Sulfur and Oxygen Isotopes].

    PubMed

    Wei, Ying; Guo, Zhao-bing; Ge, Xin; Zhu, Sheng-nan; Jiang, Wen-juan; Shi, Lei; Chen, Shu

    2015-04-01

    Abstract: To trace the sources of sulfate contributing to atmospheric aerosol, PM2.5 samples for isotopic analysis were collected in Nanjing northern suburb during January 2014. The sulfur and oxygen isotopic compositions of sulfate from these samples were determined by EA-IRMS. Source identification and apportionment were carried out using stable isotopic and chemical evidences, combined with absolute principal component analysis (APCA) method. The Δ34S values of aerosol sulfate ranged from 2.7 per thousand to 6.4 per thousand, with an average of 5.0 per thousand ± 0.9 per thousand, while the Δ18O values ranged from 10.6 per thousand to 16.1 per thousand, with an average of 12.5 per thousand ± 1.37 per thousand. In conjunction with air mass trajectories, the results suggested that aerosol sulfates were controlled by a dominance of local anthropogenic sulfate, followed by the contributions of long-distance transported sulfate. There was a minor effect of some other low-Δ34S valued sulfates, which might be expected from biogenic sources. Absolute principal component analysis results showed that the contributions of anthropogenic sulfate and long-distance transported sulfate were 46.74% and 31.54%, respectively.

  1. Marine aerosol as a possible source for endotoxins in coastal areas.

    PubMed

    Lang-Yona, Naama; Lehahn, Yoav; Herut, Barak; Burshtein, Noa; Rudich, Yinon

    2014-11-15

    Marine aerosols, that are very common in the highly populated coastal cities and communities, may contain biological constituents. Some of this biological fraction of marine aerosols, such as cyanobacteria and plankton debris, may influence human health by inflammation and allergic reactions when inhaled. In this study we identify and compare sources for endotoxins sampled on filters in an on-shore and more-inland site. Filter analysis included endotoxin content, total bacteria, gram-negative bacteria and cyanobacteria genome concentrations as well as ion content in order to identify possible sources for the endotoxins. Satellite images of chlorophyll-a levels and back trajectory analysis were used to further study the cyanobacteria blooms in the sea, close to the trajectory of the sampled air. The highest endotoxin concentrations found in the shoreline site were during winter (3.23±0.17 EU/m(3)), together with the highest cyanobacteria genome (1065.5 genome/m(3)). The elevated endotoxin concentrations were significantly correlated with cyanobacterial levels scaled to the presence of marine aerosol (r=0.90), as well as to chlorophyll-a (r=0.96). Filters sampled further inland showed lower and non-significant correlation between endotoxin and cyanobacteria (r=0.70, P value=0.19), suggesting decrease in marine-originated endotoxin, with possible contributions from other sources of gram-negative non-cyanobacteria. We conclude that marine cyanobacteria may be a dominant contributor to elevated endotoxin levels in coastal areas.

  2. Aqueous Oxidation of Green Leaf Volatiles as a Source of Secondary Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Richards-Henderson, N. K.; Hansel, A.; Pham, A. T.; Vempati, H. S.; Valsaraj, K. T.; Anastasio, C.

    2013-12-01

    Vegetation emits volatile oxygenated hydrocarbons - the green leaf volatiles (GLVs) - which are formed from the biochemical conversion of linoleic and linolenic acids within plant cells. Stress or damage to vegetation can significantly elevate emission fluxes of these compounds, some of which are fairly water soluble. Aqueous-phase reactions of the GLVs with photochemically generated oxidants - such as hydroxyl radical (OH), singlet oxygen (1O2) and excited triplet states of organic compounds (3C*) _ might then form low-volatility products that can act as secondary organic aerosol (SOA). In order to determine if GLVs can be a significant source of secondary organic carbon in fogwater, studies of GLVs in laboratory solutions are needed to elucidate the oxidation kinetics and the corresponding SOA mass yields. In this study we are determining the second-order rate constants, and SOA mass yields, for five GLVs (cis-3-hexen-1-ol, cis-3-hexenylacetate, methyl salicylate, methyl jasmonate, and 2-methyl-3-butene-2-ol) reacting with OH,1O2 and 3C*. Experiments are performed at relevant fog water pHs, temperatures, and oxidant concentrations. Rate constants are determined using a relative rate approach in which the decay of GLVs and reference compounds are monitored as function of time by HPLC. The capacity of GLVs to form aqueous SOA was determined by following the formation of their decomposition products with HPLC-UV/DAD and HPLC-ESI/MS. SOA mass yields are measured gravimetrically from laboratory solutions containing atmospherically relevant concentrations of photooxidants and GLVs, and irradiated with simulated sunlight. We will use our results to assess the potential contribution of aqueous GLV reactions as a source of SOA in cloudy or foggy atmospheres.

  3. 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

  4. Radiocarbon source apportionment of urban and wildfire black and organic carbon aerosols

    NASA Astrophysics Data System (ADS)

    Mouteva, G.; Fahrni, S. M.; Santos, G.; Randerson, J. T.; Czimczik, C. I.

    2013-12-01

    Fossil and non-fossil sources of black carbon (BC) and organic carbon (OC) in carbonaceous aerosols can be quantified unambiguously by radiocarbon (14C) measurements. However, accurate 14C-based source apportionment requires a clear and reproducible physical separation of OC and BC, as well as minimal sample contaminations with non-sample carbon. To achieve a clear separation, we used a thermo-optical aerosol analyzer (Sunset Laboratory Inc, USA) with a newly established protocol (Swiss_4S protocol, Zhang et al., 2012), specifically optimized to completely separate the OC and BC fractions with minimal charring and maximum BC recovery. A simple and efficient vacuum line was coupled to the analyzer to trap produced CO2 with high yields and low carbon blanks. Upon trapping, CO2 samples sealed into glass ampoules were converted to graphite and measured for their radiocarbon content at the Keck Carbon Cycle Accelerator Mass Spectrometry Laboratory at the University of California, Irvine. Here, we present the results from the radiocarbon analysis of a set of 14C reference materials, blanks and inter-comparison samples for both OC and BC with sample sizes as small as 5 μg C. We will also present initial results from a set of urban aerosol samples from Salt Lake City, collected throughout 2012 and 2013, and from interior Alaska, collected during the summer of 2013 near the Stuart Creek 2 wildfire.

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

    SciTech Connect

    Thornton, Joel A.; Worsnop, Douglas

    2016-09-22

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

  6. Effects of sulfuric acid aerosol on cardiopulmonary function of dogs, sheep, and humans.

    PubMed

    Sackner, M A; Ford, D; Fernandez, R; Cipley, J; Perez, D; Kwoka, M; Reinhart, M; Michaelson, E D; Schreck, R; Wanner, A

    1978-09-01

    Submicronic aerosol of sulfuric acid (H2SO4) originates from the burning of fossil fuels and discharge of vapor from the automobile engine equipped with the catalytic converter. This study was conducted to determine whether brief exposure to this aerosol in high concentrations adversely affects the cardiopulmonary system. In all studies, submicronic aerosol of sodium chloride was used as a control. Anesthetized dogs that breathed H2SO4 aerosol in concentrations up to 8 mg per m3 showed no effects on respiratory resistance, static lung compliance, and functional residual capacity. A 4-hour exposure to H2SO4 aerosol (4 mg per m3) produced no significant changes in mechanics of breathing, functional residual capacity, pulmonary and systemic arterial blood pressures, cardiac output, heart rate, and arterial blood gas tensions. Conscious sheep that breathed H2SO4 aerosol in concentrations up to 14 mg per m3 for 20 min had no alteration of tracheal mucous velocity in an immediate 3-hour follow-up period or 5 to 10 days later. Conscious sheep that breathed H2SO4 aerosol (4 mg per m3) for 4 hours had no significant alteration of tracheal mucous velocity immediately and 2 hours thereafter. Both normal and asthmatic adults breathing H2SO4 aerosol in concentrations up to 1 mg per m3 for 10 min showed no significant alteration of lung volumes, distribution of ventilation, ear oximetry, dynamic mechanics of breathing, oscillation mechanics of the chest-lung system, pulmonary capillary blood flow, diffusing capacity, O2 consumption, and pulmonary tissue volume. No delayed effects in pulmonary function nor exacerbation of bronchial asthma were observe during a follow-up period of a few weeks. The present study indicates that single exposure to submicronic H2SO4 aerosol does not produce an immediate or a delayed adverse effect on cardiopulmonary function in anesthetized dogs, conscious sheep, and normal and asthmatic adults.

  7. Optical and radiative properties of aerosols over Desalpar, a remote site in western India: Source identification, modification processes and aerosol type discrimination.

    PubMed

    Patel, Piyushkumar N; Dumka, U C; Kaskaoutis, D G; Babu, K N; Mathur, Alok K

    2017-01-01

    Aerosol optical properties are analyzed for the first time over Desalpar (23.74°N, 70.69°E, 30m above mean sea level) a remote site in western India during October 2014 to August 2015. Spectral aerosol optical depth (AOD) measurements were performed using the CIMEL CE-318 automatic Sun/sky radiometer. The annual-averaged AOD500 and Ångström exponent (α440-870) values are found to be 0.43±0.26 and 0.69±0.39, respectively. On the seasonal basis, high AOD500 of 0.45±0.30 and 0.61±0.34 along with low α440-870 of 0.41±0.27 and 0.41±0.35 during spring (March-May) and summer (June-August), respectively, suggest the dominance of coarse-mode aerosols, while significant contribution from anthropogenic sources is observed in autumn (AOD500=0.47±0.26, α440-870=1.02±0.27). The volume size distribution and the spectral single-scattering albedo also confirm the presence of coarse-mode aerosols during March-August. An overall dominance of a mixed type of aerosols (~56%) mostly from October to February is found via the AOD500 vs α440-870 relationship, while marine aerosols contribute to ~18%. Spectral dependence of α and its second derivative (α') are also used for studying the aerosol modification processes. The average direct aerosol radiative forcing (DARF) computed via the SBDART model is estimated to range from -27.08Wm(-2) to -10.74Wm(-2) at the top of the atmosphere, from -52.21Wm(-2) to -21.71Wm(-2) at the surface and from 10.97Wm(-2) to 26.54Wm(-2) within the atmosphere. This atmospheric forcing translates into heating rates of 0.31-0.75Kday(-1). The aerosol properties and DARF are also examined for different trajectory clusters in order to identify the sources and to assess the influence of long-range transported aerosols over Desalpar.

  8. 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.

  9. 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.

  10. 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.

  11. Potential sea salt aerosol sources from frost flowers in the pan-Arctic region

    NASA Astrophysics Data System (ADS)

    Xu, Li; Russell, Lynn M.; Burrows, Susannah M.

    2016-09-01

    In order to better represent observed wintertime aerosol mass and number concentrations in the pan-Arctic (60°N-90°N) region, we implemented an observationally based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM, version 1.2.1). In this work, we evaluate the potential influence of this sea salt source on the pan-Arctic climate. Results show that frost flower salt emissions increase the modeled surface sea salt aerosol mass concentration by roughly 200% at Barrow and 100% at Alert and accumulation-mode number concentration by about a factor of 2 at Barrow and more than a factor of 10 at Alert in the winter months when new sea ice and frost flowers are present. The magnitude of sea salt aerosol mass and number concentrations at the surface in Barrow during winter simulated by the model configuration that includes this parameterization agrees better with observations by 48% and 12%, respectively, than the standard CESM simulation without a frost flower salt particle source. At Alert, the simulation with this parameterization overestimates observed sea salt aerosol mass concentration by 150% during winter in contrast to the underestimation of 63% in the simulation without this frost flower source, while it produces particle number concentration about 14% closer to observation than the standard CESM simulation. However, because the CESM version used here underestimates transported sulfate in winter, the reference accumulation-mode number concentrations at Alert are also underestimated. Adding these frost flower salt particle emissions increases sea salt aerosol optical depth by 10% in the pan-Arctic region and results in a small cooling at the surface. The increase in salt aerosol mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration at supersaturation of 0.1%, as well as 10% increases in cloud droplet number and 40% increases in liquid water content

  12. 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

  13. 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

  14. 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

  15. 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.

  16. 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.

  17. 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

  18. The sources, properties, and evolution of organic aerosols in the atmosphere

    NASA Astrophysics Data System (ADS)

    Jimenez, J. L.

    2015-12-01

    Organic aerosols (OA) account for about 1/2 of the submicron particle mass in the atmosphere leading to important impacts on climate, human health, and other issues, but their sources, properties, and evolution are poorly understood. OA is comprised of primary OA (POA, emitted in the particle phase) and secondary OA (SOA, formed by gas-to-particle conversion). Together with others in the community and contrary to the understanding at the time, we demonstrated in the mid-2000s that SOA dominates over POA at most locations. This paradigm shift has led to intense research on the sources, processing, properties, and fate of SOA. Because pre-existing and commercial instruments were very limited for the analysis of the complex mixtures of highly oxidized species comprising real OA, we developed or co-developed several experimental and data analysis techniques aimed at extracting more information out of ambient and laboratory air, and pioneered their application in field experiments. We proposed a new paradigm (Jimenez et al., Science, 2009) that is consistent with worldwide measurements and in which OA and OA precursor gases evolve continuously by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. The amount of SOA formed from urban air is remarkably consistent across the world, although the contributions of different sources remain a subject of debate. Biomass burning emissions rarely form additional OA mass after emission, although rapid chemical aging is always observed. Global model-measurement comparisons suggest the need for a large (100 Tg/yr) "anthropogenically-controlled" SOA source, thought to be dominated by anthropogenically-enhanced biogenic SOA. SOA formed from several pathways from biogenic emissions is starting to be better characterized, as are key SOA properties such as

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

    NASA Astrophysics Data System (ADS)

    Liu, Shang; Ahlm, Lars; Day, Douglas A.; Russell, Lynn M.; Zhao, Yunliang; Gentner, Drew R.; Weber, Robin J.; Goldstein, Allen H.; Jaoui, Mohammed; Offenberg, John H.; Kleindienst, Tadeusz E.; Rubitschun, Caitlin; Surratt, Jason D.; Sheesley, Rebecca J.; Scheller, Scott

    2012-12-01

    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 chemical and physical properties of SOA at Bakersfield, California, a site influenced by anthropogenic and terrestrial biogenic emissions. Factor analysis was applied to the infrared and mass spectra of fine particles to identify sources and atmospheric processing that contributed to the organic mass (OM). We found that OM accounted for 56% of submicron particle mass, with SOA components contributing 80% to 90% of OM from 15 May to 29 June 2010. SOA formed from alkane and aromatic compounds, the two major classes of vehicle-emitted hydrocarbons, accounted for 65% OM (72% SOA). The alkane and aromatic SOA components were associated with 200 nm to 500 nm accumulation mode particles, likely from condensation of daytime photochemical products of VOCs. In contrast, biogenic SOA likely formed from condensation of secondary organic vapors, produced from NO3radical oxidation reactions during nighttime hours, on 400 nm to 700 nm sized primary particles, and accounted for less than 10% OM. Local petroleum operation emissions contributed 13% to the OM, and the moderate O/C (0.2) of this factor suggested it was largely of secondary origin. Approximately 10% of organic aerosols in submicron particles were identified as either vegetative detritus (10%) or cooking activities (7%), from Fourier transform infrared spectroscopic and aerosol mass spectrometry measurements, respectively. While the mass spectra of several linearly independent SOA components were nearly identical and external source markers were needed to separate them, each component had distinct infrared spectrum, likely associated with the source-specific VOCs from which they formed.

  20. 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

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

    PubMed Central

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

    2016-01-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites. PMID:27991554

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

    NASA Astrophysics Data System (ADS)

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

    2016-12-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites.

  3. 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

  4. Electro-Optical Aerosol Phase Function Database PFNDAT2005

    DTIC Science & Technology

    2005-11-01

    Pollack, J.B.; Khare, B.N. Optical Constants of Several Atmospheric Aerosol Species, Ammonium Sulphate , Aluminum Oxide and Sodium Chloride. J. of...16 Table 12. Precipitation rates, number...rain at three precipitation rates (drizzle, moderate, and heavy); and two classes of snow, “dry” and “wet”. Dusts are treated under four categories

  5. 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

  6. 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

  7. 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

  8. 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

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

    NASA Astrophysics Data System (ADS)

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

    2011-08-01

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

  10. Stable carbon isotopic compositions of total carbon, dicarboxylic acids and glyoxylic acid in the tropical Indian aerosols: Implications for sources and photochemical processing of organic aerosols

    NASA Astrophysics Data System (ADS)

    Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.; Tachibana, Eri

    2011-09-01

    The tropical Indian aerosols (PM10) collected on day- and nighttime bases in winter and summer, 2007 from Chennai (13.04°N; 80.17°E) were studied for stable carbon isotopic compositions (δ13C) of total carbon (TC), individual dicarboxylic acids (C2-C9) and glyoxylic acid (ωC2). δ13C values of TC ranged from -23.9‰ to -25.9‰ (-25.0 ± 0.6‰; n = 49). Oxalic (C2) (-17.1 ± 2.5‰), malonic (C3) (-20.8 ± 1.8‰), succinic (C4) (-22.5 ± 1.5‰) and adipic (C6) (-20.6 ± 4.1‰) acids and ωC2 acid (-22.4 ± 5.5‰) were found to be more enriched with 13C compared to TC. In contrast, suberic (C8) (-29.4 ± 1.8‰), phthalic (Ph) (-30.1 ± 3.5‰) and azelaic (C9) (-28.4 ± 5.8‰) acids showed smaller δ13C values than TC. Based on comparisons of δ13C values of TC in Chennai aerosols to those (-24.7 ± 2.2‰) found in unburned cow-dung samples collected from Chennai and isotopic signatures of the particles emitted from point sources, we found that biofuel/biomass burning are the major sources of carbonaceous aerosols in South and Southeast Asia. The decrease in δ13C values of C9 diacid by about 5‰ from winter to summer suggests that tropical plant emissions also significantly contribute to organic aerosol in this region. Significant increase in δ13C values from C4 to C2 diacids in Chennai aerosols could be attributed for their photochemical processing in the tropical atmosphere during long-range transport from source regions.

  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. Hydrolysis of organonitrate functional groups in aerosol particles

    SciTech Connect

    Liu, Shang; Shilling, John E.; Song, Chen; Hiranuma, Naruki; Zaveri, Rahul A.; Russell, Lynn M.

    2012-10-19

    Organonitrate (ON) groups are important substituents in secondary organic aerosols. Model simulations and laboratory studies indicate a large fraction of ON groups in aerosol particles, but much lower quantities are observed in the atmosphere. Hydrolysis of ON groups in aerosol particles has been proposed recently. To test this hypothesis, we simulated formation of ON molecules in a reaction chamber under a wide range of relative humidity (0% to 90%). The mass fraction of ON groups (5% to 20% for high-NOx experiments) consistently decreased with increasing relative humidity, which was best explained by hydrolysis of ON groups at a rate of 4 day-1 (lifetime of 6 hours) for reactions under relative humidity greater than 20%. In addition, we found that secondary nitrogen-containing molecules absorb light, with greater absorption under dry and high-NOx conditions. This work provides the first evidence for particle-phase hydrolysis of ON groups, a process that could substantially reduce ON group concentration in the atmosphere.

  13. 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.

  14. 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

  15. Polar organic marker compounds in atmospheric aerosols: Determination, time series, size distributions and sources

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan

    Terrestrial vegetation releases substantial amounts of reactive volatile organic compounds (VOCs; e.g., isoprene, monoterpenes) into the atmosphere. The VOCs can be rapidly photooxidized under conditions of high solar radiation, yielding products that can participate in new particle formation and growth processes above forests. This thesis focuses on the characterization, identification and quantification of oxidation products of biogenic VOC (BVOCs) as well as other species (tracer compounds) that provide information on aerosol sources and source processes. Atmospheric aerosols from various forested sites (i.e., Hyytiala, southern Finland; Rondonia, Brazil; K-Puszta, Hungary and Julich, Germany) were analyzed with Gas Chromotography/Mass Spectrometry (GC/MS) using analytical procedure that targets polar organic compounds. The study demonstrated that isoprene (i.e., 2-methyerythritol, 2-methylthreitol, 2-methylglyceric acid and C5-alkene triols (2-methyl-1,3,4-trihydroxy-l-butene (cis and trans) and 3 methyl-2,3,4-trihydroxy-1-butene)) and monoterpene (pinic acid, norpinic acid, 3-hydroxyglutaric acid and 3-methyl-1,2,3-butanetricarboxylic acid) oxidation products were present in substantial concentrations in atmospheric aerosols suggesting that oxidation of BVOC from the vegetation is an important process in all studied sites. On the other hand, presence of levoglucosan, biomass burning marker, especially in Amazonian rain forest site at Rondonia, Brazil, pointed that all sites were affected by anthropogenic activities, namely biomass burning. Other identified compounds included plyols, arabitol, mannitol and erythritol, which are marker compounds for fungal spores and monosacharides, glucose and fructose, markers for plant polens. Temporal variations as well as mass size distributions of the detected species confirmed the possible formation mechanisms of marker compounds.

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

    NASA Astrophysics Data System (ADS)

    Crippa, M.; DeCarlo, P. F.; Slowik, J. G.; Mohr, C.; Heringa, M. F.; Chirico, R.; Poulain, L.; Freutel, F.; Sciare, J.; Cozic, J.; Di Marco, C. F.; Elsasser, M.; Nicolas, J. B.; Marchand, N.; Abidi, E.; Wiedensohler, A.; Drewnick, F.; Schneider, J.; Borrmann, S.; Nemitz, E.; Zimmermann, R.; Jaffrezo, J.-L.; Prévôt, A. S. H.; Baltensperger, U.

    2013-01-01

    The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30-36%) and nitrate (28-29%), with lower contributions from sulfate (14-16%), ammonium (12-14%) and black carbon (7-13%). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11-15% of organic mass), biomass burning (13-15%) and cooking (up to 35% during meal hours). Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.

  17. 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

  18. Characterization of metal aerosols in PM10 from urban, industrial, and Asian Dust sources.

    PubMed

    Park, Kihong; Dam, Hung Duy

    2010-01-01

    Metallic elements (As, Be, Ca, Cd, Co, Cr, Fe, K, Mn, Ni, Pb, Sb, Se, and Zn) in PM10 aerosols were determined at urban and industrial sites, which are affected by traffic and residential sources, metallurgical activity, and petrochemical and steel works. The effect of the long-range transported Asian Dust on the metal content of aerosols was also examined. At the urban sampling site, concentrations of As, Cd, Pb, Se, and Zn were assigned to road traffic and combustion sources, Ca and Fe to soil dust sources from long-range transported Asian Dusts, and Cr and Ni to metallurgical sources transported from the nearby industrial complex, based on Principal Component Analysis (PCA). Enhanced Cr and Ni concentrations at the metallurgical industrial site suggest that local emissions from metal-assembly facilities and manufacture of alloys contributed to elevated levels of those metals. We also observed that petrochemical activities contributed to increased levels of Sb and Zn. When Asian Dust events occurred, Ca, Fe, K, and Zn concentrations dramatically increased compared to values without the Asian Dust. Two different types of Asian Dust events were observed. For the Asian Dust event 1 (4/1/2007), the Fe and K concentrations were much higher by a factor of 2-3 than those for the Asian Dust event 2 (3/2/2008), while As, Mn, and Zn concentrations were significantly higher on the Asian Dust event 2. Backward trajectory analysis showed that for the Asian Dust event 2, the air mass had passed over the heavily industrialized zones in China during long-range transport to the current sampling site, suggesting that the As, Mn, and Zn may have originated from industrial sources.

  19. 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.

  20. 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

  1. Characteristics and source of black carbon aerosols at Akedala station, Central Asia

    NASA Astrophysics Data System (ADS)

    Wang, Huiqin; He, Qing; Liu, Tao; Chen, Feng; Liu, Xinchun; Zhong, Yuting; Yang, Sen

    2012-11-01

    Black carbon concentration and weather data were online monitored continuously from March 2008 to February 2009 at the Akedala regional atmosphere station in the arid region of Central Asia. We present the daily, monthly and seasonal variations of BC concentration in the atmosphere and discuss the possible emission sources. Black carbon concentration in this region varies in the range of 43.7-1,559.2 ng/m3. A remarkable seasonal variation of BC in the aerosol was observed in the order of winter > spring > autumn > summer. The peak value of BC appeared at 10:00-13:00 while the lowest one at 7:00-9:00 each day. Air masses backward trajectories show the potential emission sources in the northwest from spring to autumn. Through back trajectory also revealed that BC in winter might be attributed to the emission from the anthropogenic activities, including domestic heating, cooking, combustion of oil and natural gas, and the medium-range transport from those cities in northern slope of Tianshan Mountains and Siberia. Some BC aerosols from the arid region of Central Asia were transported to the Pacific Ocean by the Westerlies.

