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

    PubMed Central

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

    2011-01-01

    Measurements of submicron particles by Fourier transform infrared spectroscopy in 14 campaigns in North America, Asia, South America, and Europe were used to identify characteristic organic functional group compositions of fuel combustion, terrestrial vegetation, and ocean bubble bursting sources, each of which often accounts for more than a third of organic mass (OM), and some of which is secondary organic aerosol (SOA) from gas-phase precursors. The majority of the OM consists of alkane, carboxylic acid, hydroxyl, and carbonyl groups. The organic functional groups formed from combustion and vegetation emissions are similar to the secondary products identified in chamber studies. The near absence of carbonyl groups in the observed SOA associated with combustion is consistent with alkane rather than aromatic precursors, and the absence of organonitrate groups can be explained by their hydrolysis in humid ambient conditions. The remote forest observations have ratios of carboxylic acid, organic hydroxyl, and nonacid carbonyl groups similar to those observed for isoprene and monoterpene chamber studies, but in biogenic aerosols transported downwind of urban areas the formation of esters replaces the acid and hydroxyl groups and leaves only nonacid carbonyl groups. The carbonyl groups in SOA associated with vegetation emissions provides striking evidence for the mechanism of esterification as the pathway for possible oligomerization reactions in the atmosphere. Forest fires include biogenic emissions that produce SOA with organic components similar to isoprene and monoterpene chamber studies, also resulting in nonacid carbonyl groups in SOA. PMID:21317360

  5. 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.

  6. 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.

  7. AERONET - Aerosol Climatology From Megalopolis Aerosol Source Regions

    NASA Astrophysics Data System (ADS)

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

    2002-05-01

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

  8. 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

  9. 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

  10. 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.

    2014-02-01

    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 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

  11. 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

  12. 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.

  13. 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.

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

    PubMed

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

    2014-02-15

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

  15. Sources and transformations of atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Cross, Eben Spencer

    transported towards Europe. In this study, particles were highly processed prior to sampling, with residence times of a few days in the atmosphere. The MILAGRO campaign focused on the evolution of the Mexico City plume as it was transported north. During this study, regional and locally emitted particles were measured with residence times varying from minutes to days in the atmosphere. In both studies, the light scattering - AMS system provided detailed information about the density and composition of single particles, leading to important insights into how atmospheric processing transforms the particle properties. In Mexico City, the light scattering-AMS system was used for the first time as a true single particle mass spectrometer and revealed specific details about the atmospheric processing of primary particles from combustion sources. To quantify the radiative effects of the particles on climate, the processing and ultimate fate of primary emissions (often containing black carbon or soot) must be understood. To provide a solid basis for the interpretation of the data obtained during the field studies, experiments were conducted with a well characterized soot generation-sampling system developed by the Boston College research group. The laboratory soot source was combined with the light scattering - AMS system and a Cloud Condensation Nuclei Counter (CCNC) to measure the change in cloud-forming activity of soot particles as they are processed in the atmosphere. Because of the importance of black carbon in the atmosphere, several instruments have been developed to measure black carbon. In July of 2008, an intercomparison study of 18 instruments was conducted in the Boston College laboratory, with soot particles produced and processed to mimic a wide range of atmospherically-relevant conditions. Transformations in the physical, chemical, and optical properties of soot particles were monitored with the combined suite of aerosol instrumentation. Results from the

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

    NASA Astrophysics Data System (ADS)

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

    2015-11-01

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

  17. 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.

  18. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-02-01

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

  20. 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.

  1. Sources and components of organic aerosols in Central Europe

    NASA Astrophysics Data System (ADS)

    Lanz, V. A.; Prévôt, A. S. H.; Alfarra, M. R.; Hüglin, C.; Mohr, C.; Weimer, S.; Baltensperger, U.