  2. 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.

  3. Tropical biomass burning is a larger than expected source of black carbon aerosol

    NASA Astrophysics Data System (ADS)

    Reddington, C.; Spracklen, D. V.; Rap, A.; Artaxo, P. P.; Carslaw, K. S.; Mann, G.; Rizzo, L. V.; Arana, A.; Morgan, W.; Coe, H.

    2013-12-01

    Biomass burning (BB) emissions are a major global source of black carbon (BC) aerosol of which agricultural burning and deforestation fires account for at least a quarter of emissions. However, high temporal and spatial variability in the emissions lead to major challenges for their quantification and representation in large scale models. Previous modelling studies have found a persistent underestimation of aerosol optical depth (AOD) observed in BB-influenced regions, requiring particulate matter (PM) emissions from fires to be scaled by a factor of ~2-4 in order to match observations. Here we evaluate a global aerosol microphysics model (GLOMAP) against long-term observations of PM, BC and AOD to better understand tropical BB aerosol and quantify its direct radiative effects (DRE). Our region of study is Amazonia, where large scale BB is the dominant source of fine mode PM and BC. We performed simulations with GLOMAP for the period 2000-2012 using two different BB emission inventories: GFED3 and GFASv1.0. Simulated monthly mean aerosol concentrations over Amazonia are comparable between the two emission inventories, with slightly longer BB seasons and a lower peak in 2010 with the GFAS emissions. We use measurements of PM2.5 (made using gravimetric filter analysis) and equivalent BC (made using optical reflectance and Multi-angle Absorption Photometry) at two ground sites in Amazonia during 2008-2012. Comparisons with these observations show that the model captures the seasonal cycle of PM2.5 and BC mass concentrations well (R2 between 0.7 and 0.8) with maximum concentrations predicted in the dry season (~July to October). However, the model substantially underpredicts the observed concentrations of BC mass at these sites throughout the 2008-2012 period (bias GFED, -63%; GFAS -75%), despite a relatively good agreement with observed total PM2.5 (bias GFED, -15%; GFAS, -28%). Over Amazonia, the uncertainties in modelled BC mass are dominated by uncertainties in the

  4. 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).

  5. The application of accelerator mass spectroscopy (AMS) in the study of source identification of aerosols in China

    SciTech Connect

    Shao Min; Tang Xiaoyan; Li Jinlong

    1995-12-01

    Accelerator Mass Spectrometry is a new physical technique and it was successfully established in China in 1992. This paper tried to apply the AMS in source identification for atmospheric aerosols which was part of our national project of AMS application in environmental research. For comparison, we also studied the aerosol sources by multivariate analysis models such as correspond factor analysis, principal factor analysis and target recognition analysis. For the samples we collected in suburb of Beijing, the results by factor analysis showed that the predominant TSP source was soil which contributed more than 50% to atmospheric particles. However, the AMS results demonstrated that carbonaceous aerosols have quite different emission sources. For carbonaceous aerosols of Beijing, Hunan and Shandong, the contribution to ambient particles from fossil fuel was nearly 2/3, and as the man-made activities (coal-burning, etc.) increased, the fossil part contributed more. Therefore, it`s significant to combine the method of factor analysis and AMS in the study of atmospheric aerosols.

  6. 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

  7. 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

  8. Calf Lung Surfactant Recovers Surface Functionality After Exposure to Aerosols Containing Polymeric Particles

    PubMed Central

    Farnoud, Amir M.

    2016-01-01

    Abstract Background: Recent studies have shown that colloidal particles can disrupt the interfacial properties of lung surfactant and thus key functional abilities of lung surfactant. However, the mechanisms underlying the interactions between aerosols and surfactant films remain poorly understood, as our ability to expose films to particles via the aerosol route has been limited. The aim of this study was to develop a method to reproducibly apply aerosols with a quantifiable particle dose on lung surfactant films and investigate particle-induced changes to the interfacial properties of the surfactant under conditions that more closely mimic those in vivo. Methods: Films of DPPC and Infasurf® were exposed to aerosols containing polystyrene particles generated using a Dry Powder Insufflator™. The dose of particles deposited on surfactant films was determined via light absorbance. The interfacial properties of the surfactant were studied using a Langmuir-Wilhelmy balance during surfactant compression to film collapse and cycles of surface compression and expansion at a fast cycling rate within a small surface area range. Results: Exposure of surfactant films to aerosols led to reproducible dosing of particles on the films. In film collapse experiments, particle deposition led to slight changes in collapse surface pressure and surface area of both surfactants. However, longer interaction times between particles and Infasurf® films resulted in time-dependent inhibition of surfactant function. When limited to lung relevant surface pressures, particles reduced the maximum surface pressure that could be achieved. This inhibitory effect persisted for all compression-expansion cycles in DPPC, but normal surfactant behavior was restored in Infasurf® films after five cycles. Conclusions: The observation that Infasurf® was able to quickly restore its function after exposure to aerosols under conditions that better mimicked those in vivo suggests that particle

  9. 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.

  10. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    DOE PAGES

    Woody, Matthew C.; Baker, Kirk R.; Hayes, Patrick L.; ...

    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

  11. 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

  12. 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

  13. A review of dicarboxylic acids and related compounds in atmospheric aerosols: Molecular distributions, sources and transformation

    NASA Astrophysics Data System (ADS)

    Kawamura, Kimitaka; Bikkina, Srinivas

    2016-03-01

    This review aims to update our understanding on molecular distributions of water-soluble dicarboxylic acids and related compounds in atmospheric aerosols with a focus on their geographical variability, size distribution, sources and formation pathways. In general, molecular distributions of diacids in aerosols from the continental sites and over the open ocean waters are often characterized by the predominance of oxalic acid (C2) followed by malonic acid (C3) and/or succinic acid (C4), while those sampled over the polar regions often follow the order of C4 ≥ C2 and C3. The most abundant and ubiquitous diacid is oxalic acid, which is principally formed via atmospheric oxidation of its higher homologues of long chain diacids and other pollution-derived organic precursors (e.g., olefins and aromatic hydrocarbons). However, its occurrence in marine aerosols is mainly due to the transport from continental outflows (e.g., East Asian outflow during winter/spring to the North Pacific) and/or governed by photochemical/aqueous phase oxidation of biogenic unsaturated fatty acids (e.g., oleic acid) and isoprene emitted from the productive open ocean waters. The long-range atmospheric transport of pollutants from mid latitudes to the Arctic in dark winter facilitates to accumulate the reactants prior to their intense photochemical oxidation during springtime polar sunrise. Furthermore, the relative abundances of C2 in total diacid mass showed similar temporal trends with downward solar irradiation and ambient temperatures, suggesting the significance of atmospheric photochemical oxidation processing. Compound-specific isotopic analyses of oxalic acid showed the highest δ13C among diacids whereas azelaic acid showed the lowest value, corroborating the significance of atmospheric aging of oxalic acid. On the other hand, other diacids gave intermediate values between these two diacids, suggesting that aging of oxalic acid is associated with 13C enrichment.

  14. Automatic identification of sources and trajectories of atmospheric Saharan dust aerosols with Latent Gaussian Models

    NASA Astrophysics Data System (ADS)

    Garbe, Christoph; Bachl, Fabian

    2013-04-01

    Dust transported from the Sahara across the ocean has a high impact on radiation fluxes and marine nutrient cycles. Significant progress has been made in characterising Saharan dust properties (Formenti et al., 2011) and its radiative effects through the 'SAharan Mineral dUst experiMent' (SAMUM) (Ansmann et al., 2011). While the models simulating Saharan dust transport processes have been considerably improved in recent years, it is still an open question which meteorological processes and surface characteristics are mainly responsible for dust transported to the Sub-Tropical Atlantic (Schepanski et al., 2009; Tegen et al., 2012). Currently, there exists a large discrepancy between modelled dust emission events and those observed from satellites. In this contribution we present an approach for classifying and tracking dust plumes based on a Bayesian hierarchical model. Recent developments in computational statistics known as Integrated Nested Laplace Approximations (INLA) have paved the way for efficient inference in a respective subclass, the Generalized Linear Model (GLM) (Rue et al., 2009). We present the results of our approach based on data from the SIVIRI instrument on board the Meteosat Second Generation (MSG) satellite. We demonstrate the accuracy for automatically detecting sources of dust and aerosol concentrations in the atmosphere. The trajectories of aerosols are also computed very efficiently. In our framework, we automatically identify optimal parameters for the computation of atmospheric aerosol motion. The applicability of our approach to a wide range of conditions will be discussed, as well as the ground truthing of our results and future directions in this field of research.

  15. Sources and radiative effects of wintertime black carbon aerosols in an urban atmosphere in east India.

    PubMed

    Verma, S; Pani, S K; Bhanja, S N

    2013-01-01

    We carried out an analysis of black carbon (BC) surface mass concentration, its radiative effects, and sources of origin in an urban atmosphere in east India, during winter season, through ground-based measurements and application of modelling tools. BC surface mass concentration exhibited diurnal variation with their higher values and a larger variability during evening to early morning hours than during daytime (1100-1600 h, Local Time, LT) hours. Daytime mean surface BC mass concentration and BC mass fraction in total aerosol (size range 0.23-20 μm) and in submicronic aerosol (size range 0.23-1 μm) during the study period, corresponding to the well-mixed atmospheric layer were 11 μg m(-3), 3-10%, and 9-16% respectively. The mean BC optical depth (BC-AOD) and BC-AOD fraction at 0.5 μm were estimated in an optical model as 0.11 and 13% respectively. Mean shortwave aerosol radiative forcing due to BC at top-of-atmosphere (TOA) during the study period was found to be +0.94 Wm(-2), which is about 59% the global mean radiative forcing due to carbon-dioxide gases. Estimates from BC simulations in a general circulation model showed BC surface concentration and BC optical depth in east India are primarily attributed to emissions from biofuel and fossil fuel combustion. Most of BC surface concentration (95%) and BC optical depth (60%) are contributed by emissions arising from the Indo-Gangetic plain (IGP) but there is a significant influence to BC columnar loading through elevated transport channels attributed mainly to emissions from open biomass burning from distant regions outside IGP.

  16. 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

  17. Investigation of the Sources and Processing of Organic Aerosol over the Central Mexican Plateau from Aircraft Measurements during MILAGRO

    NASA Astrophysics Data System (ADS)

    Decarlo, Peter; Ulbrich, Ingrid; Crounse, John; de Foy, Benjamin; Dunlea, Edward; Aiken, Allison; Wennberg, Paul; Jimenez, Jose-Luis

    2010-05-01

    Organic aerosol (OA) represents approximately half of the submicron aerosol in Mexico City and the Central Mexican Plateau. This study uses the high time resolution measurements performed onboard the NCAR/NSF C-130 aircraft during the MILAGRO/MIRAGE-Mex field campaign in March 2006 to investigate the sources and chemical processing of the OA in this region. An examination of the OA/ΔCO ratio evolution as a function of photochemical age shows distinct behavior in the presence or absence of substantial open biomass burning (BB) influence, with the latter being consistent with other studies in polluted areas. In addition, results from Positive Matrix Factorization (PMF) analysis of 12-second High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) OA spectra will be presented. Four components were resolved. Three of the components contain substantial organic oxygen and are termed semivolatile oxygenated OA (SV-OOA), low-volatility OOA (LV-OOA), and biomass burning OA (BBOA). A reduced "hydrocarbon-like OA" (HOA) component is also resolved. LV-OOA is highly oxygenated (atomic O/C~1) and is aged organic aerosol linked to regional airmasses, with likely contributions from pollution, biomass burning, and other sources. SV-OOA is strongly correlated with ammonium nitrate, Ox, and the Mexico City Basin. We interpret SV-OOA as secondary OA which is nearly all (>90%) anthropogenic in origin. In the absence of biomass burning it represents the largest fraction of OA over the Mexico City basin, consistent with other studies in this region. BBOA is identified as arising from biomass burning sources due to a strong correlation with HCN, and the elevated contribution of thes ion C2H4O2+ (m/z 60, a marker for levoglucosan and other primary BB species). WRF-FLEXPART calculated fire impact factors (FIF) show good correlation with BBOA mass concentrations within the basin, but show location offsets in the far field due to model transport errors. This component is small

  18. Polarized Imaging Nephelometer for Field and Aircraft Measurements of Aerosol Phase Function

    NASA Astrophysics Data System (ADS)

    Dolgos, G.; Martins, J.

    2012-12-01

    Aerosols have a significant impact on the radiative balance and water cycle of our planet through influencing atmospheric radiation. Remote sensing of aerosols relies on scattering phase matrix information to retrieve aerosol properties with frequent global coverage. At the Laboratory for Aerosols, Clouds and Optics (LACO) at the University of Maryland, Baltimore County we developed a new technique to directly measure the aerosol phase function and the degree of linear polarization of the scattered light (two elements of the phase matrix). We designed and built a portable instrument called the Polarized Imaging Nephelometer (PI-Neph). The PI-Neph successfully participated in dozens of flights of the NASA Development and Evaluation of satellite ValidatiOn Tools by Experimenters (DEVOTE) project and the Deep Convective Clouds and Chemistry (DC3) project. The ambient aerosol enters the PI-Neph through an inlet and the sample is illuminated by laser light (wavelength of 532 nm); the scattered light is imaged by a stationary wide field of view camera in the scattering angle range of 2° to 178°. (In some cases stray light limited the scattering angle range to 3° to 176°). The PI-Neph measurement of phase function and the AERONET (AErosol RObotic NETwork) retrievals have already been compared in some cases when the aircraft spiraled over AERONET sites, for example at NASA's Wallops Flight Facility, on October 18 2011, as shown in Figure 1. The differences between the PI-Neph and the AERONET retrievals can be attributed to differences between the ambient size distribution and the one sampled inside the aircraft. The data that is resolved with respect to scattering angle is used to compute the volume scattering coefficient. The above mentioned October 18 flight data showed good agreement between the PI-Neph measurements of volume scattering coefficient and the parallel TSI integrating nephelometer measurements. On average the TSI measurements were 1.02 times the PI

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

    NASA Astrophysics Data System (ADS)

    Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

    2017-02-01

    Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

  20. 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

  1. Complex anthropogenic sources of platinum group elements in aerosols on Cape Cod, USA.

    PubMed

    Sen, Indra S; Peucker-Ehrenbrink, Bernhard; Geboy, Nicholas

    2013-09-17

    Platinum group elements (PGE) of anthropogenic origin have been reported in rainwater, snow, roadside soil and vegetation, industrial waste, and urban airborne particles around the world. As recent studies have shown that PGE are bioavailable in the environment and pose health risks at chronic levels, the extent of PGE pollution is of global concern. In this study, we report PGE concentrations and osmium isotope ((187)Os/(188)Os) ratios of airborne particles (particulate matter, PM10) collected in Woods Hole, a small coastal village on Cape Cod, Massachusetts, U.S.A. The sampling site is more than 100 km away from the nearest urban centers (Boston, Providence) and has no large industrial emission center within a 30 km radius. The study reveals that, although PGE concentrations in rural airborne particulate matter are orders of magnitude lower than in urban aerosols, 69% of the total osmium is of anthropogenic origin. Anthropogenic PGE signatures in airborne particles are thus not restricted to large cities with high traffic flows and substantial industries; they can also be found in rural environments. We further conclude that the combination of Pt/Rh concentration ratios and (187)Os/(188)Os composition can be used to trace PGE sources. The Pt/Rh and (187)Os/(188)Os composition of Woods Hole aerosols indicate that the anthropogenic PGE fraction is primarily sourced from ore smelting processes, with possible minor contributions from fossil fuel burning and automobile catalyst-derived materials. Our results further substantiate the use of (187)Os/(188)Os in source apportionment studies on continental scales.

  2. 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

  3. n-Alkanoic monocarboxylic acid concentrations in urban and rural aerosols: Seasonal dependence and major sources

    NASA Astrophysics Data System (ADS)

    Shannigrahi, Ardhendu S.; Pettersson, Jan B. C.; Langer, Sarka; Arrhenius, Karine; Hagström, Magnus; Janhäll, Sara; Hallquist, Mattias; Pathak, Ravi Kant

    2014-06-01

    We report new data on the abundance and distribution of n-monocarboxylic acids (n-MCAs) in fine- and coarse-mode aerosols in rural and urban areas of Sweden, and determine their possible sources. Overall, C6-C16n-MCAs accounted for ~ 0.5-1.2% of the total PM10 (particulate matter ≤ 10 μm) mass. In general, the C12-C16 fraction was the most abundant (> 75%), with the exception of wintertime samples from a rural site, where C6-C11 acids accounted for 65% of the total C6-C16n-MCA mass. Positive matrix factorization analysis revealed four major sources of n-MCAs: traffic emissions, wood combustion, microbial activity, and a fourth factor that was dominated by semi-volatile n-MCAs. Traffic emissions were important in the urban environment in both seasons and at the rural site during winters, and were a major source of C9-C11 acids. Wood combustion was a significant source at urban sites during the winter and also to some extent at the rural site in both seasons. This is consistent with the use of wood for domestic heating but may also be related to meat cooking. Thus, during the winter, traffic, wood combustion and microbial activity were all important sources in the urban environment, while traffic was the dominant source at the rural site. During the summer, there was considerable day-to-day variation in n-MCA concentrations but microbial activity was the dominant source. The semi-volatile low molecular weight C6-C8 acids accounted for a small (~ 5-10%) fraction of the total mass of n-MCAs. This factor is unlikely to be linked to a single source and its influence instead reflects the partitioning of these compounds between the gas and particle phases. This would explain their greater contribution during the winter.

  4. CALIPSO observations of near-cloud aerosol properties as a function of cloud fraction

    NASA Astrophysics Data System (ADS)

    Yang, Weidong; Marshak, Alexander; Várnai, Tamás.; Wood, Robert

    2014-12-01

    This paper uses spaceborne lidar data to study how near-cloud aerosol statistics of attenuated backscatter depend on cloud fraction. The results for a large region around the Azores show that (1) far-from-cloud aerosol statistics are dominated by samples from scenes with lower cloud fractions, while near-cloud aerosol statistics are dominated by samples from scenes with higher cloud fractions; (2) near-cloud enhancements of attenuated backscatter occur for any cloud fraction but are most pronounced for higher cloud fractions; (3) the difference in the enhancements for different cloud fractions is most significant within 5 km from clouds; (4) near-cloud enhancements can be well approximated by logarithmic functions of cloud fraction and distance to clouds. These findings demonstrate that if variability in cloud fraction across the scenes used for composite aerosol statistics is not considered, a sampling artifact will affect these statistics calculated as a function of distance to clouds. For the Azores region data set examined here, this artifact occurs mostly within 5 km from clouds and exaggerates the near-cloud enhancements of lidar backscatter and color ratio by about 30%. This shows that for accurate characterization of the changes in aerosol properties with distance to clouds, it is important to account for the impact of changes in cloud fraction.

  5. CALIPSO Observations of Near-Cloud Aerosol Properties as a Function of Cloud Fraction

    NASA Technical Reports Server (NTRS)

    Yang, Weidong; Marshak, Alexander; Varnai, Tamas; Wood, Robert

    2015-01-01

    This paper uses spaceborne lidar data to study how near-cloud aerosol statistics of attenuated backscatter depend on cloud fraction. The results for a large region around the Azores show that: (1) far-from-cloud aerosol statistics are dominated by samples from scenes with lower cloud fractions, while near-cloud aerosol statistics are dominated by samples from scenes with higher cloud fractions; (2) near-cloud enhancements of attenuated backscatter occur for any cloud fraction but are most pronounced for higher cloud fractions; (3) the difference in the enhancements for different cloud fractions is most significant within 5km from clouds; (4) near-cloud enhancements can be well approximated by logarithmic functions of cloud fraction and distance to clouds. These findings demonstrate that if variability in cloud fraction across the scenes used to composite aerosol statistics are not considered, a sampling artifact will affect these statistics calculated as a function of distance to clouds. For the Azores-region dataset examined here, this artifact occurs mostly within 5 km from clouds, and exaggerates the near-cloud enhancements of lidar backscatter and color ratio by about 30. This shows that for accurate characterization of the changes in aerosol properties with distance to clouds, it is important to account for the impact of changes in cloud fraction.

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

    SciTech Connect

    Annette Rohr

    2005-03-31

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

  7. Atmospheric aerosol compositions over the South China Sea: temporal variability and source apportionment

    NASA Astrophysics Data System (ADS)

    Xiao, Hong-Wei; Xiao, Hua-Yun; Luo, Li; Shen, Chun-Yan; Long, Ai-Min; Chen, Lin; Long, Zhen-Hua; Li, Da-Ning

    2017-03-01

    In order to evaluate impacts of different source emission on marine atmospheric particles over the South China Sea (SCS), major inorganic ionic concentrations (Na+, Cl-, SO42-, Ca2+, Mg2+, K+, NH4+ and NO3-) were determined in total suspended particulates (TSPs) at Yongxing Island, from March 2014 to February 2015. The annual average concentration of TSPs was 89.6 ± 68.0 µg m-3, with 114.7 ± 82.1, 60.4 ± 27.0 and 59.5 ± 25.6 µg m-3 in cool, warm and transition seasons, respectively. Cl- had the highest concentration, with an annual average of 7.73 ± 5.99 µg m-3, followed by SO42- (5.54 ± 3.65 µg m-3), Na+ (4.00 ± 1.88 µg m-3), Ca2+ (2.15 ± 1.54 µg m-3), NO3- (1.95 ± 1.34 µg m-3), Mg2+ (0.44 ± 0.33 µg m-3), K+ (0.33 ± 0.22 µg m-3) and NH4+ (0.07 ± 0.07 µg m-3). Concentrations of TSPs and the major ions showed seasonal variations, which were higher in the cool season and lower in the warm and transition seasons. Factors of influence were wind speed, temperature, relatively humidity, rain and air mass source region. Back trajectories, concentration-weighted trajectories (CWTs), and positive matrix factorization (PMF) of chemical compositions were analyzed for source apportionment, source contribution and spatiotemporal variation of major ions. Back trajectories and CWTs showed that air masses at Yongxing Island were mainly from the northeast, southwest and southeast in the cool, warm and transition seasons, respectively. The PMF results showed that 77.4 % of Na+ and 99.3 % of Cl- were from sea salt; 60.5 % of NH4+ was from oceanic emission. Anthropogenic sources were very important for atmospheric aerosols over the island. Secondary inorganic aerosol of SO2 and NOx from fossil fuel combustion (especially coal in Chinese coastal regions) was the dominant source of NO3- (69.5 %) and SO42- (57.5 %).

  8. 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.

  9. Source apportionment of fine organic aerosol in Mexico City during the MILAGRO Experiment 2006

    NASA Astrophysics Data System (ADS)

    Stone, E. A.; Snyder, D. C.; Sheesley, R. J.; Sullivan, A. P.; Weber, R. J.; Schauer, J. J.

    2007-07-01

    Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17-30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 47% of OC in the urban area and 31% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5-30% at the urban site and 11-50% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.

  10. Source apportionment of fine organic aerosol in Mexico City during the MILAGRO experiment 2006

    NASA Astrophysics Data System (ADS)

    Stone, E. A.; Snyder, D. C.; Sheesley, R. J.; Sullivan, A. P.; Weber, R. J.; Schauer, J. J.

    2008-03-01

    Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17-30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 49% of OC in the urban area and 32% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5-26% at the urban site and 7-39% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.

  11. 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

  12. 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

  13. Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols.

    PubMed

    McNeill, V Faye

    2015-02-03

    Over the past decade, it has become clear that aqueous chemical processes occurring in cloud droplets and wet atmospheric particles are an important source of organic atmospheric particulate matter. Reactions of water-soluble volatile (or semivolatile) organic gases (VOCs or SVOCs) in these aqueous media lead to the formation of highly oxidized organic particulate matter (secondary organic aerosol; SOA) and key tracer species, such as organosulfates. These processes are often driven by a combination of anthropogenic and biogenic emissions, and therefore their accurate representation in models is important for effective air quality management. Despite considerable progress, mechanistic understanding of some key aqueous processes is still lacking, and these pathways are incompletely represented in 3D atmospheric chemistry and air quality models. In this article, the concepts, historical context, and current state of the science of aqueous pathways of SOA formation are discussed.

  14. 14C-based Source Apportionment of Carbonaceous Aerosols in Switzerland for 2008 - 2012

    NASA Astrophysics Data System (ADS)

    Zotter, Peter; Ciobanu, Gabriela; Zhang, Yanlin; El-Haddad, Imad; Szidat, Sönke; Wacker, Lukas; Baltensperger, Urs; Prévôt, André

    2013-04-01

    Carbonaceous particles (total carbon, TC) are a major fraction of the fine aerosol and affect climate and human health. TC is classified into the sub-fractions elemental carbon (EC) and organic carbon (OC). EC originates only from fossil fuel combustion and biomass burning. OC can be emitted directly as primary organic aerosol from biogenic emissions, wood burning and fossil fuel combustion or can be formed in-situ in the atmosphere (secondary organic aerosol) (Szidat et al. 2006). Radiocarbon (14C) analysis is a direct and quantitative tool for distinguishing fossil and non-fossil sources, since 14C in fossil fuels is completely depleted whereas other sources have a contemporary 14C level. This study presents source apportionment results from the winter season over a time period of 5 years (2007/2008-2011/2012) using 14C measurements on aerosol filters collected simultaneously at 16 air quality monitoring stations across Switzerland. For every year 5 winter smog episode days were selected from which filters from all stations were analyzed. To resolve a good spatial variability 11 stations north and 5 stations south of the Alps were selected. This 14C data set is unique around the world concerning the number of analyzed filters and the duration. The filter sampling was conducted using high volume samplers with PM10 inlets and a time resolution of 24h. Separation of OC and EC was carried out using the THEODORE system (Szidat et al. 2004) and a Sunset EC/OC analyzer (Zhang et al. 2012), respectively. The resulting CO2 was cryo-trapped and sealed in glass ampoules for 14C measurements, performed with the Mini Carbon Dating System MICADAS (Ruff et al. 2007) at the Swiss Federal Institute of Technology (ETH) Zürich. The results for non-fossil (NF) OC (5 year average) are 81% ± 10% for north and 85% ± 8% for south of the Alps. ECNF values range from 31% to 53% north and from 36% to 66% south of the Alps. Both, the OCNF and ECNF show higher values south of the Alps

  15. A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

    NASA Technical Reports Server (NTRS)

    Liu, Hongyu; Moore, Richard; Hostetler, Chris A.; Ferrare, Richard Anthony; Fairlie, Thomas Duncan; Hu, Youngxiang; Chen, Gao; Hair, Johnathan W.; Johnson, Matthew S.

    2016-01-01

    The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

  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. 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.

  18. Determination of the sources and impacts of aerosols on clouds and orographic precipitation during CalWater

    NASA Astrophysics Data System (ADS)

    Prather, K. A.; Suski, K.; Cazorla, A.; Cahill, J. F.; Creamean, J.; Collins, D. B.; Ralph, F. M.; Cayan, D. R.; Rosenfeld, D.; DeMott, P. J.; Sullivan, R. C.; Comstock, J. M.; Leung, L.; Tomlinson, J. M.; Roberts, G. C.; Nenes, A.; Lin, J. J.

    2011-12-01

    Climate projections for the remainder of this century for the U.S. Southwest, including parts of California, suggest a drying trend (reductions ~ 10 -15 %). Thus, understanding factors which could potentially influence the amount and type of precipitation is critical to future water resources in California. Previous studies suggest aerosols transported from the Central Valley into the mountains may be reducing the amount of orographic precipitation in the Sierra Nevada mountain range, the key region for water storage in the snowpack. CalWater, which commenced in the Winter of 2009, is an ongoing multi-year, multi-agency field campaign to investigate the primary sources of aerosols influencing clouds and precipitation in this region. Single particle measurements, used in both ground as well as PNNL G1 aircraft measurements, in the recent campaign provide insight into the sources of aerosols impacting the clouds and precipitation. Biomass burning, Central Valley pollution, long range transported Asian dust and pollution, locally generated newly formed particles, and marine aerosols all show strong impacts on the cloud microphysical properties. This presentation will provide a brief overview of the objective and key findings from CalWater measurements of aerosols, precipitation, clouds, and meteorology conducted from 2009-2011 in this region.

  19. 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

  20. Solubility of aerosol trace elements: Sources and deposition fluxes in the Canary Region

    NASA Astrophysics Data System (ADS)

    López-García, Patricia; Gelado-Caballero, María Dolores; Collado-Sánchez, Cayetano; Hernández-Brito, José Joaquín

    2017-01-01

    African dust inputs have important effects on the climate and marine biogeochemistry of the subtropical North Atlantic Ocean. The impact of dust inputs on oceanic carbon uptake and climate is dependent on total dust deposition fluxes as well as the bioavailability of nutrients and metals in the dust. In this work, the solubility of trace metals (Fe, Al, Mn, Co and Cu) and ions (Ca, sulphate, nitrate and phosphate) has been estimated from the analysis of a long-time series of 109 samples collected over a 3-year period in the Canary Islands. Solubility is primarily a function of aerosol origin, with higher solubility values corresponding to aerosols with more anthropogenic influence. Using soluble fractions of trace elements measured in this work, atmospheric deposition fluxes of soluble metals and nutrients have been calculated. Inputs of dissolved nutrients (P, N and Fe) have been estimated for the mixed layer. Considering that P is the limiting factor when ratios of these elements are compared with phytoplankton requirements, an increase of 0.58 nM of P in the mixed layer (∼150 m depth) and in a year can be estimated, which can support an increase of 0.02 μg Chla L-1 y-1. These atmospheric inputs of trace metals and nutrients appear to be significant relative to the concentrations reported in this region, especially during the summer months when the water column is more stratified and deep-water nutrient inputs are reduced.

  1. A survey of effects of gaseous and aerosol pollutants on pulmonary function of normal males.

    PubMed

    Stacy, R W; Seal, E; House, D E; Green, J; Roger, L J; Raggio, L

    1983-01-01

    A total of 231 normal male human subjects were exposed for 4 hr to air, ozone, nitrogen dioxide, or sulfur dioxide; to sulfuric acid, ammonium bisulfate, ammonium sulfate, or ammonium nitrate aerosols; or to mixtures of these gaseous and aerosol pollutants. Only one concentration of each pollutant was used. This study, therefore, represents a preliminary survey, intended to allow direct comparison of studies to plan future research. During exposure each subject had two 15-min exercise sessions on a treadmill at 4 mph and 10% grade. Environmental conditions were mildly stressful, i.e., temperature = 30 degrees C and relative humidity = 60%. A battery of 19 measurements of pulmonary function was performed just prior to exposure (air control); 2 hr into the exposure, following the first exercise session; 4 hr into the exposure, following the second exercise session; and 24 hr after exposure. Significant differences were noted in specific airway resistance (SRAW), forced vital capacity (FVC), and forced expiratory flow at 50% of FVC (FEF50) and in related measurements in those experimental groups exposed to ozone or to ozone plus aerosols. None of the aerosols alone, nitrogen dioxide or sulfur dioxide alone, or mixtures of nitrogen dioxide or sulfur dioxide with aerosols produced significant effects. A distribution analysis of subject responsivity to ozone gave a normal distribution among subjects not exposed to ozone, and a distribution shifted to the right and skewed to the right among those exposed to ozone alone or in mixture, with no evidence of bimodal distribution of ozone sensitivity.

  2. SPATIAL AND TEMPORAL VARIABILITY OF MOBILE SOURCE AIR TOXICS IN THE DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY

    EPA Science Inventory

    Data from the first two years of the Detroit Exposure and Aerosol Research Study (DEARS) were evaluated to determine spatial and temporal characteristics in concentrations of mobile source air toxics (MSATs). Outdoor concentrations of MSATs were significantly higher in samples co...

  3. 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.

  4. Stochastic methods for aerosol chemistry: a compact molecular description of functionalization and fragmentation in the heterogeneous oxidation of squalane aerosol by OH radicals.

    PubMed

    Wiegel, A A; Wilson, K R; Hinsberg, W D; Houle, F A

    2015-02-14

    The heterogeneous oxidation of organic aerosol by hydroxyl radicals (OH) can proceed through two general pathways: functionalization, in which oxygen functional groups are added to the carbon skeleton, and fragmentation, in which carbon-carbon bonds are broken, producing higher volatility, lower molecular weight products. An ongoing challenge is to develop a quantitative molecular description of these pathways that connects the oxidative evolution of the average aerosol properties (e.g. size and hygroscopicity) to the transformation of free radical intermediates. In order to investigate the underlying molecular mechanism of aerosol oxidation, a relatively compact kinetics model is developed for the heterogeneous oxidation of squalane particles by OH using free radical intermediates that convert reactive hydrogen sites into oxygen functional groups. Stochastic simulation techniques are used to compare calculated system properties over ten oxidation lifetimes with the same properties measured in experiment. The time-dependent average squalane aerosol mass, volume, density, carbon number distribution of scission products, and the average elemental composition are predicted using known rate coefficients. For functionalization, the calculations reveal that the distribution of alcohol and carbonyl groups is controlled primarily by the initial OH abstraction rate and to lesser extent by the branching ratio between secondary peroxy radical product channels. For fragmentation, the calculations reveal that the formation of activated alkoxy radicals with neighboring functional groups controls the molecular decomposition, particularly at high O/C ratios. This kinetic scheme provides a framework for understanding the oxidation chemistry of a model organic aerosol and informs parameterizations of more complex systems.

  5. Radiative Forcing of the Pinatubo Aerosol as a Function of Latitude and Time

    NASA Technical Reports Server (NTRS)

    Bergstrom, R. W.; Kinne, S.; Russell, P. B.; Bauman, J. J.; Minnis, P.

    1996-01-01

    We present calculations of the radiative forcing of the Mt. Pinatubo aerosols as a function of latitude and time after the eruption and compare the results with GOES satellite data. The results from the model indicate that the net effect of the aerosol was to cool the earth-atmosphere system with the most significant radiative effect in the tropics (corresponding to the location of the tropical stratospheric reservoir) and at latitudes greater than 60 deg. The high-latitude maximum is a combined effect of the high-latitude peak in optical depth (Trepte et al 1994) and the large solar zenith angles. The comparison of the predicted and measured net flux shows relatively good agreement, with the model consistently under predicting the cooling effect of the aerosol.

  6. 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.

  7. 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.

  8. 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.

  9. 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

  10. 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

  11. 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.

  12. 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.

  13. The Missing Source of Glyoxal (CHOCHO) over China and Its Implications on Organic Aerosol Budgets

    NASA Astrophysics Data System (ADS)

    Liu, Z.; Wang, Y.; Zhao, C.; Vrekoussis, M.; Wittrock, F.; Richter, A.; Burrows, J. P.

    2011-12-01

    Recent comparisons between satellite observed and global model simulated glyoxal (CHOCHO) have consistently revealed a large unknown source of glyoxal over China [1, 2, 3]. We explore this missing glyoxal source by analyzing SCIAMACHY observed glyoxal columns using a Regional chEmical trAnsport Model (REAM). This missing source, which is quantified by the difference between SCIAMACHY observed and REAM simulated glyoxal columns (ΔCHOCHO), is found to mostly exist over regions with low emissions of biogenic glyoxal precursors (mainly isoprene) and collocate with dense population and high anthropogenic aromatic VOC emissions. We apply inverse modeling to constrain glyoxal precursor emissions based on SCIAMACHY measurements and find that this missing source is most likely caused by substantially underestimated aromatics (up to 20 times, varying spatially) in VOC emission inventories over China used in current regional and global models [4]. Analyses of in situ observations at ground level in Beijing assist to confirm this finding. The top-down estimated aromatics emission is 13.4 Tg/yr in total, about 6 times of the bottom-up estimate (2.4 Tg/yr), and leads to ~50% increase (from 23.2Tg/yr to 34.2 Tg/yr) of the total VOC emissions over China. The associated impact on regional oxidant levels is large, e.g. ~100% increase of PAN and ~30% increase of O3 in the afternoon. Furthermore, since aromatics are important precursors of secondary organic aerosol (SOA), such significant low bias of aromatics over China in current models could also contribute to the underestimated organic aerosols (OA) over the region found in previous modeling studies [5]. The implications of the quite uncertain emissions of SOA precursors over China on regional and global OA budgets are discussed. [1] Fu et al., 2008, J. Geophys. Res., 113, D15303, doi:10.1029/2007JD009505. [2] Myriokefalitakis et al.,2008, Atmos. Chem. Phys., 8, 4965-4981. [3] Stavrakou et al.,2009, Atmos. Chem. Phys., 9, 8431

  14. 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

  15. Impact of anthropogenic aerosols from global, East Asian, and non-East Asian sources on East Asian summer monsoon system

    NASA Astrophysics Data System (ADS)

    Wang, Qiuyan; Wang, Zhili; Zhang, Hua

    2017-01-01

    The impact of the total effects due to anthropogenic aerosols from global, East Asian, and non-East Asian sources on East Asian summer monsoon (EASM) system is studied using an aerosol-climate online model BCC_AGCM2.0.1_CUACE/Aero. The results show that the summer mean net all-sky shortwave fluxes averaged over East Asian monsoon region (EAMR) at the top of the atmosphere (TOA) and surface reduce by 4.8 and 5.0 W m- 2, respectively, due to the increases of global aerosol emissions in 2000 relative to 1850. Changes in radiations and their resulting changes in heat and water transport and cloud fraction contribute together to the surface cooling over EAMR in summer. The increases in global anthropogenic aerosols lead to a decrease of 2.1 K in summer mean surface temperature and an increase of 0.4 hPa in summer mean surface pressure averaged over EAMR, respectively. It is shown that the changes in surface temperature and pressure are significantly larger over land than ocean, thus decreasing the contrast of land-sea surface temperature and pressure. This results in the marked anomalies of north and northeast winds over eastern and southern China and the surrounding oceans in summer, thereby weakening the EASM. The summer mean precipitation averaged over the EAMR reduces by 12%. The changes in non-East Asian aerosol emissions play a more important role in inducing the changes of local temperature and pressure, and thus significantly exacerbate the weakness of the EASM circulation due to local aerosol changes. The weakening of circulation due to both is comparable, and even the effect of non-local aerosols is larger in individual regions. The changes of local and non-local aerosols contribute comparably to the reductions in precipitation over oceans, whereas cause opposite changes over eastern China. Our results highlight the importance of aerosol changes outside East Asia in the impact of the changes of anthropogenic aerosols on EASM.

  16. Insights into characteristics, sources, and evolution of submicron aerosols during harvest seasons in the Yangtze River delta region, China

    NASA Astrophysics Data System (ADS)

    Zhang, Y. J.; Tang, L. L.; Wang, Z.; Yu, H. X.; Sun, Y. L.; Liu, D.; Qin, W.; Canonaco, F.; Prévôt, A. S. H.; Zhang, H. L.; Zhou, H. C.

    2015-02-01

    Atmospheric submicron particulate matter (PM1) is one of the most significant pollution components in China. Despite its current popularity in the studies of aerosol chemistry, the characteristics, sources and evolution of atmospheric PM1 species are still poorly understood in China, particularly for the two harvest seasons, namely, the summer wheat harvest and autumn rice harvest. An Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was deployed for online monitoring of PM1 components during summer and autumn harvest seasons in urban Nanjing, in the Yangtze River delta (YRD) region of China. PM1 components were shown to be dominated by organic aerosol (OA, 39 and 41%) and nitrate (23 and 20%) during the harvest seasons (the summer and autumn harvest). Positive matrix factorization (PMF) analysis of the ACSM OA mass spectra resolved four OA factors: hydrocarbon-like mixed with cooking-related OA (HOA + COA), fresh biomass-burning OA (BBOA), oxidized biomass-burning-influenced OA (OOA-BB), and highly oxidized OA (OOA); in particular the oxidized BBOA contributes ~80% of the total BBOA loadings. Both fresh and oxidized BBOA exhibited apparent diurnal cycles with peak concentration at night, when the high ambient relative humidity and low temperature facilitated the partitioning of semi-volatile organic species into the particle phase. The fresh BBOA concentrations for the harvests are estimated as BBOA = 15.1 × (m/z 60-0.26% × OA), where m/z (mass-to-charge ratio) 60 is a marker for levoglucosan-like species. The (BBOA + OOA-BB)/ΔCO, (ΔCO is the CO minus background CO), decreases as a function of f44 (fraction of m/z 44 in OA signal), which might indicate that BBOA was oxidized to less volatile OOA, e.g., more aged and low volatility OOA (LV-OOA) during the aging process. Analysis of air mass back trajectories indicates that the high BB pollutant concentrations are linked to the air masses from the western (summer harvest) and southern (autumn harvest) areas.

  17. Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Ålesund, Svalbard): An electron microscopy study

    NASA Astrophysics Data System (ADS)

    Weinbruch, Stephan; Wiesemann, David; Ebert, Martin; Schütze, Katharina; Kallenborn, Roland; Ström, Johan

    2012-03-01

    Aerosol particles were collected at the Zeppelin Mountain Atmospheric Research Station (474 m asl) near Ny Ålesund (Svalbard, Norway) on 27 different days between July 2007 and December 2008. The size, morphology and chemical composition of 57,617 individual particles were studied by high-resolution scanning electron microscopy and energy-dispersive X-ray microanalysis. Based on chemical composition, morphology, mixing state and stability under electron bombardment, the particles were assigned to one of the following groups: sea salt, aged sea salt, Ca sulphates, Na sulphates, carbonates, soot, silicates, fly ashes, secondary aerosol, secondary aerosol plus sodium, secondary aerosol plus soot, mixed particles and others. Sea salt, aged sea salt, silicates and mixed particles (mixtures of sea salt, silicates and Ca sulphates) are the most abundant groups for particles with aerodynamic diameters > 0.5 μm, secondary aerosol, mixed particles and secondary aerosol with soot inclusions below 0.5 μm. Silicate fly ashes (major source coal burning) and metal fly ashes (from metallurgical high temperature processes) occur only at very low number concentrations. In contrast to previous work, the fly ash abundance is not correlated with air masses that crossed industrialized regions in Central and Eastern Europe, Scandinavia or Russia. These observations indicate a significant reduction of long-range transport of heavy metals to Svalbard. Soot (external and internally mixed with secondary aerosol) shows a pronounced seasonal pattern with a much lower abundance during summer compared to spring, autumn and winter. The soot abundance is not correlated with the air mass back-trajectories. During summer (July and August), soot was only observed when cruise ships were present in the area around Ny Ålesund (Kongsfjorden). Pronounced seasonal patterns were observed for the abundance of the mineral dust component which is generally lower in summer compared to the other seasons. The

  18. Measurement of Organic and Inorganic Chemical Tracers for Source Apportionment of Tropospheric Aerosols Collected During the ACE-Asia Experiment

    NASA Astrophysics Data System (ADS)

    Schauer, J. J.; Park, J.; Duvall, R.; Bae, M.; Shafer, M. M.; Chuang, P.; Chuang, P.; Kim, Y. J.

    2001-12-01

    Naturally occurring dust and anthropogenic air pollutants are important contributors to tropospheric aerosols and impact air quality and the radiative balance of the Earth's atmosphere. In order to better understand the relationship between the origin, chemical composition and ultimate impact of Asian aerosols on climate forcing, aerosol samples were collected as part of the ACE-Asia experiment for detailed chemical analysis. Atmospheric particulate matter samples were collected from March 27, 2001 through May 6, 2001 at the ACE-Asia ground station located on Cheju Island, Korea. During this period, this region is impacted by anthropogenic air pollution emissions from highly urbanized region of Asia and by desert dust originating from northeastern Asia. As part of the experiment, atmospheric particulate matter samplers were also collected in urban and desert locations in Asia that represent regional sources of particulate matter in Asia. Size resolved aerosol samples were analyzed for trace metals by using microwave assisted-acid digestion and ICP-MS analysis, speciated organic compounds using solvent extraction and GC-MS analysis, as well as soluble ions and elemental and organic carbon (ECOC). These measurements provide fingerprints for source apportionment of the atmospheric particulate matter samples collected at the Cheju Island sampling site. The use of these chemical tracers for apportionment of wind-driven long range transported desert dust, local crustal derived dust, biogenically and anthropogenically derived sulfate, specific urban combustion source, and fossil fuel combustion will be presented.

  19. 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.

  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. Physicochemical characterization of Capstone depleted uranium aerosols II: particle size distributions as a function of time.

    PubMed

    Cheng, Yung Sung; Kenoyer, Judson L; Guilmette, Raymond A; Parkhurst, Mary Ann

    2009-03-01

    The Capstone Depleted Uranium (DU) Aerosol Study, which generated and characterized aerosols containing DU from perforation of armored vehicles with large-caliber DU penetrators, incorporated a sampling protocol to evaluate particle size distributions. Aerosol particle size distribution is an important parameter that influences aerosol transport and deposition processes as well as the dosimetry of the inhaled particles. These aerosols were collected on cascade impactor substrates using a pre-established time sequence following the firing event to analyze the uranium concentration and particle size of the aerosols as a function of time. The impactor substrates were analyzed using proportional counting, and the derived uranium content of each served as input to the evaluation of particle size distributions. Activity median aerodynamic diameters (AMADs) of the particle size distributions were evaluated using unimodal and bimodal models. The particle size data from the impactor measurements were quite variable. Most size distributions measured in the test based on activity had bimodal size distributions with a small particle size mode in the range of between 0.2 and 1.2 microm and a large size mode between 2 and 15 microm. In general, the evolution of particle size over time showed an overall decrease of average particle size from AMADs of 5 to 10 microm shortly after perforation to around 1 microm at the end of the 2-h sampling period. The AMADs generally decreased over time because of settling. Additionally, the median diameter of the larger size mode decreased with time. These results were used to estimate the dosimetry of inhaled DU particles.

  2. Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time

    SciTech Connect

    Cheng, Yung-Sung; Kenoyer, Judson L.; Guilmette, Raymond A.; Parkhurst, MaryAnn

    2009-03-01

    The Capstone Depleted Uranium (DU) Aerosol Study, which generated and characterized aerosols containing depleted uranium from perforation of armored vehicles with large-caliber DU penetrators, incorporated a sampling protocol to evaluated particle size distributions. Aerosol particle size distribution is an important parameter that influences aerosol transport and deposition processes as well as the dosimetry of the inhaled particles. These aerosols were collected on cascade impactor substrates using a pre-established time sequence following the firing event to analyze the uranium concentration and particle size of the aerosols as a function of time. The impactor substrates were analyzed using beta spectrometry, and the derived uranium content of each served as input to the evaluation of particle size distributions. Activity median aerodynamic diameters (AMADs) of the particle size distributions were evaluated using unimodal and bimodal models. The particle size data from the impactor measurements was quite variable. Most size distributions measured in the test based on activity had bimodal size distributions with a small particle size mode in the range of between 0.2 and 1.2 um and a large size mode between 2 and 15 um. In general, the evolution of particle size over time showed an overall decrease of average particle size from AMADs of 5 to 10 um shortly after perforation to around 1 um at the end of the 2-hr sampling period. The AMADs generally decreased over time because of settling. Additionally, the median diameter of the larger size mode decreased with time. These results were used to estimate the dosimetry of inhaled DU particles.

  3. 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

  4. Sources and abundances of leaf waxes in aerosols in central Europe

    NASA Astrophysics Data System (ADS)

    Nelson, Daniel B.; Knohl, Alexander; Sachse, Dirk; Schefuß, Enno; Kahmen, Ansgar

    2017-02-01

    Atmospheric transport is an understudied mechanism for leaf wax hydrogen isotope applications that contributes to mobilizing and depositing these compounds on the surface of the Earth. While previous efforts have identified the importance of atmospheric leaf wax deposition in remote marine locations, the processes are not well constrained on land in temperate latitudes where lakes are common and sedimentary leaf wax hydrogen isotope values are an attractive tool for understanding past precipitation changes. This work presents results from a field study that was conducted in 2010 and 2011 at Hainich National Park, Germany in order to evaluate the quantity and sources of leaf waxes in the atmosphere. Aerosols were sampled at approximately weekly intervals inside the forest canopy, and n-alkane distributions and hydrogen isotope values were compared with those from major tree species surrounding the sampling site. Despite sampling in what was expected to be a major production center, the distribution and hydrogen isotope values of atmospheric n-alkanes bore little resemblance to those of the local vegetation. Comparison with local meteorological data and to 10-day and 36-h back air mass trajectories indicated shifting effects of winds and temperature, and that mesoscale transport processes were more important than long-range mechanisms. Back trajectories also highlighted source effects, with easterly winds coinciding with relatively lower leaf wax hydrogen isotope values from more continental regions. These results suggest that leaf wax aerosols average over spatial scales that exceed typical surface catchment areas for small lake systems, even in forested areas, yet that the area over which these compounds are derived is still relatively regional. Depositional fluxes were also estimated in order to assess the potential importance of atmospheric transport to sedimentary archives. Although difficult to constrain, these estimates suggest that atmospheric deposition may

  5. 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.