    2009-04-01

    The quadrupole version of the Aerodyne Aerosol Mass Spectrometer (q-AMS) was deployed at several places in Switzerland, Austria, and Liechtenstein. The q-AMS provides real-time information on mass concentration and composition of the non-refractory species in particulate matter smaller than 1 µm (NR-PM1) with high time- and size-resolution at unit mass resolution. The combination of factor analysis and ambient AMS data represents a relatively new approach to identify organic aerosol (OA) sources/components (Zhang et al., 2005). In this study, such an approach (PMF - positive matrix factorization; Lanz et al., 2007, 2008) was applied to various OA data sets covering a wide range of pollution levels (mobile measurements on motorways, urban, rural, and even a high-alpine location) as well as all seasons of the year. Dominating aerosol components were representing oxygenated and secondary organic aerosol (OOA-I and OOA-II), primary particles from wood burning (P-BBOA; especially in residential areas in wintertime with abundances of ~50% OA and more) and primary traffic-related aerosols (usually ~10% of OA, but up to 60% on motorways). Close to sources, charbroiling and potentially food cooking aerosols could be distinguished as well. The OOAs' time series were compared to measurements of AMS inorganics (sulphate, nitrate, and ammonium) in order to facilitate their interpretation as secondary OA (SOA). Diurnal cycles of the estimated source strengths, ancillary gas-phase and meteorological data, estimated emission ratios etc. were also used to validate the interpretations of the factor analytical results. Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C., and Prévôt, A. S. H.: Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra, Atmos. Chem. Phys., 7, 1503-1522, 2007, http://www.atmos-chem-phys.net/7/1503/2007/. Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B

  2. 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.

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

    PubMed

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

    2014-08-19

    Atmospheric selenium (Se) in aerosols was investigated using X-ray absorption near-edge structure (XANES) spectroscopy and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the oxidation state and elemental associations of Se in common primary emission sources and ambient aerosols collected from the greater Atlanta area. In the majority of ambient aerosol and primary emission source samples, the spectroscopic patterns as well as the absence of elemental correlations suggest Se is in an elemental, organic, or oxide form. XRF microscopy revealed numerous Se-rich particles, or hotspots, accounting on average for ∼16% of the total Se in ambient aerosols. Hotspots contained primarily Se(0)/Se(-II). However, larger, bulk spectroscopic characterizations revealed Se(IV) as the dominant oxidation state in ambient aerosol, followed by Se(0)/Se(-II) and Se(VI). Se(IV) was the only observed oxidation state in gasoline, diesel, and coal fly ash, while biomass burning contained a combination of Se(0)/Se(-II) and Se(IV). Although the majority of Se in aerosols was in the most toxic form, the Se concentration is well below the California Environmental Protection Agency chronic exposure limit (∼20000 ng/m(3)). PMID:25075640

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

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

    PubMed

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

    2014-02-27

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-02-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  9. Urban emission hot spots as sources for remote aerosol deposition

    NASA Astrophysics Data System (ADS)

    Kunkel, D.; Lawrence, M. G.; Tost, H.; Kerkweg, A.; Jöckel, P.; Borrmann, S.

    2012-01-01

    Large point sources such as major population centers (MPCs) emit pollutants which can be deposited nearby or transported over long distances before deposition. We have used tracer simulations of aerosols emitted from MPCs worldwide to assess the fractions which are deposited at various distances away from their source location. Considering only source location, prevailing meteorology, and the aerosol size and solubility, we show that fine aerosol particles have a high potential to pollute remote regions. About half of the emitted mass of aerosol tracers with an ambient diameter ≤1.0 μm is typically deposited in regions more than 1000 km away from the source. Furthermore, using the Köppen-Geiger climate classification to categorize the sources into various climate classes we find substantial differences in the deposition potential between these classes. Tracers originating in arid regions show the largest remote deposition potentials, with values more than doubled compared to the smallest potentials from tracers in tropical regions. Seasonal changes in atmospheric conditions lead to variations in the remote deposition potentials. On average the remote deposition potentials in summer correspond to about 70-80% of the values in winter, with a large spread among the climate classes. For tracers from tropical regions the summer remote deposition values are only about 31% of the winter values, while they are about 95% for tracers from arid regions.

  10. 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.

  11. 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

  12. 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.

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

    NASA Astrophysics Data System (ADS)

    Chien, C. T.; Paytan, A.

    2014-12-01

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

  14. Atmospheric aerosol composition and source apportionments to aerosol in southern Taiwan

    NASA Astrophysics Data System (ADS)

    Tsai, Ying I.; Chen, Chien-Lung

    In this study, the chemical characteristics of winter aerosol at four sites in southern Taiwan were determined and the Gaussian Trajectory transfer coefficient model (GTx) was then used to identify the major air pollutant sources affecting the study sites. Aerosols were found to be acidic at all four sites. The most important constituents of the particulate matter (PM) by mass were SO 42-, organic carbon (OC), NO 3-, elemental carbon (EC) and NH 4+, with SO 42-, NO 3-, and NH 4+ together constituting 86.0-87.9% of the total PM 2.5 soluble inorganic salts and 68.9-78.3% of the total PM 2.5-10 soluble inorganic salts, showing that secondary photochemical solution components such as these were the major contributors to the aerosol water-soluble ions. The coastal site, Linyuan (LY), had the highest PM mass percentage of sea salts, higher in the coarse fraction, and higher sea salts during daytime than during nighttime, indicating that the prevailing daytime sea breeze brought with it more sea-salt aerosol. Other than sea salts, crustal matter, and EC in PM 2.5 at Jenwu (JW) and in PM 2.5-10 at LY, all aerosol components were higher during nighttime, due to relatively low nighttime mixing heights limiting vertical and horizontal dispersion. At JW, a site with heavy traffic loadings, the OC/EC ratio in the nighttime fine and coarse fractions of approximately 2.2 was higher than during daytime, indicating that in addition to primary organic aerosol (POA), secondary organic aerosol (SOA) also contributed to the nighttime PM 2.5. This was also true of the nighttime coarse fraction at LY. The GTx produced correlation coefficients ( r) for simulated and observed daily concentrations of PM 10 at the four sites (receptors) in the range 0.45-0.59 and biases from -6% to -20%. Source apportionment indicated that point sources were the largest PM 10 source at JW, LY and Daliao (DL), while at Meinung (MN), a suburban site with less local PM 10, SO x and NO x emissions, upwind

  15. 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.

  16. 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.

  17. 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.

  18. Identification of sources of Phoenix aerosol by positive matrix factorization.

    PubMed

    Ramadan, Z; Song, X H; Hopke, P K

    2000-08-01

    Chemical composition data for fine and coarse particles collected in Phoenix, AZ, were analyzed using positive matrix factorization (PMF). The objective was to identify the possible aerosol sources at the sampling site. PMF uses estimates of the error in the data to provide optimum data point scaling and permits a better treatment of missing and below-detection-limit values. It also applies nonnegativity constraints to the factors. Two sets of fine particle samples were collected by different samplers. Each of the resulting fine particle data sets was analyzed separately. For each fine particle data set, eight factors were obtained, identified as (1) biomass burning characterized by high concentrations of organic carbon (OC), elemental carbon (EC), and K; (2) wood burning with high concentrations of Na, K, OC, and EC; (3) motor vehicles with high concentrations of OC and EC; (4) nonferrous smelting process characterized by Cu, Zn, As, and Pb; (5) heavy-duty diesel characterized by high EC, OC, and Mn; (6) sea-salt factor dominated by Na and Cl; (7) soil with high values for Al, Si, Ca, Ti, and Fe; and (8) secondary aerosol with SO4(-2) and OC that may represent coal-fired power plant emissions. For the coarse particle samples, a five-factor model gave source profiles that are attributed to be (1) sea salt, (2) soil, (3) Fe source/motor vehicle, (4) construction (high Ca), and (5) coal-fired power plant. Regression of the PM mass against the factor scores was performed to estimate the mass contributions of the resolved sources. The major sources for the fine particles were motor vehicles, vegetation burning factors (biomass and wood burning), and coal-fired power plants. These sources contributed most of the fine aerosol mass by emitting carbonaceous particles, and they have higher contributions in winter. For the coarse particles, the major source contributions were soil and construction (high Ca). These sources also peaked in winter.