    2014-12-01

    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 photometer (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of submicron particulate matter (PM1) in Lanzhou, northwest China, during 11 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 105 μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. Organic aerosol (OA) on average 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 organic mass spectra 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-emission related OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ~ 07:00 and 15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak between ~ 08:00-13:00. The later morning and early afternoon maximum in the diurnal profiles of secondary aerosol species was likely caused by downward mixing of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during nighttime. The mass spectrum of SV-OOA was

  6. Organic composition and source apportionment of fine aerosol at Monterrey, Mexico, based on organic markers

    NASA Astrophysics Data System (ADS)

    Mancilla, Y.; Mendoza, A.; Fraser, M. P.; Herckes, P.

    2016-01-01

    attribution results obtained using the CMB (chemical mass balance) model indicate that emissions from motor vehicle exhausts are the most important, accounting for the 64 % of the PM2.5, followed by meat-cooking operations with 31 % The vegetative detritus and biomass burning had the smallest contribution (2.2 % of the PM2.5). To our knowledge, this is only the second study to explore the organic composition and source apportionment of fine organic aerosol based on molecular markers in Mexico and the first for the MMA. Particularly molecular marker were quantified by solvent extraction with dichloromethane, derivatization, and gas chromatography with mass spectrometry (GC/MS).

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

    SciTech Connect

    Annette Rohr

    2006-03-01

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

  8. Organic composition of atmospheric urban aerosol: Variations and sources of aliphatic and polycyclic aromatic hydrocarbons

    NASA Astrophysics Data System (ADS)

    Mazquiarán, Miguel A. Barrero; Cantón Ortiz de Pinedo, Lourdes

    2007-09-01

    The non-polar organic composition of airborne particulate matter was analysed over a two year period in an urban area under oceanic climate conditions (Errenteria, Basque Country, Spain). In addition, the distribution of polycyclic aromatic hydrocarbons (PAH) among different aerosol particle sizes was determined. Clues as to the origin of various particle types were gained by using scanning electron microscopy to view the morphology of the particulates in each size fraction. Samples were collected on glass fibre filters and analysed by means of soxhlet extraction and gas chromatography (either with a flame ionization detector or coupled to a mass spectrometry). In general, total PAH levels were moderate (0.96-50 ng m - 3 ) as compared to other studies conducted in Europe, and showed clear seasonal variation with maxima in winter and minima in summer. Vehicular traffic was identified as a major source of PAHs in the study area. Regarding particle size, a bimodal distribution was observed. The large sized particles exhibited an apparent seasonal variation with higher concentrations in winter than in summer. The dependences between particle size, PAH distribution and meteorological variables were studied with multivariate statistics. Three main sources of organic compounds were identified: combustion, vegetation, and atmospheric oxidation.

  9. Seasonal pattern of source and transport processes of natural and anthropic surfactants in coastal aerosol (Tuscany coast - Italy).

    NASA Astrophysics Data System (ADS)

    Becagli, Silvia; Ghedini, Costanza; Peeters, Stephane; Rottiers, Andre; Traversi, Rita; Udisti, Roberto; Jalba, Adriana; Dayan, Uri; Temara, Ali

    2010-05-01

    Surface active agents have been detected in coastal aerosols for decades. Their partial hydrophilicity could affect the hygroscopicity of aerosol particles. The ecological significance of surface active substances has thus been much debated, including pre-biotic processes, global climate changes by influencing optical properties and Cloud Condensation Nuclei forming ability, and in decline of coastal vegetation exposed to sea spray. Based on results obtained using non specific analytical methods (e.g., Methylene Blue coloration - MBAS), MBAS reactive surface active agents, like surfactants used in detergents, have been singled out as one of the causing factors of some of these aerosol effects. In order to increase the knowledge on the atmospheric concentration, source and distribution of surfactants, an aerosol sampling campaign was arranged at San Rossore (Pisa): a costal site located in the NW Mediterranean sea.The aerosols were collected at a distance of 500 meters from the sea, on the roof of a building at about 10 m above the sea level. A preliminary spot sampling campaign, at weekly resolution, was carried out in February-March 2006, using an Andersen 8-stages impactor. The main sampling campaign covered more than one year (from March 2007 to June 2008) and the sampling was accomplished at daily resolution by two sequential aerosol samplers operating in parallel way. The samplers were equipped with PM10 and PM2.5 sampling heads designed according to EN12341 European rule. After weighting, the filter was analysed for ionic content by ion chromatography. The concentration of the anthropogenic surfactant LAS was measured in all collected samples using specific analytical techniques (LC-MS-MS) and was compared with the MBAS signal. In the PM10 aerosol, MBAS concentration was on average 887 ng/m3 MBAS, while the LAS concentration detected in the same aerosol samples represent less than 5% of the total MBAS signal. Analysis of the temporal trends in LAS and MBAS in

  10. Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

    NASA Astrophysics Data System (ADS)

    Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

    2010-03-01

    This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

  11. A Novel Approach for Determining Source-Receptor Relationships of Aerosols in Model Simulations

    NASA Astrophysics Data System (ADS)

    Ma, P.; Gattiker, J.; Liu, X.; Rasch, P. J.

    2013-12-01

    The climate modeling community usually performs sensitivity studies in the 'one-factor-at-a-time' fashion. However, owing to the a-priori unknown complexity and nonlinearity of the climate system and simulation response, it is computationally expensive to systematically identify the cause-and-effect of multiple factors in climate models. In this study, we use a Gaussian Process emulator, based on a small number of Community Atmosphere Model Version 5.1 (CAM5) simulations (constrained by meteorological reanalyses) using a Latin Hypercube experimental design, to demonstrate that it is possible to characterize model behavior accurately and very efficiently without any modifications to the model itself. We use the emulator to characterize the source-receptor relationships of black carbon (BC), focusing specifically on describing the constituent burden and surface deposition rates from emissions in various regions. Our results show that the emulator is capable of quantifying the contribution of aerosol burden and surface deposition from different source regions, finding that most of current Arctic BC comes from remote sources. We also demonstrate that the sensitivity of the BC burdens to emission perturbations differs for various source regions. For example, the emission growth in Africa where dry convections are strong results in a moderate increase of BC burden over the globe while the same emission growth in the Arctic leads to a significant increase of local BC burdens and surface deposition rates. These results provide insights into the dynamical, physical, and chemical processes of the climate model, and the conclusions may have policy implications for making cost-effective global and regional pollution management strategies.

  12. Concentrations and sources of aerosol ions and trace elements during ANTCI-2003

    NASA Astrophysics Data System (ADS)

    Arimoto, R.; Zeng, T.; Davis, D.; Wang, Y.; Khaing, H.; Nesbit, C.; Huey, G.

    As part of the Antarctic Tropospheric Chemistry Investigation (ANTCI), bulk aerosol-particle samples collected at the South Pole were analyzed for nitrate, sulfate, methanesulfonate (MSA), selected trace elements and radionuclides. The samples were collected in the same manner as in the Investigation of Sulfur Chemistry in the Antarctic Troposphere (ISCAT) campaigns of 1998 and 2000. The ANTCI mean sulfate (124 ng m -3) and MSA (9.1 ng m -3) concentrations were comparable to those during ISCAT, but high MSA and sodium and high MSA/sulfate in late November/early December indicated pervasive maritime influences during that time. Trajectory analyses indicate that the Weddell Sea and the Southern Ocean near Wilkes Land were probable sources for the ocean-derived sulfate. The transport of marine air occurs mainly in the buffer layer or free troposphere, and the rapid oxidation of biogenic sulfur to SO 2 appears to be the basis for the observed low MSA/sulfate ratios. Elements typically associated with mineral dust (Al, Fe, K) and other elements with continental sources (Pb, Sb, Zn) had higher concentrations during ANTCI than ISCAT. The mean filterable nitrate (f-NO 3-) concentration (280 ng m -3) also was conspicuously higher than during ISCAT (39 and 150 ng m -3). Several peaks in f-NO 3- were synchronous with those for MSA and sulfate, but some samples had high f-NO 3- but neither high MSA nor sulfate. While there is some evidence that nitrate or nitric acid is transported to SP from distant sources, local emissions of nitrogen oxides from the snow are a far more important source overall.

  13. Chemical characterization of fine organic aerosol for source apportionment at Monterrey, Mexico

    NASA Astrophysics Data System (ADS)

    Mancilla, Y.; Mendoza, A.; Fraser, M. P.; Herckes, P.

    2015-07-01

    , source attribution results obtained using the CMB model indicate that emissions from motor vehicle exhausts are the most important, accounting for the 64 % of the PM2.5. The vegetative detritus and biomass burning had the smallest contribution (2.2 % of the PM2.5). To our knowledge, this is the second study to explore the broad chemical characterization of fine organic aerosol in Mexico and the first for the MMA.

  14. Aerosol measurements during COPE: composition, size, and sources of CCN and INPs at the interface between marine and terrestrial influences

    NASA Astrophysics Data System (ADS)

    Taylor, Jonathan W.; Choularton, Thomas W.; Blyth, Alan M.; Flynn, Michael J.; Williams, Paul I.; Young, Gillian; Bower, Keith N.; Crosier, Jonathan; Gallagher, Martin W.; Dorsey, James R.; Liu, Zixia; Rosenberg, Philip D.

    2016-09-01

    Heavy rainfall from convective clouds can lead to devastating flash flooding, and observations of aerosols and clouds are required to improve cloud parameterisations used in precipitation forecasts. We present measurements of boundary layer aerosol concentration, size, and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation-mode aerosol mass loadings were typically 2-3 µg m-3 (corrected to standard cubic metres at 1013.25 hPa and 273.15 K), the majority of which was sulfuric acid over the sea, or ammonium sulfate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ˜ 150-280 cm-3 at 0.1 % and 400-500 cm-3 at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100 to 500 cm-3. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulfate, meaning marine sulfate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to previous measurements of sea spray OA and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulfate, and black carbon. The CCN concentrations here were around 6 times higher than in the clean cases, and the cloud drop number concentrations were 3-4 times higher. Sources of ice-nucleating particles (INPs) were assessed by comparing different parameterisations used to predict INP concentrations, using measured

  15. Aerosol measurements at L'Aquila EARLINET station in central Italy: Impact of local sources and large scale transport resolved by LIDAR

    NASA Astrophysics Data System (ADS)

    Pitari, Giovanni; Di Carlo, Piero; Coppari, Eleonora; De Luca, Natalia; Di Genova, Glauco; Iarlori, Marco; Pietropaolo, Ermanno; Rizi, Vincenzo; Tuccella, Paolo

    2013-01-01

    Surface measurements of multi-channel aerosol mass concentration are analyzed together with LIDAR observations at L'Aquila, a central Italy site part of the EARLINET network (http://www.earlinet.org/), with the main purpose of discriminating aerosol particles originated from in-situ sources and those transported from remote sites, and their effects on local aerosol load and on the aerosol optical depth. Four major episodes of both Saharan desert and forest fire aerosol transport were observed during spring-summer months of 2007. The analysis of these events shows that at the ground surface the aerosol mass concentration increase due to desert dust particles is about 160% of the PMcoarse, whereas forest fires increase the PM1 by about 150%, with respect to typical reference unperturbed conditions during the same time period. Calculation of the aerosol optical depth (AOD) from the LIDAR retrieved aerosol extinction at 351 nm shows that the corresponding increases in AOD are 95% for Saharan dust and 220% in case of forest fires. These results show that in a site impacted by aerosol transport from the desert and frequent forest fires, the first has the bigger effect in terms of local aerosol load in the coarse mode, whereas the latter impacts more the PM1 and the UV aerosol extinction and optical depth. A well tested radiative transfer model (TUV, Madronich and Floke, 1998), extended to the solar near infrared spectrum, has been used to calculate the top-of-atmosphere radiative change due to these transported aerosols: the calculated change is of the order of 0.5-1 W/m2 for forest fire events end 1-2 W/m2 for Saharan dust. The larger impact of desert aerosols is due to their much larger effective radius with respect to forest fire aerosols, whose scattering efficiency rapidly declines for solar wavelengths in the visible and near infrared range.

  16. Using Thermal-Optical Analysis to Examine the OC-EC Split that Characterizes Ambient and Source Emissions Aerosols

    NASA Astrophysics Data System (ADS)

    Khan, B.; Hays, M. D.; Geron, C.; Jetter, J.

    2010-12-01

    Thermal-optical analysis (TOA) is typically used to measure OC-EC (organic carbon-elemental carbon) ratio in atmospheric aerosols. The present study utilizes a single dual-optics carbon aerosol analyzer to examine the effects of temperature-programming and optics on the OC-EC ratios. The OC-EC ratios for a variety of atmospheric and source emissions aerosols were measured using a National Institute of Occupational Safety and Health method (NIOSH 5040), the Interagency Monitoring of Protected Visual Environments method (IMPROVE), and a modified NIOSH 5040 method (referred in this paper as NIST-EPA). Use of the dual-optics instrument allowed simultaneous monitoring of the reflectance (TOR) and transmission (TOT) during each thermal protocol. Results showed no statistical difference between NIST-EPA and NIOSH OC-EC ratios for residential cookstove emissions and for an urban aerosol collected in Nairobi, Kenya. However, the OC-EC ratios for diesel exhaust (NIST [TOT and TOR]) and for a denuded rural North Carolina forest aerosol (NIST [TOT]) were significantly greater than the corresponding NIOSH values. Significantly lower IMPROVE (TOT and TOR) OC-EC ratios, compared to NIST-EPA and NIOSH, may be ascribed to the lower temperature protocol of this method. The ratio of TOT-to-TOR for the OC-EC ratio ranged between 1.37 - 1.71 (residential cookstoves), 1.05 - 1.24 (diesel exhaust), 1.63 - 2.23 (rural), and 0.80 - 1.12 (urban) for the three methods. Aerosols containing components susceptible to charring (such as water soluble organic compounds typical of rural and cookstove aerosols) tend to show the higher OC-EC variability among the methods when compared to diesel-impacted aerosols, which showed little to no detectable pyrolyzed carbon (PyC). Different sample types, due to their various chemical compositions, behave differently under dissimilar thermal and optical conditions, such that the search for a “universal” thermal-optical method for all sample types remain

  17. In-situ determination of atmospheric aerosol composition as a function of hygroscopic growth

    SciTech Connect

    Herich, Hanna; Kammermann, Lukas; Gysel, Martin; Weingartner, E.; Baltensperger, Urs; Lohmann, U.; Cziczo, Daniel J.

    2008-08-30

    An in-situ measurement setup to determine the chemical composition of aerosols as a function of hygroscopicity is presented. This has been done by connecting a custom-built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) and an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS), commercially available from TSI (Model 3800). Single particle bipolar mass spectra from aerosols leaving the HTDMA could thus be obtained as a function of the hygroscopic growth factor. For these studies the HTDMA was set at a relative humidity of 82% and particles with a dry diameter of 260 nm were selected. The setup was first laboratory tested after which field experiments were performed. Two datasets were obtained during wintertime 2007 in Switzerland: the first in the urban Zurich environment and the other at the remote high alpine research station Jungfraujoch (JFJ). In Zurich several thousand mass spectra were obtained in less than two days of sampling due to a high aerosol loading. At the JFJ, due to low particle concentrations in free tropospheric airmasses, a longer sampling period was required. Both in Zurich and at the JFJ two different growth factor modes were observed. Results from these two locations show that most aerosol particles were a mixture of several compounds. A large contribution of organics and combustion species was found in the less hygroscopic growth mode for both locations. Non-combustion refractory material (e.g. metals, mineral dust, and fly ash) was also highly enhanced in the non-hygroscopic particles. Sulfate, normally considered highly soluble, was found to be a constituent in almost all particles independent of their hygroscopic growth factor.

  18. Effects of Microbial Aerosol in Poultry House on Meat Ducks' Immune Function.

    PubMed

    Yu, Guanliu; Wang, Yao; Wang, Shouguo; Duan, Changmin; Wei, Liangmeng; Gao, Jing; Chai, Tongjie; Cai, Yumei

    2016-01-01

    The aim of this study was to evaluate effects of microbial aerosols on immune function of ducks and shed light on the establishment of microbial aerosol concentration standards for poultry. A total of 1800 1-d-old cherry valley ducks were randomly divided into five groups (A, B, C, D, and E) with 360 ducks in each. To obtain objective data, each group had three replications. Concentrations of airborne bacteria, fungi, endotoxin in different groups were created by controlling ventilation and bedding cleaning frequency. Group A was the control group and hygienic conditions deteriorated progressively from group B to E. A 6-stage Andersen impactor was used to detect the aerosol concentration of aerobes, gram-negative bacteria, fungi, and AGI-30 microbial air sampler detect the endotoxin, and Composite Gas Detector detect the noxious gas. In order to assess the immune function of meat ducks, immune indicators including H5 AIV antibody titer, IgG, IL-2, T-lymphocyte transformation rate, lysozyme and immune organ indexes were evaluated. Correlation coefficients were also calculated to evaluate the relationships among airborne bacteria, fungi, endotoxin, and immune indicators. The results showed that the concentration of airborne aerobe, gram-negative bacteria, fungi, endotoxin have a strong correlation to H5 AIV antibody titer, IgG, IL-2, T-lymphocyte transformation rate, lysozyme, and immune organ indexes, respectively. In addition, when the concentration of microbial aerosol reach the level of group D, serum IgG (6-8 weeks), lysozyme (4 week) were significantly higher than in group A (P < 0.05); serum IL-2 (7 and 8 weeks), T-lymphocyte transformation rate, lysozyme (7 and 8 weeks), spleen index (6 and 8 weeks), and bursa index (8 week) were significantly lower than in group A (P < 0.05 or P < 0.01). The results indicated that a high level of microbial aerosol adversely affected the immune level of meat ducks. The microbial aerosol values in group D provide a basis for

  19. Effects of Microbial Aerosol in Poultry House on Meat Ducks' Immune Function

    PubMed Central

    Yu, Guanliu; Wang, Yao; Wang, Shouguo; Duan, Changmin; Wei, Liangmeng; Gao, Jing; Chai, Tongjie; Cai, Yumei

    2016-01-01

    The aim of this study was to evaluate effects of microbial aerosols on immune function of ducks and shed light on the establishment of microbial aerosol concentration standards for poultry. A total of 1800 1-d-old cherry valley ducks were randomly divided into five groups (A, B, C, D, and E) with 360 ducks in each. To obtain objective data, each group had three replications. Concentrations of airborne bacteria, fungi, endotoxin in different groups were created by controlling ventilation and bedding cleaning frequency. Group A was the control group and hygienic conditions deteriorated progressively from group B to E. A 6-stage Andersen impactor was used to detect the aerosol concentration of aerobes, gram-negative bacteria, fungi, and AGI-30 microbial air sampler detect the endotoxin, and Composite Gas Detector detect the noxious gas. In order to assess the immune function of meat ducks, immune indicators including H5 AIV antibody titer, IgG, IL-2, T-lymphocyte transformation rate, lysozyme and immune organ indexes were evaluated. Correlation coefficients were also calculated to evaluate the relationships among airborne bacteria, fungi, endotoxin, and immune indicators. The results showed that the concentration of airborne aerobe, gram-negative bacteria, fungi, endotoxin have a strong correlation to H5 AIV antibody titer, IgG, IL-2, T-lymphocyte transformation rate, lysozyme, and immune organ indexes, respectively. In addition, when the concentration of microbial aerosol reach the level of group D, serum IgG (6–8 weeks), lysozyme (4 week) were significantly higher than in group A (P < 0.05); serum IL-2 (7 and 8 weeks), T-lymphocyte transformation rate, lysozyme (7 and 8 weeks), spleen index (6 and 8 weeks), and bursa index (8 week) were significantly lower than in group A (P < 0.05 or P < 0.01). The results indicated that a high level of microbial aerosol adversely affected the immune level of meat ducks. The microbial aerosol values in group D provide a basis for

  20. Radiocarbon-Based Source apportionment of Elemental Carbon Aerosols at Seoul, South Korea

    NASA Astrophysics Data System (ADS)

    Shakerian Ghahferrokhi, Farid; Ahn, Jinho; Czimczik, Claudia I.; Holden, Sandra; Park, JinSoo

    2016-04-01

    In this study, 10 samples of PM2.5 (aerosol particle with diameter less than 2.5 μm) were collected in the Northeast of Seoul (37.60o N, 127.05o E), South Korea, over 2-4 day periods in May and June of 2015 with a high volume air sampler. The samples were analyzed for their bulk carbon (TC) and nitrogen (N) elemental and stable isotope composition with EA-IRMS. Elemental carbon (EC) was quantified with the Swiss_4S protocol using a Sunset OC/EC analyzer. Both, TC and EC were analyzed for their radiocarbon (14C) content via accelerator mass spectrometry. The mass and isotopic composition of organic carbon (OC) was quantified by (isotope) mass balance. TC loads were 6.6 +/- 1.5 ug C m-3 air (ave. +/- sd; range 4.7-9.7), with a ∆14C ranging from 240 to -446 per mill and a δ13C of -25.4+/-0.3 per mill. EC was a minor fraction of TC (7.2+/-1.9% or 0.5+/-0.2 ug C m-3 air). EC was strongly depleted in 14C (∆14C = -915 to -819 per mill), with fossil sources accounting for 88+/-3% of EC (6.3+/-1.7% of TC). OC was enriched in 14C above natural levels (∆14C = -401 to 309 per mill), and thus could not be partitioned into fossil and modern sources. Local wind directions showed that air masses originated from the South, demonstrating that regional sources may be the crucial contributor to PM pollution in Seoul during that sampling period (early summer).

  1. Long-range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the western Mediterranean basin

    NASA Astrophysics Data System (ADS)

    Ancellet, Gerard; Pelon, Jacques; Totems, Julien; Chazette, Patrick; Bazureau, Ariane; Sicard, Michaël; Di Iorio, Tatiana; Dulac, Francois; Mallet, Marc

    2016-04-01

    Long-range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground-based and airborne lidar measurements were deployed in the western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three-dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Minorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agrees very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (i) pure BB layer, (ii) weakly dusty BB, (iii) significant mixture of BB and dust transported from the trade wind region, and (iv) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at an altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS aerosol optical depth horizontal distribution during this episode over the western Mediterranean Sea shows that the Canadian fire contributions were as large as the direct northward dust outflow

  2. 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)

    Budisulistiorini, S. H.; Baumann, K.; Edgerton, E. S.; Bairai, S. T.; Mueller, S.; Shaw, S. L.; Knipping, E. M.; Gold, A.; Surratt, J. D.

    2015-08-01

    A yearlong near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia) and rural (Look Rock, Tennessee) 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 (50-76 %) and inorganic sulfate (12-31 %). 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 one 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 (OOA), isoprene-derived epoxydiol (IEPOX) OA (IEPOX-OA), and 91Fac OA (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 30-66 % of total OA mass. HOA was also observed during the entire year only at the urban site (15-24 % 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 proposed as an additional marker for IEPOX-OA, as it is shown to correlate well with the m/z 82 ion shown to be associated with the aerosol mass spectrum of

  3. Sugars as source indicators of biogenic organic carbon in aerosols collected above the Howland Experimental Forest, Maine

    NASA Astrophysics Data System (ADS)

    Medeiros, Patricia M.; Conte, Maureen H.; Weber, John C.; Simoneit, Bernd R. T.

    Bulk aerosols (>1 μm) were collected continuously above the canopy at the Howland Experimental Forest, Maine, USA from May to October 2002. Each sample integrated over an approximately 2-week period. Mono- and disaccharide sugars were extracted using a microscale technique and were analyzed as their TMS derivatives by gas chromatography-mass spectrometry (GC-MS). Concentrations of total aerosol sugars ranged from 10 to 180 ng m -3. Glucose was the most abundant sugar (40-75% of the total sugars). The monosaccharides arabinose, fructose, galactose, mannose, arabitol and mannitol, and the disaccharides sucrose, maltose and mycose (aka trehalose) were also present in lower concentrations. The sugar composition in the aerosols varied seasonally. Fructose and sucrose were prevalent in early spring and decreased in relative abundance as the growing season progressed. Sugar polyols (arabitol and mannitol) and the disaccharide mycose (a fungal metabolite) were more prevalent in autumn during the period of leaf senescence. The changes in the sugar composition in the aerosol samples appear to reflect the seasonality of sugar production and utilization by the ecosystem. Plant waxes were present as significant components also indicating an input from biogenic background. Smoke plumes from Quebec forest fires passed over the Howland site in early July 2002. Levoglucosan, a biomarker of biomass burning, increased by an order of magnitude in the aerosol samples collected during this time. Glucose, mannose, arabinose, galactose, and also, plant waxes increased in concentration by factors of 2-5 in the smoke-impacted samples, indicating that wildfires enhance atmospheric emissions of uncombusted organic compounds. In contrast, concentrations of fructose, sugar polyols and disaccharides were not significantly higher in the smoke-impacted samples and indicated that biomass burning was not a significant source of these compounds in the aerosols.

  4. Impact of interannual variations in sources of insoluble aerosol species 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.

    2015-06-01

    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 (2011). Although differences in the sources of insoluble residues 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 insoluble 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. Ultimately, the goal is to use such observations to improve the mechanistic linkages between aerosol sources and precipitation processes

  5. Black carbon aerosol in winter northeastern Qinghai-Tibetan Plateau, China: the source, mixing state and optical property

    NASA Astrophysics Data System (ADS)

    Wang, Q. Y.; Huang, R.-J.; Cao, J. J.; Tie, X. X.; Ni, H. Y.; Zhou, Y. Q.; Han, Y. M.; Hu, T. F.; Zhu, C. S.; Feng, T.; Li, N.; Li, J. D.

    2015-11-01

    Black carbon (BC) aerosol at high altitudes of the Qinghai-Tibetan Plateau has potential effects on the regional climate and hydrological cycle. An intensive measurement campaign was conducted at Qinghai Lake (~ 3200 m above sea level) at the edge of the northeastern Qinghai-Tibetan Plateau during winter using a ground-based single particle soot photometer (SP2) and a photoacoustic extinctiometer (PAX). The average concentration of refractory BC (rBC) and number fraction of coated rBC were found to be 160 ± 190 ng m-3 and 59 % for the entire campaign, respectively. Significant enhancements of rBC loadings and number fraction of coated rBC were observed during a pollution episode, with an average value of 390 ng m-3 and 65 %, respectively. The mass size distribution of rBC particles showed log-normal distribution, with a peak diameter of ~ 187 nm regardless of the pollution level. Five-day backward trajectory analysis suggests that the air masses from north India contributed to the increased rBC loadings during the campaign. The potential source contribution function (PSCF) model combined with the fire counts map further proves that biomass burning from north India is an important potential source influencing the northeastern Qinghai-Tibetan Plateau during the pollution episode. The rBC mass absorption cross section (MACrBC) at λ = 532 nm was slightly larger in clean days (14.9 m2 g-1) than during the pollution episode (9.3 m2 g-1), likely due to the effects of brown carbon and the uncertainty of the MACrBC calculation. The MACrBC was positively correlated with number fraction of coated rBC during the pollution episode with an increasing rate of 0.18 (m2 g-1) %-1. The number fraction of coated rBC particles showed positive correlation with light absorption, suggesting that the increase of coated rBC particles will enhance the light absorption. Compared to rBC mass concentration, rBC mixing sate is more important in determining absorption during the pollution

  6. On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol - Part 1: Source fluxes

    NASA Astrophysics Data System (ADS)

    Fuentes, E.; Coe, H.; Green, D.; de Leeuw, G.; McFiggans, G.

    2010-10-01

    , which revealed a higher production of particles with Dp0<100 nm at regions with high biological activity. These findings suggest that the increase in the atmospheric aerosol modal sizes from winter to summer, reported by long-term observations in North Atlantic waters, is not directly due to an impact of the higher primary organic matter production occurring during warm periods. A novel sub-micrometric size-resolved source flux function, explicitly defined as a function of the diatomaceous exudate concentration, was derived from the size distribution measurements and the estimation of the fractional whitecap coverage. According to the defined parameterisation, a 300 μM OC<0.2 μm concentration of diatomaceous exudate in seawater produces an overall increment in the total source particle flux of ~20% with respect to the organics-free seawater case. The effect increases with decreasing particle size for Dp0<100 nm, resulting in multiplicative factors between 1.02-2 with respect to the particle flux generated from seawater devoid of marine organics. The total source flux derived from the presented parameterisation was compared to recent definitions of sea-spray source fluxes based on laboratory and field observations in the literature.

  7. Quantification of long-term primary and secondary source contributions to carbonaceous aerosols.

    PubMed

    Shi, Guoliang; Peng, Xing; Liu, Jiayuan; Tian, Yingze; Song, Danlin; Yu, Haofei; Feng, Yinchang; Russell, Armistead G

    2016-12-01

    Ambient fine particulate matter samples were collected during 2009-2013 in Chengdu, a megacity in western China, and the samples were speciated into organic carbon (OC), elemental carbon (EC), char-EC, soot-EC, eight carbon fractions, inorganic elements and water-soluble ions. Char-EC and soot-EC contribute to the better understanding of the sources and properties of EC. The highest levels of most carbon fractions were found in winter and May. The higher OC/EC ratio in winter suggests higher SOC fraction in winter, and higher char-EC/soot-EC ratio in May are the direct consequences of straw burning activities. Source contributions to PM2.5 and carbonaceous aerosols were quantified using the ME2 receptor model. Major contributors to OC in PM2.5 are vehicular exhaust (36.5%), coal combustion & straw burning (35.2%) and SOC (27.0%). The first two categories also contributed 51.4% and 49.3% of char-EC in PM2.5. Vehicular exhaust dominated soot-EC, contributing 63.0% to soot-EC in PM2.5. SOC contributed to high OC levels in winter due to the increase of precursor emissions and stable meteorological conditions. Coal combustion & straw burning show higher contributions to OC, char-EC and soot-EC in winter months and in May, which can be explained, in part, by increased coal consumption in winter and straw burning activities in May. Vehicular exhaust contributions are not strongly associated with monthly nor weekday-weekend patterns, resulting in that soot-EC vary insignificantly by month nor by weekday.

  8. Source apportionment of organic aerosol across Houston, TX during DISCOVER-AQ

    NASA Astrophysics Data System (ADS)

    Yoon, S.; Clark, A. E.; Ortiz, S. M.; Usenko, S.; Sheesley, R. J.

    2015-12-01

    As part of the ground-based sampling efforts during DISCOVER-AQ's Houston month-long campaign in September 2013, atmospheric particulate matter (PM) samples were collected at four sites: Moody Tower (urban), Manvel Croix (southern suburb), Conroe (northern suburb), and La Porte (urban industrial). The Houston metropolitan area, especially the Houston Ship Channel, is a densely industrialized urban city with large concentrations of petroleum refining, petrochemical manufacturing, and heavy traffic during peak hours. Due to these and other emission sources, the area is heavily impacted by ambient PM. This study will be looking at fine PM (diameter less than 2.5µm, PM2.5) from all four sites. PM2.5fraction is relevant for understanding fate and transport of organic contaminants and is widely known to negatively impact human health. Chemical analysis including radiocarbon (14C) and organic tracer measurements (polycyclic aromatic hydrocarbons, alkanes, hopanes, steranes, and levoglucosan) were used for source apportionment. The 14C measurements constrained CMB results to estimate both primary and secondary contributions to total organic carbon (TOC). Results indicate that Moody Tower had consistent primary motor vehicle exhaust contribution (18-27%) and a fossil secondary organic aerosol (SOA) contribution from 5-33% depending on atmospheric conditions. Conroe had a lower contribution of motor vehicle exhaust (5-10%) and similarly variable fraction of fossil SOA (4-25%). Manvel Croix had an interim motor vehicle contribution (9-15%) with a variable fossil SOA (5-30%). For contemporary OC, there was minimal contribution of wood smoke during examined weeks (0-9%) but larger contributor of biogenic SOA ranging from 40-75% at Moody Tower, 56-81% at Manvel Croix and 60-79% at Conroe. Overall, the motor vehicle contribution was consistent at each site during the analysis week, biogenic SOA was consistently high, while fossil SOA showed the most variability.

  9. Identification and characterisation of local aerosol sources using high temporal resolution measurements.

    PubMed

    Contini, D; Donateo, A; Cesari, D; Belosi, F; Francioso, S

    2010-09-01

    Aerosol and gaseous pollution measurements were carried out at an urban background site in the south of Italy located near an industrial complex. Collection of 24 h samples of PM10 and PM2.5 and successive chemical quantification of metals were performed. Data were compared with measurements taken at a suburban background site, located at 25 km distance. The comparison showed the presence of an industrial contribution with a well defined chemical emission profile, similar, in terms of metals content, to urban emissions. As this made difficult the quantitative characterisation of the contribution of the two sources to atmospheric PM, a statistical method based on the treatment of data arising from high temporal resolution measurements was developed. Data were taken with a micrometeorological station based on an integrating nephelometer (Mie pDR-1200) for optical detection of PM2.5 concentration, with successive evaluation of vertical turbulent fluxes using the eddy-correlation method. Results show that the contribution from the two sources (urban emissions and industrial releases) have a very different behaviour, with the industrial contribution being present at high wind velocity with short concentration peaks (average duration 4 min) associated to strong positive and negative vertical fluxes. The estimated contribution to PM2.5 is 2.3% over long-term averages. The urban emissions are mainly present at low wind velocity, with longer concentration peaks in the morning and late evening hours, generally associated to small positive vertical fluxes. The characterisation of the contribution was performed using deposition velocity V(d) that is on average -3.5 mm s(-1) and has a diurnal pattern, with negligible values during the night and a minimum value of around -9 mm s(-1) late in the afternoon. Results show a correlation between V(d), friction velocity and wind velocity that could be the basis for a parameterisation of V(d) to be used in dispersion codes.

  10. 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).

  11. Arctic Sea Salt Aerosol from Blowing Snow and Sea Ice Surfaces - a Missing Natural Source in Winter

    NASA Astrophysics Data System (ADS)

    Frey, M. M.; Norris, S. J.; Brooks, I. M.; Nishimura, K.; Jones, A. E.

    2015-12-01

    Atmospheric particles in the polar regions consist mostly of sea salt aerosol (SSA). SSA plays an important role in regional climate change through influencing the surface energy balance either directly or indirectly via cloud formation. SSA irradiated by sunlight also releases very reactive halogen radicals, which control concentrations of ozone, a pollutant and greenhouse gas. However, models under-predict SSA concentrations in the Arctic during winter pointing to a missing source. It has been recently suggested that salty blowing snow above sea ice, which is evaporating, to be that source as it may produce more SSA than equivalent areas of open ocean. Participation in the 'Norwegian Young Sea Ice Cruise (N-ICE 2015)' on board the research vessel `Lance' allowed to test this hypothesis in the Arctic sea ice zone during winter. Measurements were carried out from the ship frozen into the pack ice North of 80º N during February to March 2015. Observations at ground level (0.1-2 m) and from the ship's crows nest (30 m) included number concentrations and size spectra of SSA (diameter range 0.3-10 μm) as well as snow particles (diameter range 50-500 μm). During and after blowing snow events significant SSA production was observed. In the aerosol and snow phase sulfate is fractionated with respect to sea water, which confirms sea ice surfaces and salty snow, and not the open ocean, to be the dominant source of airborne SSA. Aerosol shows depletion in bromide with respect to sea water, especially after sunrise, indicating photochemically driven release of bromine. We discuss the SSA source strength from blowing snow in light of environmental conditions (wind speed, atmospheric turbulence, temperature and snow salinity) and recommend improved model parameterisations to estimate regional aerosol production. N-ICE 2015 results are then compared to a similar study carried out previously in the Weddell Sea during the Antarctic winter.

  12. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 1: Fine particle composition and organic source apportionment

    SciTech Connect

    Aiken, A.C.; Wang, J.; Salcedo, D.; Cubison, M. J.; Huffman, J. A.; DeCarlo, P. F.; Ulbrich, I. M.; Docherty, K. S.; Sueper, D.; Kimmel, J. R.; Worsnop, D. R.; Trimborn, A.; Northway, M.; Stone, E. A.; Schauer, J. J.; Volkamer, R. M.; Fortner, E.; de Foy, B.; Laskin, A.; Shutthanandan, V.; Zheng, J.; Zhang, R.; Gaffney, J.; Marley, N. A.; Paredes-Miranda, G.; Arnott, W. P.; Molina, L. T.; Sosa, G.; Jimenez, J. L.

    2009-09-01

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM{sub 2.5} chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM{sub 2.5} emissions by a factor of {approx}4, and it is {approx}16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.

  13. Identification of source contributions to visibility-reducing organic aerosols in the vicinity of Grand Canyon National Park. Interim final report

    SciTech Connect

    Mazurek, M.A.; Hallock, K.A.; Leach, M.; Mason-Jones, M.; Mason-Jones, H.; Salmon, L.G.; Winner, D.A.; Cass, G.R.

    1993-06-01

    Sulfates and carbonaceous aerosols are the largest contributors to the fine particle burden in the atmosphere near Grand Canyon National Park. While the effects of sulfate particles on visibility at the Grand Canyon has been extensively studied, much less is known about the nature and origin of the carbonaceous aerosols that are present. This disparity in understanding arises from at least two causes: aerosol carbon data for the region are less plentiful and many of the sources that could contribute to that organic aerosol are both diverse and not well characterized. The objective of this present study is to examine the origin of the carbonaceous aerosol at Grand Canyon National Park during the summer season based on molecular tracer techniques applied to source and ambient samples collected specifically for this purpose.

  14. The generation of diesel exhaust particle aerosols from a bulk source in an aerodynamic size range similar to atmospheric particles

    PubMed Central

    Cooney, Daniel J; Hickey, Anthony J

    2008-01-01

    The influence of diesel exhaust particles (DEP) on the lungs and heart is currently a topic of great interest in inhalation toxicology. Epidemiological data and animal studies have implicated airborne particulate matter and DEP in increased morbidity and mortality due to a number of cardiopulmonary diseases including asthma, chronic obstructive pulmonary disorder, and lung cancer. The pathogeneses of these diseases are being studied using animal models and cell culture techniques. Real-time exposures to freshly combusted diesel fuel are complex and require significant infrastructure including engine operations, dilution air, and monitoring and control of gases. A method of generating DEP aerosols from a bulk source in an aerodynamic size range similar to atmospheric DEP would be a desirable and useful alternative. Metered dose inhaler technology was adopted to generate aerosols from suspensions of DEP in the propellant hydrofluoroalkane 134a. Inertial impaction data indicated that the particle size distributions of the generated aerosols were trimodal, with count median aerodynamic diameters less than 100 nm. Scanning electron microscopy of deposited particles showed tightly aggregated particles, as would be expected from an evaporative process. Chemical analysis indicated that there were no major changes in the mass proportion of 2 specific aromatic hydrocarbons (benzo[a]pyrene and benzo[k]fluoranthene) in the particles resulting from the aerosolization process. PMID:19337412

  15. Monitoring the environmental impact of aerosol loading and dispersion from distinct industrial sources in Cubatao, Brazil, using a scanning lidar

    NASA Astrophysics Data System (ADS)

    da Costa, Renata F.; Marques, Márcia Talita Amorim; Lopes, Daniel Silveira; Guardani, Maria Lucia Goncalves; Macedo, Fernanda d. M.; Landulfo, Eduardo; Guardani, Roberto

    2016-10-01

    This paper reports the results of campaigns carried out with a scanning lidar system in an industrial area for monitoring the spatial distribution of atmospheric aerosol. The aim of the study was to verify the possibility of applying a lidar system to identify fixed sources of aerosol emission, as well as to monitor the dispersion of the emitted plume, and the ability of the system to evaluate pertinent properties of the suspended particles, such as particle number concentration and representative particle size. The data collection was carried out with a scanning backscatter lidar system in the biaxial mode with a three-wavelength light source, based on a commercial Nd:YAG laser, operating at 355 nm, 532 nm, and 1064 nm. The campaigns were carried out in an industrial site close to the city of Cubatao, Brazil, 23° 53' S and 46° 25' W, one of the largest industrial sites of the Country, comprising a steel plant, two fertilizer complexes, a cement plant and a petrochemical complex. Backscattered light intensity plots were made from the primary data collected via 360-degree scans at 15 degree elevation. The collected data correspond to distances ranging from 200 m to 1500 m from the measurement location. The results indicate that the technique can provide valuable information on the spatial and temporal distribution of aerosol concentration in the area, which therefore can represent a valuable tool in source apportionment and to validate plume dispersion models.

  16. Long range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the Western Mediterranean basin

    NASA Astrophysics Data System (ADS)

    Ancellet, G.; Pelon, J.; Totems, J.; Chazette, P.; Bazureau, A.; Sicard, M.; Di Iorio, T.; Dulac, F.; Mallet, M.

    2015-11-01

    Long range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground based and airborne lidar measurements were deployed in the Western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Menorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agree very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from Western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the Westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (I) pure BB layer, (II) weakly dusty BB, (III) significant mixture of BB and dust transported from the trade wind region (IV) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS AOD horizontal distribution during this episode over the Western Mediterranean sea shows that the Canadian fires contribution were as large as the direct northward dust outflow from Sahara.

  17. Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies

    NASA Astrophysics Data System (ADS)

    Murphy, B. N.; Donahue, N. M.; Fountoukis, C.; Dall'Osto, M.; O'Dowd, C.; Kiendler-Scharr, A.; Pandis, S. N.

    2012-04-01

    Multigenerational oxidation chemistry of atmospheric organic compounds and its effects on aerosol loadings and chemical composition is investigated by implementing the Two-Dimensional Volatility Basis Set (2-D-VBS) in a Lagrangian host chemical transport model. Three model formulations were chosen to explore the complex interactions between functionalization and fragmentation processes during gas-phase oxidation of organic compounds by the hydroxyl radical. The base case model employs a conservative transformation by assuming a reduction of one order of magnitude in effective saturation concentration and an increase of oxygen content by one or two oxygen atoms per oxidation generation. A second scheme simulates functionalization in more detail using group contribution theory to estimate the effects of oxygen addition to the carbon backbone on the compound volatility. Finally, a fragmentation scheme is added to the detailed functionalization scheme to create a functionalization-fragmentation parameterization. Two condensed-phase chemistry pathways are also implemented as additional sensitivity tests to simulate (1) heterogeneous oxidation via OH uptake to the particle-phase and (2) aqueous-phase chemistry of glyoxal and methylglyoxal. The model is applied to summer and winter periods at three sites where observations of organic aerosol (OA) mass and O:C were obtained during the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaigns. The base case model reproduces observed mass concentrations and O:C well, with fractional errors (FE) lower than 55% and 25%, respectively. The detailed functionalization scheme tends to overpredict OA concentrations, especially in the summertime, and also underpredicts O:C by approximately a factor of 2. The detailed functionalization model with fragmentation agrees well with the observations for OA concentration, but still underpredicts O:C. Both heterogeneous oxidation and aqueous

  18. Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies

    NASA Astrophysics Data System (ADS)

    Murphy, B. N.; Donahue, N. M.; Fountoukis, C.; Dall'Osto, M.; O'Dowd, C.; Kiendler-Scharr, A.; Pandis, S. N.

    2012-11-01

    Multigenerational oxidation chemistry of atmospheric organic compounds and its effects on aerosol loadings and chemical composition is investigated by implementing the Two-Dimensional Volatility Basis Set (2-D-VBS) in a Lagrangian host chemical transport model. Three model formulations were chosen to explore the complex interactions between functionalization and fragmentation processes during gas-phase oxidation of organic compounds by the hydroxyl radical. The base case model employs a conservative transformation by assuming a reduction of one order of magnitude in effective saturation concentration and an increase of oxygen content by one or two oxygen atoms per oxidation generation. A second scheme simulates functionalization in more detail using group contribution theory to estimate the effects of oxygen addition to the carbon backbone on the compound volatility. Finally, a fragmentation scheme is added to the detailed functionalization scheme to create a functionalization-fragmentation parameterization. Two condensed-phase chemistry pathways are also implemented as additional sensitivity tests to simulate (1) heterogeneous oxidation via OH uptake to the particle-phase and (2) aqueous-phase chemistry of glyoxal and methylglyoxal. The model is applied to summer and winter periods at three sites where observations of organic aerosol (OA) mass and O:C were obtained during the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaigns. The base case model reproduces observed mass concentrations and O:C well, with fractional errors (FE) lower than 55% and 25%, respectively. The detailed functionalization scheme tends to overpredict OA concentrations, especially in the summertime, and also underpredicts O:C by approximately a factor of 2. The detailed functionalization model with fragmentation agrees well with the observations for OA concentration, but still underpredicts O:C. Both heterogeneous oxidation and aqueous

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

    PubMed Central

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

    2016-01-01

    The chemical content of water-soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for periods when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5 % of particle mass for particles with δp > 0.96 μm and 10 % of particle mass for particles with δp < 0.96 μm. Non-exchangeable aliphatic (H–C), unsaturated aliphatic (H–C–C=), oxygenated saturated aliphatic (H–C–O), acetalic (O–CH–O) and aromatic (Ar–H) protons were determined by proton nuclear magnetic resonance (1H-NMR). The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m−3 for particles with 1.5 < δp < 3.0 μm to 73.9 ± 12.3 nmol m−3 for particles with δp < 0.49 μm. The molar H/C ratios varied from 0.48 ± 0.05 to 0.92 ± 0.09, which were comparable to those observed for combustion-related organic aerosol. The R–H was the most abundant group, representing about 45 % of measured total non-exchangeable organic hydrogen concentrations, followed by H–C–O (27 %) and H–C–C= (26 %). Levoglucosan, amines, ammonium and methanesulfonate were identified in NMR fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of 1H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosols and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from −26.81 ± 0.18 ‰ for the smallest particles to

  20. Real-Time Observations of Secondary Aerosol Formation and Aging from Different Emission Sources and Environments

    NASA Astrophysics Data System (ADS)

    Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Rappenglueck, B.; Bon, D.; Graus, M.; Warneke, C.; Gilman, J.; Kuster, W.; De Gouw, J. A.; Jimenez, J. L.

    2013-12-01

    To investigate atmospheric processing of direct urban and wildfire emissions, we deployed a photochemical flow reactor (Potential Aerosol Mass, PAM) with submicron aerosol size and chemical composition measurements during FLAME-3, a biomass-burning study at USDA Fire Sciences Laboratory in Missoula, MT, and CalNex, a field study investigating the nexus of air quality and climate change at a receptor site in the LA-Basin at Pasadena, CA. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent aging of ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min in both field studies. Results show the value of this approach as a tool for in-situ evaluation of changes in OA concentration and composition due to photochemical processing. In FLAME-3, the average OA enhancement factor was 1.42 × 0.36 of the initial POA. Reactive VOCs, such as toluene, monoterpenes, and acetaldehyde, decreased with increased OHexp; however, formic acid, acetone, and some unidentified OVOCs increased after significant exposure. Net SOA formation in the photochemical reactor increased with OHexp, typically peaking around 3 days of equivalent atmospheric photochemical age (OHexp ~3.9e11 molecules cm-3 s), then leveling off at higher exposures. Unlike other studies, no decrease in OA is observed at high exposure, likely due to lower max OHexp in this study due to very high OH reactivity. The amount of additional OA mass added from aging is positively correlated with initial POA concentration, but not with the total VOC concentration or the concentration of known SOA precursors. The mass of SOA formed often exceeded the mass of the known VOC precursors, indicating the likely importance of primary semivolatile/intermediate volatility species, and possibly of unidentified VOCs as SOA precursors in biomass burning smoke. Results from CalNex show enhancement of OA and inorganic aerosol from gas-phase precursors

  1. Aerosol characteristics and sources for the Amazon basin during the wet season

    SciTech Connect

    Artaxo, P. ); Maenhaut, W. ); Storms, H.; Van Grieken, R. )

    1990-09-20

    Fine (< 2.0 {mu}m) and coarse (2.0 - 15 {mu}m) aerosol fractions were collected using stacked filter units, at three sites under the forest canopy and at three levels of a tower inside the jungle. Particle-induced x-ray emission (PIXE) was used to measure concentrations Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, Zr, and Pb. Morphological and trace element measurements of individual particles were carried out by automated electron probe x-ray microanalysis. Gravimetric analysis was performed to obtain the fine and coarse aerosol mass concentration. The concentrations of soil dust related elements (Al, Si, Ti, Fe, Mn) were 5 times larger in the wet season compared to the 1985 ABLE 2A dry season experiment. Biogenic aerosol related elements in the fine fraction showed lower concentrations in the wet season. Fine aerosol mass concentration averaged only 2.1 {plus minus} 0.7 {mu}g m{sup {minus}3}, while the average coarse mass concentration was 6.1 {plus minus} 1.8 {mu}g m{sup {minus}3}. Sulfur concentrations averaged 76 {plus minus} 14 ng m{sup {minus}3} in the fine fraction and 37 {plus minus} 9 ng m{sup {minus}3} in the coarse fraction. Only two factors explained about 90% of the data variability for the fine and coarse aerosol fractions. These were soil dust (represented mainly by Al, Si, Ti, Mn, and Fe) and biogenic aerosol (represented by K, P, Cl, S, Zn, and the aerosol mass concentration). Biogenic particles account for 55-95% of the airborne concentrations and consisted of leaf fragments, pollen grains, fungi, algae, and other types of particles. It is possible that biogenic particles can play an important role in the global aerosol budget and in the global biogeochemical cycles of various elements.