  19. 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

  20. Aerosol light scattering measurements as a function of relative humidity.

    PubMed

    Day, D E; Malm, W C; Kreidenweis, S M

    2000-05-01

    The hygroscopic nature of atmospheric fine aerosol was investigated at a rural site in the Great Smoky Mountains National Park during July and August 1995. Passing the sample aerosol through an inlet, which housed an array of Perma Pure diffusion dryers, controlled the sample aerosol's relative humidity (RH). After conditioning the aerosol sample in the inlet, the light scattering coefficient and the aerosol size distribution were simultaneously measured. During this study, the conditioned aerosol's humidity ranged between 5% < RH < 95%. Aerosol response curves were produced using the ratio bspw/bspd; where bspw is the scattering coefficient measured at some RH greater than 20% and bspd is the scattering coefficient of the "dry" aerosol. For this work, any sample RH values below 15% were considered dry. Results of this investigation showed that the light scattering ratio increased continuously and smoothly over the entire range of relative humidity. The magnitude of the ratio at a particular RH value, however, varied considerably in time, particularly for RH values greater than approximately 60%. Curves of the scattering coefficient ratios as a function of RH were generated for each day and compared to the average 12-hour chemical composition of the aerosol. This comparison showed that for any particular RH value the ratio was highest during time periods of high sulfate concentrations and lowest during time periods of high soil or high organic carbon concentrations.

  1. 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.

  2. 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

  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. 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.

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

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu Hemant

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

  6. The Composition of Droplet-Forming Aerosol as a Function of Supersaturation

    NASA Astrophysics Data System (ADS)

    Friedman, B.; Browne, E. C.; Ardon-Dryer, K.; Carrasquillo, A. J.; Daumit, K. E.; Boulanger, K.; Kroll, J. H.; Thornton, J. A.; Cziczo, D. J.

    2013-12-01

    Ambient aerosol measurements were conducted during February 2013 as part of the Department of Energy's Two Column Aerosol Project (TCAP). Located in North Truro, MA, the site provided access to a variety of air mass sources, including marine, continental, and aged urban outflow. A CCN closure study was conducted with measurements from a commercial Cloud Condensation Nuclei Counter (CCNC, Droplet Measurement Technologies) at a range of supersaturation conditions, as well as an Aerosol Mass Spectrometer (AMS, Aerodyne). Further measurements were conducted utilizing a Pumped Counterflow Virtual Impactor (PCVI) in order to separate the activated droplets, as a function of supersaturation, from un-activated aerosol at the output of the CCNC. Subsequent composition measurements of the droplet residuals were conducted with the AMS. High-resolution residual aerosol composition will be presented as a function of instrument supersaturation and air mass, and will be compared to the total ambient aerosol composition. Results indicate an enhancement of nitrate as well as compositional differences between the organic content of the un-activated aerosol and the droplet residuals. The advantages and disadvantages of the CCNC/PCVI/AMS instrumental setup will be discussed with a focus on how this new technique allows for an improvement in our understanding of warm cloud formation.

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

  9. 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

  10. 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

  11. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  13. 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.

  14. Study of the CCN formation as a function of aerosol components

    NASA Astrophysics Data System (ADS)

    Fanourgakis, George S.; Myriokefalitakis, Stelios; Kanakidou, Maria

    2016-04-01

    Understanding the role of aerosols in Earth's climate through direct and indirect effects has attracted a lot of attention over the last years. Due to the chemical complexity of aerosols along with the variety of the primary emissions sources and the conversions from gas to particle in atmosphere, accurate predictions for the aerosols impact on a regional and global scale still remains a challenging problem. In this study, we examine the relative contribution of directly emitted particles in the atmosphere (primary particles) and particles formed from gas-to-particle conversion (secondary particles) to the global aerosols and to the cloud condensation nuclei (CCN) formation. The Chemistry Transport Model v4.0 (TM4-ECPL) coupled with an extended version of the aerosol micro-physics model M7, which describes microphysical processes (nucleation, coagulation, condensation of gas-phase species) for sulfate, black carbon, organic carbon sea salt, dust and various secondary organic aerosols, is here used. A systematic analysis on the CCN production as a function of the aerosol chemical composition is performed. The sensitivity of the results to physical parameters that affect the CCN formation and cannot be accurately determined, such as hygroscopicity, is investigated based on a detailed sensitivity analysis. This work has been supported by the European FP7 collaborative project BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding).

  15. 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

  16. 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.

  17. 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.

  18. 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

  19. 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

  20. 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.

  1. 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. PMID:23844635

  2. 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.

  3. 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

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

    DOEpatents

    Reilly, Peter T. A.

    2007-08-14

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

  5. 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.

  6. 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.

  7. 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

  8. Investigating water soluble organic aerosols: Sources and evolution

    NASA Astrophysics Data System (ADS)

    Hecobian, Arsineh N.

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

  9. 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).

  10. Polar Nephelometer Measurements of Aerosol Phase Functions: Calibration and Field Measurements in Hawaii and the UAE

    NASA Astrophysics Data System (ADS)

    Porter, J. N.

    2005-12-01

    A custom polar nephelometer was built to make open air aerosol phase function measurements. The system is calibrated using filtered air as well as known aerosols. Measurements of aerosol phase functions were made in Hawaii and the United Arab Emirates. Using Mie and Pollack and Cuzzi code, aerosol size distributions are inverted. Time permiting these results will be compared with aerosol size distribution measurements obtained by other techniques.

  11. 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

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  15. 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.

  16. 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.

  17. 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...

  18. “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...

  19. MISR observations at dust source regions: 10-year analysis of aerosol properties and plume heights.

    NASA Astrophysics Data System (ADS)

    Kalashnikova, Olga; Sokolik, Irina; Garay, Michael; Wu, Dong

    Multiangle remote sensing, in particular from Terra/MISR, provides a unique, independent source of data for study dust emission and transport. MISR/Terra is an imaging instrument that uses combination of multi-spectral and multi-angle data to retrieve aerosol properties and aerosol plume heights. A number of validation studies have shown that MISR provides reliable optical depth values over the bright desert. We use the 10-year aerosol data record from the Multi-angle Imaging SpectroRadiometer (MISR) aboard the Terra satellite to investigate the inter-annual and seasonal variability of dust loadings and properties as retrieved by MISR at selected dust source regions. In particular, we examine the Taklamakan, East and Central Gobi regions in Asia, and Mauritania desert and Bodélé Basin regions in Africa. Within each ee selected region, the analysis was performed to examine the multi-annual mean and variability of the aerosol optical depth and particle properties, taking into account the effects of MISR sampling and cloud coverage. To avoid the gridding and averaging effects as much as possible we use the instantaneous Level 2 MISR data for the analysis. We use AERONET data and other independent measurements where available to supplement and constrain MISR product. In addition to the optical depth/property analysis, we report 10-year climatology of dust plume heights over Bodélé Basin as function of the distance from the source. We demonstrate that, ee while there are some effects of large-scale dynamics on dust loadings and heights, the various differences in anomaly time series (including month-to-month differences) reveal the role of meso-scale systems specific to the each source region. These source-specific differences provide valuable information for testing/validating the regional dust transport models. The results will be presented and interpreted in the context of atmospheric dynamics variability, including variability of meteorological regimes in dust

  20. Insights Into Water-Soluble Organic Aerosol Sources From Carbon-13 Ratios of Size Exclusion Chromatography Fractions

    NASA Astrophysics Data System (ADS)

    Ruehl, C. R.; Chuang, P. Y.; McCarthy, M. D.

    2008-12-01

    Many sources of organic aerosols have been identified and quantified, and much of this work has used individual (mosty water-insoluble) compounds as tracers of primary sources. However, most organic aerosol cannot be molecularly characterized, and the water-soluble organic carbon (WSOC) in many aerosols is thought to originate from gaseous precursors (i.e., it is secondary in nature). It can therefore be difficult to infer aerosol sources, particularly of background (i.e., aged) aerosols, and of the relatively high-MW component of aerosols. The stable isotope ratios (δ13C) of organic aerosols have been used to distinguish between sources, with lighter values (-30‰ to -25‰) interpreted as having originated from fossil fuel combustion and C4 biogenic emission, and heavier values (-25‰ to - 20‰) indicating a marine or C3 biogenic source. Most published measurements were of either total suspended particulates or PM2.5, however, and it is unknown to what extent these fractions differ from submicron WSOC. We report δ13C for submicron WSOC collected at a variety of sites, ranging from marine to polluted to background continental. Bulk marine organic δ13C ranged from -30.4 to - 27.6‰, slightly lighter than previously published results. This could be due to the elimination of supermicron cellular material or other biogenic primary emissions from the sample. Continental WSOC δ13C ranged from -19.1 to -29.8‰, with heavier values (-19.8 ± 1.0‰) in Oklahoma and lighter values at Great Smoky Mountain National Park in Tennessee (-25.8 ± 2.6‰) and Illinois (-24.5 ± 1.0‰). This likely results from the greater proportional of C3 plant material in the Oklahoma samples. In addition to bulk samples, we used size exclusion chromatography (SEC) to report δ13C of organic aerosols as a function of hydrodynamic diameter. Variability and magnitude of hydrodynamic diameter was greatest at low SEC pH, indicative of the acidic character of submicron WSOC. Tennessee

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  3. 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

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

    DOE PAGES

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

  5. 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...