  2. Use of Probability Distribution Functions for Discriminating Between Cloud and Aerosol in Lidar Backscatter Data

    NASA Technical Reports Server (NTRS)

    Liu, Zhaoyan; Vaughan, Mark A.; Winker, Davd M.; Hostetler, Chris A.; Poole, Lamont R.; Hlavka, Dennis; Hart, William; McGill, Mathew

    2004-01-01

    In this paper we describe the algorithm hat will be used during the upcoming Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) mission for discriminating between clouds and aerosols detected in two wavelength backscatter lidar profiles. We first analyze single-test and multiple-test classification approaches based on one-dimensional and multiple-dimensional probability density functions (PDFs) in the context of a two-class feature identification scheme. From these studies we derive an operational algorithm based on a set of 3-dimensional probability distribution functions characteristic of clouds and aerosols. A dataset acquired by the Cloud Physics Lidar (CPL) is used to test the algorithm. Comparisons are conducted between the CALIPSO algorithm results and the CPL data product. The results obtained show generally good agreement between the two methods. However, of a total of 228,264 layers analyzed, approximately 5.7% are classified as different types by the CALIPSO and CPL algorithm. This disparity is shown to be due largely to the misclassification of clouds as aerosols by the CPL algorithm. The use of 3-dimensional PDFs in the CALIPSO algorithm is found to significantly reduce this type of error. Dust presents a special case. Because the intrinsic scattering properties of dust layers can be very similar to those of clouds, additional algorithm testing was performed using an optically dense layer of Saharan dust measured during the Lidar In-space Technology Experiment (LITE). In general, the method is shown to distinguish reliably between dust layers and clouds. The relatively few erroneous classifications occurred most often in the LITE data, in those regions of the Saharan dust layer where the optical thickness was the highest.

  3. Attribution of Particulate Sulfur in the Grand Canyon to Specific Point Sources Using Tracer-Aerosol Gradient Interpretive Technique (TAGIT).

    PubMed

    Kuhns, Hampden; Green, Mark; Pitchford, Marc; Vasconcelos, Luis; White, Warren; Mirabella, Vince

    1999-08-01

    Since aerosol particulate sulfur is generally a secondary airborne pollutant, most source attribution techniques require many assumptions about the transport and chemistry of sulfur dioxide (SO2) emissions. Uncertainties in our understanding of these processes impair our ability to generate reliable attribution information that is necessary for designing cost-effective pollution control policies. A new attribution technique using artificial tracer is presented in hopes of reducing the uncertainty of secondary aerosol source attribution. The Tracer-Aerosol Gradient Interpretive Technique (TAGIT) uses tracer data from a monitoring network to distinguish sites impacted by a source tagged with tracer from nonimpacted sites. Sites determined not to be influenced by the plume are considered to represent background particulate sulfur concentrations. The particulate sulfur attributable to the source at sites within the plume is calculated as the difference between observed and background particulate sulfur. TAGIT is applied to measurements made in the vicinity of the east and west ends of the Grand Canyon in order to attribute particulate sulfur to the sources within the Eastern Colorado River Valley (ECRV) and the Mohave Power Project (MPP), respectively. TAGIT results indicate that during the winter intensive field sampling experiment (January 15-February 13, 1992), an average of 59 + 12% of the particulate sulfur at Marble Canyon, AZ, was attributable to ECRV sources. Similarly, during the summer field sampling experiment (July 13-August 30, 1992), MPP is estimated to have contributed an average of 7 + 3% of the particulate sulfur at Meadview, AZ. Uncertainties associated with the assumptions of TAGIT are discussed and quantified. The attribution results suggest that SO2-to-sulfate conversion rates are highly variable from day to day in this region.

  4. Marine aerosol source regions to Prince of Wales Icefield, Ellesmere Island, and influence from the tropical Pacific, 1979-2001

    NASA Astrophysics Data System (ADS)

    Criscitiello, Alison S.; Marshall, Shawn J.; Evans, Matthew J.; Kinnard, Christophe; Norman, Ann-Lise; Sharp, Martin J.

    2016-08-01

    Using a coastal ice core collected from Prince of Wales (POW) Icefield on Ellesmere Island, we investigate source regions of sea ice-modulated chemical species (methanesulfonic acid (MSA) and chloride (Cl-)) to POW Icefield and the influence of large-scale atmospheric variability on the transport of these marine aerosols (1979-2001). Our key findings are (1) MSA in the POW Icefield core is derived primarily from productivity in the sea ice zone of Baffin Bay and the Labrador Sea, with influence from waters within the North Water (NOW) polynya, (2) sea ice formation processes within the NOW polynya may be a significant source of sea-salt aerosols to the POW core site, in addition to offshore open water source regions primarily in Hudson Bay, and (3) the tropical Pacific influences the source and transport of marine aerosols to POW Icefield through its remote control on regional winds and sea ice variability. Regression analyses during times of MSA deposition reveal sea level pressure (SLP) anomalies favorable for opening of the NOW polynya and subsequent oceanic dimethyl sulfide production. Regression analyses during times of Cl- deposition reveal SLP anomalies that indicate a broader oceanic region of sea-salt sources to the core site. These results are supported by Scanning Multichannel Microwave Radiometer- and Special Sensor Microwave/Imager-based sea ice reconstructions and air mass transport density analyses and suggest that the marine biogenic record may capture local polynya variability, while sea-salt transport to the site from larger offshore source regions in Baffin Bay is likely. Regression analyses show a link to tropical dynamics via an atmospheric Rossby wave.

  5. Physical properties, chemical composition, sources, spatial distribution and sinks of indoor aerosol particles in a university lecture hall

    NASA Astrophysics Data System (ADS)

    Salma, I.; Dosztály, K.; Borsós, T.; Söveges, B.; Weidinger, T.; Kristóf, G.; Péter, N.; Kertész, Zs.

    2013-01-01

    PM10 mass, particle number (N) and CO2 concentrations, particle number size distributions and meteorological parameters were determined with high time resolution, and daily aerosol samples were collected in the PM10-2.0 and PM2.0 size fractions for chemical analysis in the middle of a university lecture hall for one week. Median concentrations for the PM10 mass and N of 15.3 μg m-3 and 3.7 × 103 cm-3, respectively were derived. The data are substantially smaller than the related outdoor levels or typical values for residences. There were considerable concentration differences for workdays, weekends and various lectures. Main sources of PM10 mass include the usage of chalk sticks for writing, wiping the blackboard, ordinary movements and actions of students and cleaning. High PM10 mass concentration levels up to 100 μg m-3 were realised for short time intervals after wiping the blackboard. The mass concentrations decreased rapidly after the emission source ceased to be active. Two classes of coarse particles were identified. General indoor dust particles exhibited a residence time of approximately 35 min, while the residence time for the chalk dust particles was approximately 20 min as lower estimates. Emission source rate for wiping the blackboard was estimated to be between 8 and 14 mg min-1. This represents a substantial emission rate but the source is active only up to 1 min. Suspension of the chalk (made mainly of gypsum) dust particles was confirmed by enrichment of Ca and S in the hall with respect to ambient urban aerosol. Contribution of ambient aerosol via the heating, ventilation and air conditioning (HVAC) facility was considerable for time intervals when the indoor sources of PM10 mass were not intensive. The HVAC facility introduces, however, the major amount of aerosol particles from the outdoors as far as their number concentration is regarded. Mean contribution of ultrafine particles to the total particle number was (69 ± 7)%, which is smaller

  6. Aerosol particles collected on aircraft flights over the northwestern Pacific region during the ACE-Asia campaign: Composition and major sources of the organic compounds

    NASA Astrophysics Data System (ADS)

    Simoneit, Bernd R. T.; Kobayashi, Minoru; Mochida, Michihiro; Kawamura, Kimitaka; Huebert, Barry J.

    2004-10-01

    Atmospheric particulate matter, collected over the polluted east Asia/Pacific region in spring 2001 during research flights with the National Center for Atmospheric Research (NCAR) C-130 aircraft, was analyzed for different types of organic compounds using capillary gas chromatography-mass spectrometry. More than 70 organic species were detected in the aerosols and grouped into different compound classes on the basis of functional groups, including n-alkanes, polycyclic aromatic hydrocarbons, fatty acids, dehydroabietic acid, alkanols, water-soluble sugars (including glucose, sucrose, mycose, and levoglucosan), monocarboxylic and dicarboxylic acids, urea, and phthalates. Interestingly, the water-soluble compounds (72-133 ng m-3) were found to account for 16-50% (average 34%) of the total identified compound mass (TCM). Organic compounds were further categorized into several groups to suggest their sources. Fossil fuel combustion was recognized as the most significant source for the TCM (contributing 33-80% of TCM, average 50%), followed by soil resuspension (5-25%, average 19%) and secondary oxidation products (4-15%, average 9%). In contrast, the contribution of natural sources such as terrestrial plant wax and marine lipids (fatty acids and alkanols) was relatively small (3.4% and 9.4% on average, respectively). Biomass burning was suggested to contribute only a minor portion to the TCM of the Asian aerosols during the spring season (1.4% on average based on levoglucosan). However, levoglucosan may have been hydrolyzed and/or oxidized in part during long-range transport, and therefore this value represents a lower limit. The organic compound compositions of these samples are very different from those reported for aerosol particles of the Atlantic Ocean and from the earlier data for the mid-Pacific in terms of the abundant presence of water-soluble compounds consisting of saccharides, anhydrosaccharides, and the secondary dicarboxylic acids. This study

  7. Aerosol species concentrations and source apportionment of ammonia at Rocky Mountain National Park.

    PubMed

    Malm, William C; Schichtel, Bret A; Barna, Michael G; Gebhart, Kristi A; Rodriguez, Marco A; Collett, Jeffrey L; Carrico, Christian M; Benedict, Katherine B; Prenni, Anthony J; Kreidenweis, Sonia M

    2013-11-01

    Changes in ecosystem function at Rocky Mountain National Park (RMNP) are occurring because of emissions of nitrogen and sulfate species along the Front Range of the Colorado Rocky Mountains, as well as sources farther east and west. The nitrogen compounds include both oxidized and reduced nitrogen. A year-long monitoring program of various oxidized and reduced nitrogen species was initiated to better understand their origins as well as the complex chemistry occurring during transport from source to receptor. Specifically the goals of the study were to characterize the atmospheric concentrations of nitrogen species in gaseous, particulate, and aqueous phases (precipitation and clouds) along the east and west sides of the Continental Divide; identify the relative contributions to atmospheric nitrogen species in RMNP from within and outside of the state of Colorado; identify the relative contributions to atmospheric nitrogen species in RMNP from emission sources along the Colorado Front Range versus other areas within Colorado; and identify the relative contributions to atmospheric nitrogen species from mobile sources, agricultural activities, and large and small point sources within the state of Colorado. Measured ammonia concentrations are combined with modeled releases of conservative tracers from ammonia source regions around the United States to apportion ammonia to its respective sources, using receptor modeling tools.

  8. Characterization and sources assignation of PM2.5 organic aerosol in a rural area of Spain

    NASA Astrophysics Data System (ADS)

    Pindado, Oscar; Pérez, Rosa M. a.; García, Susana; Sánchez, Miguel; Galán, Pilar; Fernández, Marta

    The results from a year-long study of the organic composition of PM2.5 aerosol collected in a rural area influenced by a highway of Spain are reported. The lack of prior information related to the organic composition of PM2.5 aerosol in Spain, concretely in rural areas, led definition of the goals of this study. As a result, this work has been able to characterize the main organic components of atmospheric aerosols, including several compounds of SOA, and has conducted a multivariate analysis in order to assign sources of particulate matter. A total of 89 samples were taken between April 2004 and April 2005 using a high-volume sampler. Features and abundance of n-alkanes, polycyclic aromatic hydrocarbons (PAHs), alcohols and acids were separately determined using gas chromatography/mass spectrometry and high performance liquid chromatography analysis. The Σ n-alkane and ΣPAHs ranged from 3 to 81 ng m -3 and 0.1 to 6 ng m -3 respectively, with higher concentrations during colder months. Ambient concentrations of Σalcohols and Σacids ranged from 21 to 184 ng m -3 and 39 to 733 ng m -3, respectively. Also, several components of secondary organic aerosol have been quantified, confirming the biogenic contribution to ambient aerosol. In addition, factor analysis was used to reveal origin of organic compounds associated to particulate matter. Eight factors were extracted accounting more than 83% of the variability in the original data. These factors were assigned to a typical high pollution episode by anthropogenic particles, crustal material, plant waxes, fossil fuel combustion, temperature, microbiological emissions, SOA and dispersion of pollutants by wind action. Finally, a cluster analysis was used to compare the organic composition between the four seasons.

  9. Sources, Sinks, and Transatlantic Transport of North African Dust Aerosol: A Multimodel Analysis and Comparison With Remote Sensing Data

    NASA Technical Reports Server (NTRS)

    Kim, Dongchul; Chin, Mian; Yu, Hongbin; Diehl, Thomas; Tan, Qian; Kahn, Ralph A.; Tsigaridis, Kostas; Bauer, Susanne E.; Takemura, Toshihiko; Pozzoli, Luca; Bellouin, Nicolas; Schulz, Michael; Peyridieu, Sophie; Chedin, Alain; Koffi, Brigitte

    2014-01-01

    This study evaluates model-simulated dust aerosols over North Africa and the North Atlantic from five global models that participated in the Aerosol Comparison between Observations and Models phase II model experiments. The model results are compared with satellite aerosol optical depth (AOD) data from Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), and Sea-viewing Wide Field-of-view Sensor, dust optical depth (DOD) derived from MODIS and MISR, AOD and coarse-mode AOD (as a proxy of DOD) from ground-based Aerosol Robotic Network Sun photometer measurements, and dust vertical distributions/centroid height from Cloud Aerosol Lidar with Orthogonal Polarization and Atmospheric Infrared Sounder satellite AOD retrievals. We examine the following quantities of AOD and DOD: (1) the magnitudes over land and over ocean in our study domain, (2) the longitudinal gradient from the dust source region over North Africa to the western North Atlantic, (3) seasonal variations at different locations, and (4) the dust vertical profile shape and the AOD centroid height (altitude above or below which half of the AOD is located). The different satellite data show consistent features in most of these aspects; however, the models display large diversity in all of them, with significant differences among the models and between models and observations. By examining dust emission, removal, and mass extinction efficiency in the five models, we also find remarkable differences among the models that all contribute to the discrepancies of model-simulated dust amount and distribution. This study highlights the challenges in simulating the dust physical and optical processes, even in the best known dust environment, and stresses the need for observable quantities to constrain the model processes.

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

    NASA Astrophysics Data System (ADS)

    Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

    2015-12-01

    The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. Aerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 μg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi

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

    DOE PAGES

    Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; ...

    2016-05-02

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

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

    NASA Astrophysics Data System (ADS)

    Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

    2016-05-01

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

  13. Long-term dust aerosol production from natural sources in Iceland.

    PubMed

    Dagsson-Waldhauserova, Pavla; Arnalds, Olafur; Olafsson, Haraldur

    2017-02-01

    Iceland is a volcanic island in the North Atlantic Ocean with maritime climate. In spite of moist climate, large areas are with limited vegetation cover where >40% of Iceland is classified with considerable to very severe erosion and 21% of Iceland is volcanic sandy deserts. Not only do natural emissions from these sources influenced by strong winds affect regional air quality in Iceland ("Reykjavik haze"), but dust particles are transported over the Atlantic ocean and Arctic Ocean >1000 km at times. The aim of this paper is to place Icelandic dust production area into international perspective, present long-term frequency of dust storm events in northeast Iceland, and estimate dust aerosol concentrations during reported dust events. Meteorological observations with dust presence codes and related visibility were used to identify the frequency and the long-term changes in dust production in northeast Iceland. There were annually 16.4 days on average with reported dust observations on weather stations within the northeastern erosion area, indicating extreme dust plume activity and erosion within the northeastern deserts, even though the area is covered with snow during the major part of winter. During the 2000s the highest occurrence of dust events in six decades was reported. We have measured saltation and Aeolian transport during dust/volcanic ash storms in Iceland, which give some of the most intense wind erosion events ever measured. Icelandic dust affects the ecosystems over much of Iceland and causes regional haze. It is likely to affect the ecosystems of the oceans around Iceland, and it brings dust that lowers the albedo of the Icelandic glaciers, increasing melt-off due to global warming. The study indicates that Icelandic dust may contribute to the Arctic air pollution.

  14. Daily measurement of organic compounds in ambient particulate matter in Augsburg, Germany: new aspects on aerosol sources and aerosol related health effects.

    PubMed

    Schnelle-Kreis, Jürgen; Küpper, Ute; Sklorz, Martin; Cyrys, Josef; Briedé, Jacob Jan; Peters, Annette; Zimmermann, Ralf

    2009-07-01

    Several epidemiological studies have shown that in the human population ambient particulate matter (PM) is associated with adverse health effects. Little is known, however, about the relative effects of aerosol constituents. Since 2002, diurnal samples of ambient PM2.5 were analysed by automated methods for the quantification of particle-associated organic compounds (POC). Data on chemical composition have been investigated in epidemiological and biological effect studies. As a result of these studies, the associations found between PAH concentration and symptoms of myocardial infarction survivors suggest a major influence of combustion sources on cardiovascular health effects. The correlations found between formation of reactive oxygen species and the presence of specific organic compounds suggests an important influence of biomass combustion particles in PM2.5-associated oxidative stress.

  15. On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol - Part 1: Source fluxes

    NASA Astrophysics Data System (ADS)

    Fuentes, E.; Coe, H.; Green, D.; de Leeuw, G.; McFiggans, G.

    2010-06-01

    MBLe cruise, which revealed a higher production of particles with Dp0<100 nm at regions with high biological activity. A novel sub-micrometric size-resolved source flux function, explicitly defined as a function of the diatomaceous exudate concentration, was derived from the size distribution measurements and the estimation of the fractional whitecap coverage. According to the defined parameterisation, a 300 μM OC<0.2μm concentration of diatomaceous exudate in seawater produces an overall increment in the total source particle flux of ~20% with respect to the organics-free seawater case. The effect increases with decreasing particle size for Dp0<100 nm, resulting in multiplicative factors between 1.02-2 with respect to the particle flux generated from seawater devoid of marine organics. The total source flux derived from the presented parameterisation was compared to recent definitions of sea-spray source fluxes based on laboratory and field observations in the literature.

  16. Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

    SciTech Connect

    Kumar, R.; Barth, M. C.; Nair, V. S.; Pfister, G. G.; Babu, S. Suresh; Satheesh, S. K.; Moorthy, K. Krishna; Carmichael, G. R.; Lu, Z.; Streets, D. G.

    2015-01-01

    This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March-May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model-observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average +/- standard deviation (representing spatial and temporal variability) BC mass concentration (1341 +/- 2353 ng m(-3)) in South Asia. BC emissions from residential (61 %) and industrial (23 %) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.

  17. Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

    SciTech Connect

    Kumar, R.; Barth, M. C.; Nair, V. S.; Pfister, G. G.; Suresh Babu, S.; Satheesh, S. K.; Moorthy, K. Krishna; Carmichael, G. R.; Lu, Z.; Streets, D. G.

    2015-05-19

    This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March–May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model–observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m-3) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.

  18. Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

    DOE PAGES

    Kumar, R.; Barth, M. C.; Nair, V. S.; ...

    2015-05-19

    This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March–May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inlandmore » sites. In general, the model underestimates the observed BC mass concentrations. However, the model–observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m-3) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.« less

  19. Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

    NASA Astrophysics Data System (ADS)

    Kumar, R.; Barth, M. C.; Nair, V. S.; Pfister, G. G.; Babu, S. Suresh; Satheesh, S. K.; Krishna Moorthy, K.; Carmichael, G. R.; Lu, Z.; Streets, D. G.

    2015-05-01

    This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March-May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model-observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m-3) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.

  20. Evaluation of New and Proposed Organic Aerosol Sources and Mechanisms using the Aerosol Modeling Testbed. MILAGRO, CARES, CalNex, BEACHON, and GVAX

    SciTech Connect

    Hodzic, Alma; Jimenez, Jose L.

    2015-04-09

    This work investigated the formation and evolution of organic aerosols (OA) arising from anthropogenic and biogenic sources in a framework that combined state-of-the-science process and regional modeling, and their evaluation against advanced and emerging field measurements. Although OA are the dominant constituents of submicron particles, our understanding of their atmospheric lifecycle is limited, and current models fail to describe the observed amounts and properties of chemically formed secondary organic aerosols (SOA), leaving large uncertainties on the effects of SOA on climate. Our work has provided novel modeling constraints on sources, formation, aging and removal of SOA by investigating in particular (i) the contribution of trash burning emissions to OA levels in a megacity, (ii) the contribution of glyoxal to SOA formation in aqueous particles in California during CARES/CalNex and over the continental U.S., (iii) SOA formation and regional growth over a pine forest in Colorado and its sensitivity to anthropogenic NOx levels during BEACHON, and the sensitivity of SOA to (iv) the sunlight exposure during its atmospheric lifetime, and to (v) changes in solubility and removal of organic vapors in the urban plume (MILAGRO, Mexico City), and over the continental U.S.. We have also developed a parameterization of water solubility for condensable organic gases produced from major anthropogenic and biogenic precursors based on explicit chemical modeling, and made it available to the wider community. This work used for the first time constraints from the explicit model GECKO-A to improve SOA representation in 3D regional models such as WRF-Chem.

  1. Sources and light absorption of water-soluble brown carbon aerosols in the outflow from northern China

    NASA Astrophysics Data System (ADS)

    Kirillova, E. N.; Andersson, A.; Han, J.; Lee, M.; Gustafsson, Ö.

    2013-07-01

    High loadings of anthropogenic carbonaceous aerosols in Chinese air influence the air quality for over 1 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 (WS-BrC) and its relation to sources is poorly understood. Here, we combine source estimates constrained by dual-carbon-isotope with light absorption measurements of WS-BrC for a March 2011 campaign at the Korea Climate Observatory at Gosan (KCOG), a receptor station in SE Yellow Sea for the outflow from N. China. The mass absorption cross-section (MAC) of WS-BrC 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). We estimate that this effect corresponds to 13-49% of the radiative forcing caused by light absorption by black carbon. Radiocarbon constraints show that the WS-BrC in Chinese outflow had significantly higher amounts of fossil sources (30-50%) compared to previous findings in S. Asia, N. America and Europe. Stable carbon (δ13C) measurements indicated influence of aging during air mass transport. These results indicate the importance of incorporating WS-BrC in climate models and the need to constrain climate effects by emission source sector.

  2. Functional Group Composition of Semivolatile Compounds Present in Submicron Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Ruggeri, G.; Modini, R. L.; Iannarelli, R.; Rossi, M. J.; Takahama, S.

    2014-12-01

    Semivolatile organic compounds can partition between gas and particle phase in atmospheric conditions and can be volatilized and lost when the aerosol sampling is performed onto PTFE filters (Eatough et al., 1993). In this work, semivolatile compounds are collected onto carbon impregnated glass fiber-cellulose filters placed in series after an activated carbon denuder and PTFE filter which collects submicron aerosol particles of low volatility (Subramanian et al., 2004). The semivolatile compounds accumulated on the cellulose-glass fiber filters are desorbed by vacuum and injected into a stainless steel chamber that enables cold-trapping. The vapors in this chamber are condensed onto a low-temperature silicon window, and the composition of deposited vapors are analysed by transmission-mode Fourier Transform Infrared (FTIR) spectroscopy (Delval and Rossi, 2004). Functional group composition of semivolatile compounds that can be desorbed from the aerosol phase and its relationship with the apparent low-volatile fraction composition will be presented. Eatough, D.J., Wadsworth, A., Eatough, D.A., Crawford, J.W., Hansen, L.D., Lewis, E.A., 1993. A multiple-system, multi-channel diffusion denuder sampler for the determination of fine-particulate organic material in the atmosphere. Atmospheric Environment. Part A. General Topics 27, 1213-1219. Subramanian, R., Khlystov, A.Y., Cabada, J.C., Robinson, A.L., 2004. Positive and negative artifacts in particulate organic carbon measurements with denuded and undenuded sampler configurations. Aerosol Science and Technology 38, 27-48. Delval, C., Rossi, M.J., 2004. The kinetics of condensation and evaporation of H2O from pure ice in the range 173-223 K: a quartz crystal microbalance study. Physical Chemistry Chemical Physics 6, 4665-4676.

  3. Aerosol Deposition of Molybdenum: A Control on Nitrogen-Fixation and Tropical Forest Function

    NASA Astrophysics Data System (ADS)

    Wong, M.; Howarth, R. W.; Marino, R. M.; Mahowald, N. M.; Williams, E. R.

    2015-12-01

    Nitrogen fixation, the primary source of new nitrogen (N) to tropical forests, is exclusively catalyzed by the nitrogenase enzyme, which almost always requires molybdenum (Mo). Increasing evidence in recent years suggests that Mo availability may be low in highly weathered soils and can constrain N-fixation rates. Mo is generally either present in a highly soluble form (MoO42-) that is susceptible to leaching or tightly bound in minerals unavailable for biological uptake. To address how Mo is retained in highly weathered tropical systems to support N-fixation, atmospheric transport through dust and sea-salt aerosol spray were examined. Using a global atmospheric transport model computed from modeled meteorological fields, extrapolated dust and sea-salt aerosol Mo sources were used to calculate global distribution of Mo deposition. Dust deposition occurs across the entirety of some tropical forests, particularly the world's largest tropical forest in the Amazon Basin. The model indicates that the Amazon Basin receives substantial inputs of dust, especially the entire northern Amazon Basin, while the southern half receives less. Most of the dust reaching the Amazon originates from the Sahara Desert, and about half of this dust originates from one part of the Sahara, the Bodélé Depression. Mo in dust from the Bodélé Depression was measured with an average concentration of 1.14 ± 0.05 μg/g, similar to the crustal abundance. The model predicts Mo inputs from sea-salt aerosols in coastal regions up to 0.002 mg m-2yr-1. Significant sea-salt deposition occurs up to 300 km inland. Mo from fossil fuel combustion and biomass burning were also evaluated to determine the potential influence of anthropogenic emissions on releasing Mo into the environment.

  4. Airflow dynamics of human jets: sneezing and breathing - potential sources of infectious aerosols.

    PubMed

    Tang, Julian W; Nicolle, Andre D; Klettner, Christian A; Pantelic, Jovan; Wang, Liangde; Suhaimi, Amin Bin; Tan, Ashlynn Y L; Ong, Garrett W X; Su, Ruikun; Sekhar, Chandra; Cheong, David D W; Tham, Kwok Wai

    2013-01-01

    Natural human exhalation flows such as coughing, sneezing and breathing can be considered as 'jet-like' airflows in the sense that they are produced from a single source in a single exhalation effort, with a relatively symmetrical, conical geometry. Although coughing and sneezing have garnered much attention as potential, explosive sources of infectious aerosols, these are relatively rare events during daily life, whereas breathing is necessary for life and is performed continuously. Real-time shadowgraph imaging was used to visualise and capture high-speed images of healthy volunteers sneezing and breathing (through the nose - nasally, and through the mouth - orally). Six volunteers, who were able to respond to the pepper sneeze stimulus, were recruited for the sneezing experiments (2 women: 27.5±6.36 years; 4 men: 29.25±10.53 years). The maximum visible distance over which the sneeze plumes (or puffs) travelled was 0.6 m, the maximum sneeze velocity derived from these measured distances was 4.5 m/s. The maximum 2-dimensional (2-D) area of dissemination of these sneezes was 0.2 m(2). The corresponding derived parameter, the maximum 2-D area expansion rate of these sneezes was 2 m(2)/s. For nasal breathing, the maximum propagation distance and derived velocity were 0.6 m and 1.4 m/s, respectively. The maximum 2-D area of dissemination and derived expansion rate were 0.11 m(2) and 0.16 m(2)/s, respectively. Similarly, for mouth breathing, the maximum propagation distance and derived velocity were 0.8 m and 1.3 m/s, respectively. The maximum 2-D area of dissemination and derived expansion rate were 0.18 m(2) and 0.17 m(2)/s, respectively. Surprisingly, a comparison of the maximum exit velocities of sneezing reported here with those obtained from coughing (published previously) demonstrated that they are relatively similar, and not extremely high. This is in contrast with some earlier estimates of sneeze velocities, and some reasons for this difference are discussed.

  5. Airflow Dynamics of Human Jets: Sneezing and Breathing - Potential Sources of Infectious Aerosols

    PubMed Central

    Tang, Julian W.; Nicolle, Andre D.; Klettner, Christian A.; Pantelic, Jovan; Wang, Liangde; Suhaimi, Amin Bin; Tan, Ashlynn Y. L.; Ong, Garrett W. X.; Su, Ruikun; Sekhar, Chandra; Cheong, David D. W.; Tham, Kwok Wai

    2013-01-01

    Natural human exhalation flows such as coughing, sneezing and breathing can be considered as ‘jet-like’ airflows in the sense that they are produced from a single source in a single exhalation effort, with a relatively symmetrical, conical geometry. Although coughing and sneezing have garnered much attention as potential, explosive sources of infectious aerosols, these are relatively rare events during daily life, whereas breathing is necessary for life and is performed continuously. Real-time shadowgraph imaging was used to visualise and capture high-speed images of healthy volunteers sneezing and breathing (through the nose – nasally, and through the mouth - orally). Six volunteers, who were able to respond to the pepper sneeze stimulus, were recruited for the sneezing experiments (2 women: 27.5±6.36 years; 4 men: 29.25±10.53 years). The maximum visible distance over which the sneeze plumes (or puffs) travelled was 0.6 m, the maximum sneeze velocity derived from these measured distances was 4.5 m/s. The maximum 2-dimensional (2-D) area of dissemination of these sneezes was 0.2 m2. The corresponding derived parameter, the maximum 2-D area expansion rate of these sneezes was 2 m2/s. For nasal breathing, the maximum propagation distance and derived velocity were 0.6 m and 1.4 m/s, respectively. The maximum 2-D area of dissemination and derived expansion rate were 0.11 m2 and 0.16 m2/s, respectively. Similarly, for mouth breathing, the maximum propagation distance and derived velocity were 0.8 m and 1.3 m/s, respectively. The maximum 2-D area of dissemination and derived expansion rate were 0.18 m2 and 0.17 m2/s, respectively. Surprisingly, a comparison of the maximum exit velocities of sneezing reported here with those obtained from coughing (published previously) demonstrated that they are relatively similar, and not extremely high. This is in contrast with some earlier estimates of sneeze velocities, and some reasons for this difference are discussed. PMID

  6. 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

  7. Submicron aerosol analysis and organic source apportionment in an urban atmosphere in Pearl River Delta of China using high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    He, Ling-Yan; Huang, Xiao-Feng; Xue, Lian; Hu, Min; Lin, Yun; Zheng, Jun; Zhang, Renyi; Zhang, Yuan-Hang

    2011-06-01

    The Pearl River Delta (PRD) region in South China is one of the most economically developed regions in China while also noted for its severe air pollution, especially in the urban environments. In order to understand in depth the aerosol chemistry and the emission sources in PRD, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site in the Hong Kong-Shenzhen metropolitan area between 25 October and 2 December 2009. Ten minute-resolved measurement data were analyzed, and an average mass concentration of 44.5 ± 34.0 μg m-3 was calculated for the entire campaign. On average, organic matter was the most abundant PM1 component accounting for 39.7% of the total mass, followed by sulfate (24.5%), black carbon (measured by aethalometer, 14.0%), ammonium (10.2%), nitrate (10.0%), and chloride (1.6%). Moreover, organic matter comprised an increasing fraction of the PM1 loading as the PM1 loading increased, denoting its key role in particulate pollution in this region. Calculations of organic elemental composition based on the high-resolution organic mass spectra obtained indicated that C, H, O, and N on average contributed 33.8%, 55.1%, 10.2%, and 0.9%, respectively, to the total atomic numbers of organic aerosol (OA), which corresponded to an OM/OC ratio (the ratio of organic matter mass/organic carbon mass) of 1.57 ± 0.08. Positive matrix factorization analysis was then conducted on the high-resolution organic mass spectral data set. Four OA components were identified, including a hydrocarbon-like (HOA), a biomass burning (BBOA), and two oxygenated (LV-OOA and SV-OOA) components, which on average accounted for 29.5%, 24.1%, 18.8%, and 27.6%, respectively, of the total organic mass. The HOA was found to have contributions from both fossil fuel combustion and cooking emissions, while the BBOA was well correlated with acetonitrile, a known biomass burning marker. The LV-OOA and SV-OOA corresponded to more aged and

  8. Retrieval of the columnar aerosol phase function and single-scattering albedo from sky radiance over the ocean - Simulations

    NASA Technical Reports Server (NTRS)

    Wang, Menghua; Gordon, Howard R.

    1993-01-01

    Based on the fact that the part of downward radiance that depends on the optical properties of the aerosol in the atmosphere can be extracted from the measured sky radiance, a new scheme for retrieval of the aerosol phase function and the single-scattering albedo over the ocean is developed. This retrieval algorithm is tested with simulations for several cases. It is found that the retrieved aerosol phase function and the single-scattering albedo are virtually error-free if the vertical structure of the atmosphere is known and if the sky radiance and the aerosol optical thickness can be measured accurately. The robustness of the algorithm in realistic situations, in which the measurements are contaminated by calibration errors or noise, is examined. It is found that the retrieved value of omega(0) is usually in error by less than about 10 percent, and the phase function is accurately retrieved for theta less than about 90 deg. However, as the aerosol optical thickness becomes small, e.g., less than about 0.1, errors in the sky radiance measurement can lead to serious problems with the retrieval algorithm, especially in the blue. The use of the retrieval scheme should be limited to the red and near IR when the aerosol optical thickness is small.

  9. Insights into the molecular level composition, sources, and formation mechanisms of dissolved organic matter in aerosols and precipitation

    NASA Astrophysics Data System (ADS)

    Altieri, Katye Elisabeth

    Atmospheric aerosols scatter and absorb light influencing the global radiation budget and climate, and are associated with adverse effects on human health. Precipitation is an important removal mechanism for atmospheric dissolved organic matter (DOM), and a potentially important input for receiving ecosystems. However, the sources, formation, and composition of atmospheric DOM in aerosols and precipitation are not well understood. This dissertation investigates the composition and formation mechanisms of secondary organic aerosol (SOA) formed through cloud processing reactions, elucidates the composition and sources of DOM in rainwater, and provides links connecting the two. Photochemical batch aqueous-phase reactions of organics with both biogenic and anthropogenic sources (i.e., methylglyoxal, pyruvic acid) and OH radical were performed to simulate cloud processing. The composition of products formed through cloud processing experiments and rainwater collected in New Jersey, USA was investigated using a combination of electrospray ionization mass spectrometry techniques, including ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry. This dissertation has resulted in the first evidence that oligomers form through cloud processing reactions, the first detailed chemical mechanism of aqueous phase oligomerization, the first identification of oligomers, organosulfates, and nitrooxy organosulfates in precipitation, and the first molecular level chemical characterization of organic nitrogen in precipitation. The formation of oligomers in SOA helps to explain the presence of large multifunctional compounds and humic like substances (HULIS) that dominate particulate organic mass. Oligomers have low vapor pressures and remain in the particle phase after cloud evaporation, enhancing SOA. The chemical properties of the oligomers suggest that they are less hygroscopic than the monomeric reaction products (i.e., organic acids). Their elemental

  10. European isotopic signatures for lead in atmospheric aerosols: a source apportionment based upon 206Pb/207Pb ratios.

    PubMed

    Flament, Pascal; Bertho, Marie-Laure; Deboudt, Karine; Véron, Alain; Puskaric, Emile

    2002-09-16

    To investigate the capability of the lead isotope signature technique to support a source apportionment study at a Continental scale, atmospheric particulate matter was collected at Cap Gris-Nez (Eastern Channel, northern France), over one year (1995-1996). Four days retrospective trajectories of air masses were available during each sampling experiment. Twenty-eight samples, for which the origin of aerosols was unambiguously determined, were selected for isotopic measurements. Considering the Enrichment Factors, EF(Crust) of lead and its size distribution, we show that lead is mostly from anthropogenic origin and mainly associated with [0.4 < diameter < 0.9 microm] particles. The extent to which various Continental sources influence the lead abundance in aerosols is exhibited by considering both the lead concentration and the origin of air masses. Lead concentration is higher by a factor of approximately seven, when air masses are derived from Continental Europe, by comparison with marine air masses. Taking into account these concentrations and the vertical movements of air masses, we compare the different isotopic compositions using a statistical non-parametric test (Kolmogorov-Smirnov). We produce evidence that, for most of the cases, air masses originating from Continental Europe exhibit a more radiogenic composition (1.134 < 206Pb/207Pb < 1.172) than air masses coming from the United Kingdom (1.106 < 206Pb/207Pb < 1.124). Generally, lead isotopic compositions in aerosols are clearly distinct from the gasoline signatures in European countries, strongly suggesting that automotive lead is no longer the major component of this metal in the air. Gasoline and industrial isotopic signatures could explain the origin of lead in our aerosol samples. A source apportionment based upon 206Pb/207Pb ratios, suggests that the difference between British (206Pb/207Pb = 1.122 +/- 0.038) and Continental (206Pb/207Pb = 1.155 +/- 0.022) signatures may be largely explained by

  11. Possible indicators of long-range transport for aerosol emitted from various source regions in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Park, S.; Kim, C.

    2013-12-01

    Air pollutant is affected by both long-range transboundary processes and local air pollution emission. Therefore it is important to identify the origin of air pollutant, for example, by classifying air pollutants into long-range transport (LRT) dominant process and local emission dominant (LED) cases. This study proposed several chemical and physical indicators of LRT process of aerosol concentrations observed at Korean peninsula. In order to identify the source regions and to estimate the contributions of both LRT and LED, we performed Lagrangian particle dispersion model(FLEXPART) and selected high pollution days over the three source regions in China inland and one Korea peninsula defined in this study; LRT-I to III and LED case. Next, we investigated the chemical and physical characteristics of LRT process of aerosol, and contrasted to those in the LED case over the Northeast Asia. We examined the difference of both modeled features simulated by CMAQ and as well measured aerosol optical properties of satellite-based sensor MODIS and AERONET data. Modeling study showed that the most effective indicator is the sulfur conversion ratios such as SO42-/(SO2+ SO42-) and SO42-/ SO2 for high sulfate condition. The ratio of N-containing species such as NOx (or NOy) to CO were the next best alternative indicators. In the meteorological fields, the results showed that pressure pattern and streamline flow are similar on a case by case basis. For observational physical features, we obtained the spatial distributions of the mean AOD, fine mode fraction (FMF), angstrom exponent (AE) by taking the average of MODIS aerosol products for the each analysis period. The highest AOD was found over the industrialized coastal region regardless of cases. AERONET data showed that aerosol size distribution showed significantly higher concentration of fine-mode particle in LED cases in comparison with that of LRT groups, suggesting that the amplitude fine modes of LRT relative to LED could

  12. Sources and elemental composition of summer aerosols in the Larsemann Hills (Antarctica).

    PubMed

    Budhavant, Krishnakant; Safai, P D; Rao, P S P

    2015-02-01

    Atmospheric aerosols play a major role in the global climate change. A better physical characterization of the chemical composition of atmospheric aerosols, especially in remote atmosphere, is an important step to reduce the current uncertainty in their effect on the radiative forcing of the climate. In the present work, surface aerosols have been studied over the Southern Ocean and over Bharati, Indian Research Station at Larsemann Hills at the Antarctic coast during the summer season of 2009-2010. Aerosol samples were collected using optical particle counter (OPC) and high-volume air sampler. PM10 and PM2.5 aerosol samples were analyzed for various water-soluble and acid-soluble ionic constituents. The Hysplit model was used to compute the history of the air masses for their possible origin. Supplementary measurements of meteorological parameters were also used. The average mass concentration for PM10 over the Southern Ocean was found to be 13.4 μg m(3). Over coastal Antarctica, the mass of PM10 was 5.13 μg m(-3), whereas that of PM2.5 was 4.3 μg m(-3). Contribution of marine components, i.e., Na, Cl and Mg was dominant over the Southern Ocean (79 %) than over the coastal Antarctica where they were dominant in coarse mode (67 %) than in fine mode (53 %) aerosols. The NH4/nss-SO4 ratio of 1.12 in PM2.5 indicates that the NH4 and SO4 ions were in the form of NH4HSO4. Computation of enrichment factors indicate that elements of anthropogenic origin, e.g., Zn, Cu, Pb, etc., were highly enriched with respect to crustal composition.

  13. Emission sources and atmospheric processing of carbonaceous aerosols in India and China: Insights from dual carbon isotope techniques

    NASA Astrophysics Data System (ADS)

    Andersson, A.; Kirillova, E. N.; Bosch, C.; Suresh, T.; Lee, M.; Du, K.; Sheesley, R. J.; Budhavant, K.; Gustafsson, O. M.

    2013-12-01

    The large emissions of carbonaceous aerosols, e.g., black carbon (BC), in India and China have detrimental effects on both human health and the regional climate. However, mitigation efforts as well as accurate modeling of these effects are currently hampered by large uncertainties regarding the contributions from different emission sources, including both primary and secondary processes. Here, we present dual carbon isotope constraints on emissions sources and atmospheric processing from multiple sites capturing the outflow from India and China. Radiocarbon (14C) studies of elemental carbon (EC) - a tracer for BC - show larger relative fossil contributions than expected from bottom-up emission inventories, for both India (49+-5) and China (80 +-6%). Similarly to EC, radiocarbon constraints of water soluble organic carbon (WSOC) shows substantially larger relative fossil contributions in Chinese outflow (30-50%) as compared with India, but also compared to Europe and USA (10-20%). In contrast to the radiocarbon data, stable carbon (d13C) analysis of WSOC shows substantial variability for different sites capturing the Indian outflow. Strong enrichment of heavy isotopes in WSOC is coupled to expected transport time from sources, indicating the influence of photochemical aging during transport. Such trends in the d13C signature are not observed for the EC fraction. Taken together this work show that carbon isotope techniques provide firm constraints on emission sources of different fractions of carbonaceous aerosols, and may also offer insights into atmospheric processing of these constituents during air mass transport.

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

    PubMed

    Jathar, Shantanu H; Gordon, Timothy D; Hennigan, Christopher J; Pye, Havala O T; Pouliot, George; Adams, Peter J; Donahue, Neil M; Robinson, Allen L

    2014-07-22

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10-20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y(-1) of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations.

  15. Toward correlating functional MRI and EEG sources

    NASA Astrophysics Data System (ADS)

    Singh, Manbir; Khosla, Deepak

    1996-04-01

    Though excellent spatial resolution (on the order of 1 mm) is obtainable in functional MRI (fMRI), its temporal resolution is limited to about 1 second by hemodynamics. On the other hand, magnetoencephalography (MEG) and electroencephalography (EEG) provide millisecond temporal resolution but a relatively crude (on the order of 1 cm) spatial resolution to localized sources. Thus, techniques that could combine the high temporal resolution of MEG or EEG with the high spatial resolution of fMRI would be of great significance in imaging the spatiotemporal distribution of neuronal activation. With the ultimate objective of combining fMRI and EEG activation studies, we have conducted experiments to determine how pixels activated in fMRI correlate with underlying EEG sources in a given subject during visual stimulation. Results of a three-subject study suggest good correlation between the center-of-gravity of activated pixels seen in fMRI and the center-of-gravity of regions localized through EEG measurements.

  16. Smoke aerosol properties and ageing effects for Northern temperate and boreal regions derived from AERONET source and age attribution

    NASA Astrophysics Data System (ADS)

    Nikonovas, T.; North, P. R. J.; Doerr, S. H.

    2015-03-01

    Particulate emissions from wildfires impact human health and have a large but uncertain effect on climate. Modelling schemes depend on information about emission factors, emitted particle microphysical and optical properties and ageing effects, while satellite retrieval algorithms make use of characteristic aerosol models to improve retrieval. Ground based remote sensing provides detailed aerosol characterisation, but does not contain information on source. Here, a method is presented to estimate plume origin land cover type and age for AERONET aerosol observations, employing trajectory modelling using the HYSPLIT model, and satellite active fire and aerosol optical thickness (AOT) observations from MODIS and AATSR. It is applied to AERONET stations located in or near Northern temperate and boreal forests, for the period 2002-2013. The results from 629 fire attributions indicate significant differences in size distributions and particle optical properties between different land cover types. Smallest fine mode median radius are attributed to plumes from cropland - natural vegetation mosaic (0.143 μm) and grasslands (0.147 μm) fires. Evergreen needleleaf forest emissions show a significantly smaller fine mode median radius (0.164 μm) than plumes from woody savannas (0.184 μm) and mixed forest (0.193 μm) fires. Smoke plumes are predominantly scattering for all of the classes with median single scattering albedo at 440 nm (SSA(440)) values close to 0.95 except the cropland emissions which have a SSA(440) value of 0.9. Overall fine mode volume median radius increase rate is 0.0095 μm per day for the first 4 days of ageing and 0.0084 μm per day for seven days of ageing. Changes in size were consistent with a decrease in Angstrom Exponent and increase in Asymmetry parameter. No significant changes in SSA(λ) with ageing were found. These estimates have implications for

  17. Smoke aerosol properties and ageing effects for Northern temperate and boreal regions derived from AERONET source and age attribution

    NASA Astrophysics Data System (ADS)

    Nikonovas, Tadas; North, Peter; Doerr, Stefan H.

    2015-04-01

    Particulate emissions from wildfires impact human health and have a large but uncertain effect on climate. Modelling schemes depend on information about emission factors, emitted particle microphysical and optical properties and ageing effects, while satellite retrieval algorithms make use of characteristic aerosol models to improve retrieval. Ground based remote sensing provides detailed aerosol characterisation, but does not contain information on source. A new method is presented to estimate plume origin land cover type and age for AERONET aerosol observations, employing trajectory modelling using the HYSPLIT model, and satellite active fire and aerosol optical thickness (AOT) observations from MODIS and AATSR. It is applied to AERONET stations located in or near Northern temperate and boreal forests, for the period 2002-2013. The results from 629 fire attributions indicate significant differences insize distributions and particle optical properties between different land cover types. Smallest fine mode median radius are attributed to plumes from cropland/natural vegetation mosaic (0.143 μm) and grasslands (0.147 μm) fires. Evergreen needleleaf forest emissions show a significantly smaller fine mode median radius (0.164 μm) than plumes from woody savannas (0.184 μm) and mixed forest (0.193 μm) fires. Smoke plumes are predominantly scattering for all of the classes with median single scattering albedo at 440 nm (SSA(440)) values close to 0.95 except the cropland emissions which have SSA(440) value of 0.9. Overall fine mode volume median radius increase rate is 0.0095μm per day for the first 4 days of ageing and 0.0084 μm per day for seven days of ageing. Changes in size were consistent with a decrease in Angstrom Exponent and increase in Asymmetry parameter. No significant changes in SSA(λ) with ageing were found. The implications of this work for improved modeling of aerosol radiative effects, which are relevant to both climate modelling and satellite

  18. Using FLEXPART-WRF to Identify Source Regions Influencing Arctic Trace Gases and Aerosols During the Summer 2014 NETCARE Campaign

    NASA Astrophysics Data System (ADS)

    Thomas, J. L.