  6. 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

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

    PubMed

    Dillon, Michael B

    2011-06-22

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

  8. Aerosol source plume physical characteristics from space-based multiangle imaging

    NASA Astrophysics Data System (ADS)

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

    2007-06-01

    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.

  9. Columnar Aerosol Single-Scattering Albedo and Phase Function Retrieved from Sky Radiance Over the Ocean: Measurements of African Dust

    NASA Technical Reports Server (NTRS)

    Cattrall, Christopher; Carder, Kendall L.; Gordon, Howard R.

    2001-01-01

    The single-scattering albedo and phase function of African mineral dust are retrieved from ground-based measurements of sky radiance collected in the Florida Keys. The retrieval algorithm employs the radiative transfer equation to solve by iteration for these two properties which best reproduce the observed sky radiance using an assumed aerosol vertical structure and measured aerosol optical depth. Thus, no assumptions regarding particle size, shape, or composition are required. The single-scattering albedo, presented at fourteen wavelengths between 380 and 870 nm, displays a spectral shape expected of iron-bearing minerals but is much higher than current dust models allow. This indicates the absorption of light by mineral dust is significantly overestimated in climate studies. Uncertainty in the retrieved albedo is less than 0.02 due to the small uncertainty in the solar-reflectance-based calibration (12.2%) method employed. The phase function retrieved at 860 nm is very robust under simulations of expected experimental errors, indicating retrieved phase functions at this wavelength may be confidently used to describe aerosol scattering characteristics. The phase function retrieved at 443 nm is very sensitive to expected experimental errors and should not be used to describe aerosol scattering. Radiative forcing by aerosol is the greatest source of uncertainty in current climate models. These results will help reduce uncertainty in the absorption of light by mineral dust. Assessment of the radiative impact of aerosol species is a key component to NASA's Earth System Enterprise.

  10. 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

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

    NASA Astrophysics Data System (ADS)

    Chen, Yang; Yang, Fumo

    2016-04-01

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

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

    EPA Science Inventory

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

  13. 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

  14. 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.

  15. 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.

  16. Functional group composition of organic aerosol from combustion emissions and secondary processes at two contrasted urban environments

    NASA Astrophysics Data System (ADS)

    El Haddad, Imad; Marchand, Nicolas; D'Anna, Barbara; Jaffrezo, Jean Luc; Wortham, Henri

    2013-08-01

    The quantification of major functional groups in atmospheric organic aerosol (OA) provides a constraint on the types of compounds emitted and formed in atmospheric conditions. This paper presents functional group composition of organic aerosol from two contrasted urban environments: Marseille during summer and Grenoble during winter. Functional groups were determined using a tandem mass spectrometry approach, enabling the quantification of carboxylic (RCOOH), carbonyl (RCOR‧), and nitro (RNO2) functional groups. Using a multiple regression analysis, absolute concentrations of functional groups were combined with those of organic carbon derived from different sources in order to infer the functional group contents of different organic aerosol fractions. These fractions include fossil fuel combustion emissions, biomass burning emissions and secondary organic aerosol (SOA). Results clearly highlight the differences between functional group fingerprints of primary and secondary OA fractions. OA emitted from primary sources is found to be moderately functionalized, as about 20 carbons per 1000 bear one of the functional groups determined here, whereas SOA is much more functionalized, as in average 94 carbons per 1000 bear a functional group under study. Aging processes appear to increase both RCOOH and RCOR‧ functional group contents by nearly one order of magnitude. Conversely, RNO2 content is found to decrease with photochemical processes. Finally, our results also suggest that other functional groups significantly contribute to biomass smoke and SOA. In particular, for SOA, the overall oxygen content, assessed using aerosol mass spectrometer measurements by an O:C ratio of 0.63, is significantly higher than the apparent O:C* ratio of 0.17 estimated based on functional groups measured here. A thorough examination of our data suggests that this remaining unexplained oxygen content can be most probably assigned to alcohol (ROH), organic peroxides (ROOH

  17. Source apportionment of aerosol iron in the marine environment using iron isotope analysis

    NASA Astrophysics Data System (ADS)

    Mead, Chris; Herckes, Pierre; Majestic, Brian J.; Anbar, Ariel D.