    2015-12-01

    In July and August 2014 the Canadian Network on Aerosols and Climate: Addressing Key Uncertainties in Remote Canadian Regions (NETCARE) project conducted aircraft and ship based campaigns with the goal of identifying both emissions and atmospheric processes influencing Arctic trace gas and aerosol concentrations. The aircraft campaign was conducted using the Alfred Wegener Institute's POLAR 6 aircraft (based in Resolute Bay, Canada) and the ship based campaign was conducted onboard the CCGS Amundsen (icebreaker and Arctic Ocean research vessel). Here, we use the Weather Research and Forecasting Model (WRF) to study meteorology and transport patterns that influence airmasses sampled during the aircraft campaign (5-21 July 2012) and research Legs 1a and 1b for Amundsen (1a: 8 - 24 July Quebec City to Resolute and 24 July - 14 August Resolute to Kugluktuk). The FLEXible PARTicle dispersion model driven by WRF meteorology (FLEXPART-WRF) run in backwards mode is used to study source regions that influenced enhanced concentrations in trace gases including DMS and NH3 as well as aerosols. Links between biomass burning in Northern Canada and measurements during the campaign are discussed. Finally FLEXPART-WRF run in forward mode is used to study links between shipping emissions from the Amundsen and enhanced pollution sampled by the POLAR 6 aircraft when both were operating in the same region of Lancaster Sound during the campaigns.

  19. Probing the impact of different aerosol sources on cloud microphysics and precipitation through in-situ measurements of chemical mixing state

    NASA Astrophysics Data System (ADS)

    Prather, K. A.; Suski, K.; Cazorla, A.; Cahill, J. F.; Creamean, J.; Collins, D. B.; Heymsfield, A.; Roberts, G. C.; DeMott, P. J.; Sullivan, R. C.; Rosenfeld, D.; Comstock, J. M.; Tomlinson, J. M.

    2011-12-01

    Aerosol particles play a crucial role in affecting cloud processes by serving as cloud nuclei. However, our understanding of which particles actually form cloud and ice nuclei limits our ability to treat aerosols properly in climate models. In recent years, it has become possible to measure the chemical composition of individual cloud nuclei within the clouds using on-line mass spectrometry. In-situ high time resolution chemistry can now be compared with cloud physics measurements to directly probe the impact of aerosol chemistry on cloud microphysics. This presentation will describe results from two recent field campaigns, CalWater in northern California and ICE-T in the western Caribbean region. Ground-based and aircraft measurements will be presented of aerosol mixing state, cloud microphysics, and meteorology. Results from single particle mass spectrometry will show the sources of the cloud seeds, including dust, biomass burning, sea spray, and biological particles. Details will be provided on how we are now able to probe the sources and cycling of atmospheric aerosols by measuring individual aerosols, cloud nuclei, and precipitation chemistry. The important role of dust, both Asian and African, and bioparticles in forming ice nuclei will be discussed. Finally, a summary will be provided discussing how these new in-situ measurements are being used to advance our understanding of complex atmospheric processes, and improve our understanding of aerosol impacts on climate.

  20. Aerosol Health Impact Source Attribution Studies with the CMAQ Adjoint Air Quality Model

    NASA Astrophysics Data System (ADS)

    Turner, M. D.

    , reductions in emissions from large industrial combustion sources that are not classified as EGUs (i.e., non-EGU) are estimated to have up to triple the benefits per unit emission of reductions to onroad diesel sectors, and provide similar benefits per unit of reduced emission to that of onroad gasoline emissions in the region. While a majority of vehicle emission controls that regulate PM focus on diesel emissions, our analysis shows the most efficient target for stricter controls is actually onroad gasoline emissions. From an analysis of the health impacts of BC emissions on specific demographic populations, we find that emissions in the southern half of the US tend to disproportionally affect persons with a below high school education and persons below 50% of the poverty level. Analysis of national risk (independent of population and mortality rates) shows that the largest risks are associated with drier climates, due to the increased atmospheric lifetime resulting from less wet removal of aerosols. Lastly, analysis of the impacts of BC emissions on maximum individual risk shows that contributions to maximum individual risk are weakly to strongly correlated with emissions (R2 ranging from 0.23 in the San Joaquin Valley to 0.93 in the Dallas region). Overall, this thesis shows the value of high-resolution, adjoint-based source attribution studies for determining the locations, seasons, and sectors that have the greatest estimated impact on human health in air quality models.

  1. Organic aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis

    NASA Astrophysics Data System (ADS)

    Reyes-Villegas, Ernesto; Green, David C.; Priestman, Max; Canonaco, Francesco; Coe, Hugh; Prévôt, André S. H.; Allan, James D.

    2016-12-01

    The multilinear engine (ME-2) factorization tool is being widely used following the recent development of the Source Finder (SoFi) interface at the Paul Scherrer Institute. However, the success of this tool, when using the a value approach, largely depends on the inputs (i.e. target profiles) applied as well as the experience of the user. A strategy to explore the solution space is proposed, in which the solution that best describes the organic aerosol (OA) sources is determined according to the systematic application of predefined statistical tests. This includes trilinear regression, which proves to be a useful tool for comparing different ME-2 solutions. Aerosol Chemical Speciation Monitor (ACSM) measurements were carried out at the urban background site of North Kensington, London from March to December 2013, where for the first time the behaviour of OA sources and their possible environmental implications were studied using an ACSM. Five OA sources were identified: biomass burning OA (BBOA), hydrocarbon-like OA (HOA), cooking OA (COA), semivolatile oxygenated OA (SVOOA) and low-volatility oxygenated OA (LVOOA). ME-2 analysis of the seasonal data sets (spring, summer and autumn) showed a higher variability in the OA sources that was not detected in the combined March-December data set; this variability was explored with the triangle plots f44 : f43 f44 : f60, in which a high variation of SVOOA relative to LVOOA was observed in the f44 : f43 analysis. Hence, it was possible to conclude that, when performing source apportionment to long-term measurements, important information may be lost and this analysis should be done to short periods of time, such as seasonally. Further analysis on the atmospheric implications of these OA sources was carried out, identifying evidence of the possible contribution of heavy-duty diesel vehicles to air pollution during weekdays compared to those fuelled by petrol.

  2. Direct Radiative Effect and Heating Rate of black carbon aerosol: high time resolution measurements and source-identified forcing effects

    NASA Astrophysics Data System (ADS)

    Ferrero, Luca; Mocnik, Grisa; Cogliati, Sergio; Comi, Alberto; Degni, Francesca; Di Mauro, Biagio; Colombo, Roberto; Bolzacchini, Ezio

    2016-04-01

    Black carbon (BC) absorbs sunlight in the atmosphere heating it. However, up to now, heating rate (HR) calculations from the divergence of the net radiative flux with altitude or from the modelling activity are too sparse. This work fills the aforementioned gap presenting a new methodology based on a full set of physical equations to experimentally determine both the radiative power density absorbed into a ground-based atmospheric layer (ADRE), and the consequent HR induced by the absorptive component of aerosol. In urban context, it is essentially related to the BC. The methodology is also applicable to natural components (i.e. dust) and is obtained solving the first derivative of the main radiative transfer equations. The ADRE and the consequent HR can be determined coupling spectral aerosol absorption measurements with the spectrally resolved measurements of the direct, diffuse downward radiation and the surface reflected radiance components. Moreover, the spectral absorption of BC aerosol allows its source apportionment (traffic and biomass burning (BB)) allowing the same apportionment on HR. This work reports one year of high-time resolution measurements (5 min) of sunlight absorption and HR induced by BC aerosol over Milan. A unique sampling site was set up from March 2015 with: 1) Aethalometer (AE-31, Magee Scientific, 7-λ), 2) the Multiplexer-Radiometer-Irradiometer which detects downward and reflected radiance (350-1000 nm in 3648 spectral bands) coupled with a rotating shadow-band to measure spectrally-resolved global and diffuse radiation (thus direct), 3) a meteorological station (LSI-Lastem) equipped with 3 pyranometers (global, diffuse and refrected radiation; 300-3000 nm), a thermohygrometer, a barometer, an anemometer, 4) condensation and optical particle counters (TSI 3775 and Grimm 1.107), 5) low volume sampler (FAI Hydra dual sampler, PM2.5 and PM10) for sample collection and chemistry determination. Results concerning the radiative power

  3. Aerosolized vaccine as an unexpected source of false-positive Bordetella pertussis PCR results.

    PubMed

    Salimnia, Hossein; Lephart, Paul R; Asmar, Basim I; Prebelich, Dawn; Paulson, Erin; Fairfax, Marilynn R

    2012-02-01

    When 13 of 13 nasal wash specimens from a single pediatrician's office tested positive for low quantities of Bordetella pertussis DNA, we suspected prelaboratory contamination. Investigation revealed that Pentacel and Adacel vaccines contain high copy numbers of B. pertussis DNA, which can be aerosolized, causing false-positive B. pertussis PCR results.

  4. Sources of excess urban carbonaceous aerosol in the Pearl River delta region, China

    EPA Science Inventory

    Carbonaceous aerosol is one of the important constituents of fine particulate matter (PM2.5) 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...

  5. Organic Aerosol Composition and Sources in Pasadena, California during the 2010 CalNex Campaign

    EPA Science Inventory

    Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) ...

  6. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    EPA Science Inventory

    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 Specia...

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

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

    NASA Astrophysics Data System (ADS)

    Ulevicius, V.; Byčenkienė, S.; Bozzetti, C.; Vlachou, A.; Plauškaitė, K.; Mordas, G.; Dudoitis, V.; Abbaszade, G.; Remeikis, V.; Garbaras, A.; Masalaite, A.; Blees, J.; Fröhlich, R.; Dällenbach, K. R.; Canonaco, F.; Slowik, J. G.; Dommen, J.; Zimmermann, R.; Schnelle-Kreis, J.; Salazar, G. A.; Agrios, K.; Szidat, S.; El Haddad, I.; Prévôt, A. S. H.

    2015-09-01

    In early spring the Baltic region is frequently affected by high pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m-3 and black carbon (BC) up to 17 μg m-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26-44 % and 13-23 % to the TC, respectively. 5-8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4-13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13-24 % and 7-12 %, respectively. Isotope ratio of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

  9. Development of a Metastable Atom Bombardment (MAB) Source for Penning Ionization Time-of-flight Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Robinson, C. B.; Kimmel, J. R.; David, D.; Jayne, J. T.; Trimborn, A.; Worsnop, D. R.; Jimenez, J. L.

    2009-12-01

    The Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS) utilizes thermal vaporization followed by electron ionization (EI) to convert aerosol components to gas-phase ions. The method enables quantification of chemical classes, but the extensive fragmentation caused by EI limits the specificity of both chemical analysis and source identification by factor analysis. To better identify the molecular components of aerosols, we have constructed a metastable atom bombardment (MAB) ionization source that can be interfaced to standard ToF-AMS hardware. A beam of metastable rare gas atoms is produced by a low-voltage DC discharge and focused toward the vaporization plume, yielding Penning Ionization of the analyte molecules. By changing gases, the excited energies of the metastables can be adjusted between 20.61 eV (He) and 9.92 eV (Kr). Source parameters, including pressures, current, geometry, and materials, were optimized for He, Ar, and Kr. Instrument sensitivity and induced fragmentation was characterized for each using lab-generated oleic acid particles. The demonstrated sensitivities are 0.1% of EI (3% of the SNR of EI in the V-mode, comparable to the Q-AMS SNR), which is sufficient for ambient monitoring. A metastable flux of 2.6e14 sr-1sec-1 has been achieved. The MAB-AMS has been deployed to the FLAME-3 campaign at the USDA Fire Sciences Laboratory in Missoula, MT, and used to sample smoke from open burning of different biomass samples. Preliminary results from FLAME-3 will be presented.

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

    NASA Technical Reports Server (NTRS)

    Sittler, E. C., Jr.; Ali, A.; Cooper, J. F.; Hartle, R. E.; Johnson, R. E.; Coates, A. J.; Young, D. T.

    2009-01-01

    Discovery by Cassini's plasma instrument of heavy positive and negative ions within Titan's upper atmosphere and ionosphere has advanced our understanding of ion neutral chemistry within Titan's upper atmosphere, primarily composed of molecular nitrogen, with approx.2.5% methane. The external energy flux transforms Titan's upper atmosphere and ionosphere into a medium rich in complex hydrocarbons, nitriles and haze particles extending from the surface to 1200 km altitudes. The energy sources are solar UV, solar X-rays, Saturn's magnetospheric ions and electrons, solar wind and shocked magnetosheath ions and electrons, galactic cosmic rays (CCR) and the ablation of incident meteoritic dust from Enceladus' E-ring and interplanetary medium. Here it is proposed that the heavy atmospheric ions detected in situ by Cassini for heights >950 km, are the likely seed particles for aerosols detected by the Huygens probe for altitudes <100km. These seed particles may be in the form of polycyclic aromatic hydrocarbons (PAH) containing both carbon and hydrogen atoms CnHx. There could also be hollow shells of carbon atoms, such as C60, called fullerenes which contain no hydrogen. The fullerenes may compose a significant fraction of the seed particles with PAHs contributing the rest. As shown by Cassini, the upper atmosphere is bombarded by magnetospheric plasma composed of protons, H(2+) and water group ions. The latter provide keV oxygen, hydroxyl and water ions to Titan's upper atmosphere and can become trapped within the fullerene molecules and ions. Pickup keV N(2+), N(+) and CH(4+) can also be implanted inside of fullerenes. Attachment of oxygen ions to PAH molecules is uncertain, but following thermalization O(+) can interact with abundant CH4 contributing to the CO and CO2 observed in Titan's atmosphere. If an exogenic keV O(+) ion is implanted into the haze particles, it could become free oxygen within those aerosols that eventually fall onto Titan's surface. The process

  12. Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.: URBAN INFLUENCE ON RURAL AEROSOL

    SciTech Connect

    Zhou, Shan; Collier, Sonya; Xu, Jianzhong; Mei, Fan; Wang, Jian; Lee, Yin-Nan; Sedlacek, Arthur J.; Springston, Stephen R.; Sun, Yele; Zhang, Qi

    2016-05-19

    Continuous real-time measurements of atmospheric aerosol with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the DOE Aerosol Life Cycle Intensive Operational Period (ALC-IOP) campaign.

  13. Mechanically Ventilated Broiler Sheds: a Possible Source of Aerosolized Salmonella, Campylobacter, and Escherichia coli▿

    PubMed Central

    Chinivasagam, H. N.; Tran, T.; Maddock, L.; Gale, A.; Blackall, P. J.

    2009-01-01

    This study assessed the levels of two key pathogens, Salmonella and Campylobacter, along with the indicator organism Escherichia coli in aerosols within and outside poultry sheds. The study ranged over a 3-year period on four poultry farms and consisted of six trials across the boiler production cycle of around 55 days. Weekly testing of litter and aerosols was carried out through the cycle. A key point that emerged is that the levels of airborne bacteria are linked to the levels of these bacteria in litter. This hypothesis was demonstrated by E. coli. The typical levels of E. coli in litter were ∼108 CFU g−1 and, as a consequence, were in the range of 102 to 104 CFU m−3 in aerosols, both inside and outside the shed. The external levels were always lower than the internal levels. Salmonella was only present intermittently in litter and at lower levels (103 to 105 most probable number [MPN] g−1) and consequently present only intermittently and at low levels in air inside (range of 0.65 to 4.4 MPN m−3) and once outside (2.3 MPN m−3). The Salmonella serovars isolated in litter were generally also isolated from aerosols and dust, with the Salmonella serovars Chester and Sofia being the dominant serovars across these interfaces. Campylobacter was detected late in the production cycle, in litter at levels of around 107 MPN g−1. Campylobacter was detected only once inside the shed and then at low levels of 2.2 MPN m−3. Thus, the public health risk from these organisms in poultry environments via the aerosol pathway is minimal. PMID:19801461

  14. MBAS (Methylene Blue Active Substances) and LAS (Linear Alkylbenzene Sulphonates) in Mediterranean coastal aerosols: Sources and transport processes

    NASA Astrophysics Data System (ADS)

    Becagli, S.; Ghedini, C.; Peeters, S.; Rottiers, A.; Traversi, R.; Udisti, R.; Chiari, M.; Jalba, A.; Despiau, S.; Dayan, U.; Temara, A.

    2011-12-01

    Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) concentrations, together with organic carbon and ions were measured in atmospheric coastal aerosols in the NW Mediterranean Basin. Previous studies have suggested that the presence of surfactants in coastal aerosols may result in vegetation damage without specifically detecting or quantifying these surfactants. Coastal aerosols were collected at a remote site (Porquerolles Island-Var, France) and at a more anthropised site (San Rossore National Park-Tuscany, Italy). The chemical data were interpreted according to a comprehensive local meteorological analysis aiming to decipher the airborne source and transport processes of these classes of compounds. The LAS concentration (anthropogenic surfactants) was measured in the samples using LC-MS/MS, a specific analytical method. The values were compared with the MBAS concentration, determined by a non-specific analytical method. At Porquerolles, the MBAS concentration (103 ± 93 ng m -3) in the summer samples was significantly higher than in the winter samples. In contrast, LAS concentrations were rarely greater than in the blank filters. At San Rossore, the mean annual MBAS concentration (887 ± 473 ng m -3 in PM10) contributed about 10% to the total atmospheric particulate organic matter. LAS mean concentration in these same aerosol samples was 11.5 ± 10.5 ng m -3. A similar MBAS (529 ± 454 ng m -3) - LAS (7.1 ± 4.1 ng m -3 LAS) ratio of ˜75 was measured in the fine (PM2.5) aerosol fraction. No linear correlation was found between MBAS and LAS concentrations. At San Rossore site the variation of LAS concentrations was studied on a daily basis over a year. The LAS concentrations in the coarse fraction (PM10-2.5) were higher during strong sea storm conditions, characterized by strong air flow coming from the sea sector. These events, occurring with more intensity in winter, promoted the formation of primary marine aerosols containing LAS

  15. Basic biogenic aerosol precursors: Agricultural source attribution of volatile amines revised

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Sintermann, J.; Spirig, C.; Jocher, M.; Ammann, C.; Neftel, A.

    2011-08-01

    Despite recent evidence on an important role of volatile amines in the nucleation of particulate matter, very scarce information is available on their atmospheric abundance and source distribution. Previous measurements in animal housings had identified livestock husbandry as the main amine source, with trimethylamine (TMA) being the key component. This has led to the assumption that the agricultural sources for amines are similar as for ammonia, emitted throughout the cascade of animal excretion, storage and application in the field. In this study, we present the first micrometeorological flux measurements as well as dynamic enclosure experiments showing that the amine source strength from stored slurry is negligible, implying significant consequences for the global amine emission inventory. In the case of cattle, amine production is attributed to the animal's rumination activity and exhalation is suggested to be an important emission pathway, similar to the greenhouse gas methane. Fodder like hay and silage also emits volatile amines, potentially assigning these alkaloid compounds a key function in enhancing particle formation in remote areas.

  16. Aerosol Composition and Source Apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and Multivariate Analysis

    SciTech Connect

    Johnson, Kirsten S.; de Foy, B.; Zuberi, Bilal M.; Molina, Luisa; Molina, Mario J.; Xie, YuLong; Laskin, Alexander; Shutthanandan, V.

    2006-10-12

    Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA). The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish ef- 5 fective pollution control standards. For these reasons, samples of particulate matter _2.5 µm (PM2.5) were collected during the MCMA-2003 Field Campaign for elemental and multivariate analyses. Proton-Induced X-ray Emission (PIXE), Proton-Elastic Scattering Analysis (PESA) and Scanning Transmission Ion Microscopy (STIM) techniques were done to determine concentrations of 19 elements from Na to Pb, hydrogen, and 10 total mass, respectively. The most abundant elements from PIXE analysis were S, Si, K, Fe, Ca, and Al, while the major emissions sources associated with these elements were industry, wind-blown soil, and biomass burning. Wind trajectories suggest that metals associated with industrial emissions came from northern areas of the city whereas soil aerosols came from the southwest and increased in concentration during 15 dry conditions. Elemental markers for fuel oil combustion V and Ni correlated with a large SO2 plume to suggest an anthropogenic, rather than volcanic, emissions source. By subtracting major components of soil and sulfates determined by PIXE analysis from STIM total mass measurements, we estimate that approximately 50% of PM2.5 consisted of carbonaceous material.

  17. Review of heterogeneous photochemical reactions of NOy on aerosol - A possible daytime source of nitrous acid (HONO) in the atmosphere.

    PubMed

    Ma, Jinzhu; Liu, Yongchun; Han, Chong; Ma, Qingxin; Liu, Chang; He, Hong

    2013-02-01

    As an important precursor of hydroxyl radical, nitrous acid (HONO) plays a key role in the chemistry of the lower atmosphere. Recent atmospheric measurements and model calculations show strong enhancement for HONO formation during daytime, while they are inconsistent with the known sources in the atmosphere, suggesting that current models are lacking important sources for HONO. In this article, heterogeneous photochemical reactions of nitric acid/nitrate anion and nitrogen oxide on various aerosols were reviewed and their potential contribution to HONO formation was also discussed. It is demonstrated that HONO can be formed by photochemical reaction on surfaces with deposited HNO3, by photocatalytic reaction of NO2 on TiO2 or TiO2-containing materials, and by photochemical reaction of NO2 on soot, humic acids or other photosensitized organic surfaces. Although significant uncertainties still exist in the exact mechanisms and the yield of HONO, these additional sources might explain daytime observations in the atmosphere.

  18. Changes in concentration, composition and source contribution of atmospheric organic aerosols by shifting coal to natural gas in Urumqi

    NASA Astrophysics Data System (ADS)

    Ren, Yanqin; Wang, Gehui; Wu, Can; Wang, Jiayuan; Li, Jianjun; Zhang, Lu; Han, Yanni; Liu, Lang; Cao, Cong; Cao, Junji; He, Qing; Liu, Xinchun

    2017-01-01

    Size-segregated aerosols were collected in Urumqi, a megacity in northwest China, during two heating seasons, i.e., before (heating season І: January-March 2012) and after (heating season II: January-March 2014) the project "shifting coal to natural gas", and determined for n-alkanes, PAHs and oxygenated PAHs to investigate the impact of replacement of coal by natural gas on organic aerosols in the urban atmosphere. Our results showed that compared to those in heating season I concentrations of n-alkanes, PAHs and OPAHs decreased by 74%, 74% and 82% in heating season II, respectively. Source apportionment analysis suggested that coal combustion, traffic emission and biomass burning are the major sources of the determined organics during the heating seasons in Urumqi. Traffic emission is the main source for n-alkanes in the city. Coal combustion is the dominant source of PAHs and OPAHs in heating season І, but traffic emission becomes their major source in heating season ІI. Relative contributions of coal combustion to n-alkanes, PAHs and OPAHs in Urumqi decreased from 21 to 75% in heating season I to 4.0-21% in heating season II due to the replacement of coal with natural gas for house heating. Health risk assessment further indicated that compared with that in heating season I the number of lung cancer related to PAHs exposure in Urumqi decreased by 73% during heating season II due to the project implementation. Our results suggest that replacing coal by clean energy sources for house heating will significantly mitigate air pollution and improve human health in China.

  19. Assessing the impact of atmospheric stability on locally and remotely sourced aerosols at Richmond, Australia, using Radon-222

    NASA Astrophysics Data System (ADS)

    Crawford, Jagoda; Chambers, Scott; Cohen, David; Williams, Alastair; Griffiths, Alan; Stelcer, Eduard

    2016-02-01

    A flexible radon-based scheme for the classification of nocturnal stability regimes was used for the interpretation of daily-integrated PM2.5 aerosol observations collected at Richmond, Australia, between 2007 and 2011. Source fingerprint concentrations for the dominant locally and remotely sourced aerosols were analysed by nocturnal radon stability category to characterise the influences of day-to-day changes in daily integrated atmospheric mixing. The fingerprints analysed included: smoke, vehicle exhaust, secondary sulfate and aged industrial sulfur. The largest and most consistent stability influences were observed on the locally sourced pollutants. Based on a 5-year composite, daily integrated concentrations of smoke were almost a factor of 7 higher when nocturnal conditions were classed as "stable" than when they were "near neutral". For vehicle emissions a factor of 4 was seen. However, when the winter months were considered in isolation, it was found that these factors increased to 11.5 (smoke) and 5.5 (vehicle emissions) for daily average concentrations. The changes in concentration of the remotely sourced pollutants with atmospheric stability were comparatively small and less consistent, probably as a result of the nocturnal inversion frequently isolating near-surface observations from non-local sources at night. A similar classification was performed using the commonly-adopted Pasquill-Gifford (PG) stability typing technique based on meteorological parameters. While concentrations of fingerprints associated with locally-sourced pollutants were also shown to be positively correlated with atmospheric stability using the PG classification, this technique was found to underestimate peak pollutant concentrations under stable atmospheric conditions by almost a factor of 2.

  20. 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