    2013-11-01

    (Fe) is a critical nutrient for phytoplankton. In the open ocean, this demand coupled with scarce supply often makes Fe the limiting factor in phytoplankton growth. The largest source, by mass, of Fe to the open ocean is windblown soil dust, but this Fe is much less soluble than Fe from other aerosol sources. Therefore, to fully understand how Fe reaches this ecosystem, it is necessary to understand the range of sources of aerosol Fe. To do this, we collected size-segregated aerosol samples from Bermuda and analyzed them to determine their Fe isotope composition. From this analysis, we found clear evidence in the fine size fraction (< 2.5 µm) of an important non-soil-dust Fe source. Our isotope analysis of multiple oil and coal fly ashes shows that those materials cannot explain our finding. We suggest biomass burning as the most likely source.

  18. 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

  19. 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.

  20. Source apportionment of ambient aerosol applying PMF on AMS mobile and stationary data

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Weimer, S.; Richter, R.; Decarlo, P. F.; Chirico, R.; Heringa, M. F.; Prévôt, A. S. H.; Baltensperger, U.

    2009-04-01

    Ambient aerosols are divided into the categories "primary" and "secondary", referring to particles directly emitted into the air, or formed out of precursor species such as volatile organic compounds, respectively. Main sources for primary urban aerosol and precursor species are traffic emissions, but also wood burning for domestic heating purposes especially in winter time (Alfarra et al., 2007). The quantification of various types of aerosol components is important for source identification which in turn is the basis of all mitigation activities. Positive Matrix Factorization (PMF) is a statistical based source apportionment tool that uses constrained, weighted least squares estimation to determine source profiles and strengths. PMF has been applied recently for the first time on highly time resolved organic mass spectra (Lanz et al., 2007) measured by an Aerodyne aerosol mass spectrometer (AMS) (Canagaratna et al., 2007). For the data presented here, two AMS were deployed together with additional instrumentation in the metropolitan area of Zurich in winter 2007/2008. The high-resolution time-of-flight AMS was stationed at an urban background site in the center, 30 meters from and shielded against direct traffic emissions. The quadrupole-based AMS was deployed in a mobile van allowing for on-road submicron aerosol composition measurements, and investigations into the spatial variability of aerosol concentration and composition. Results indicate that traffic emissions are the main contributor to submicron aerosol concentrations measured on-road. Hydrocarbon-like organic aerosol (HOA), a marker for traffic emissions (Lanz et al. 2007), dominates the primary aerosol mass, together with black carbon (BC). BC was monitored with the MAAP (multi angle absorption photometer). Another significant contributor to primary organic aerosol mass in downtown Zurich is domestic wood burning for heating purposes. Traffic and wood burning emissions make up roughly 50% of the total

  1. Monte Carlo simulation of light scattering in the atmosphere and effect of atmospheric aerosols on the point spread function.

    PubMed

    Colombi, Joshua; Louedec, Karim

    2013-11-01

    We present a Monte Carlo simulation for the scattering of light in the case of an isotropic light source. The scattering phase functions are studied particularly in detail to understand how they can affect the multiple light scattering in the atmosphere. We show that, although aerosols are usually in lower density than molecules in the atmosphere, they can have a non-negligible effect on the atmospheric point spread function. This effect is especially expected for ground-based detectors when large aerosols are present in the atmosphere.

  2. 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.

  3. 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.

  4. 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.

  5. 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

  6. 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...

  7. Trace elements and metal pollution in aerosols at an alpine site, New Zealand: Sources, concentrations and implications

    NASA Astrophysics Data System (ADS)

    Marx, Samuel K.; Lavin, Karen S.; Hageman, Kimberly J.; Kamber, Balz S.; O'Loingsigh, Tadhg; McTainsh, Grant H.

    2014-01-01

    Atmospheric aerosol samples were collected at a remote site in New Zealand's Southern Alps. Collected samples were found to be a mixture of New Zealand and Australian sourced sediment, using their trace element signatures. Aerosol concentrations and the relative contribution of different sources was found to be a function of specific air-mass trajectories influencing the study site, dust entrainment rates in source areas and rainfall. Results show that Australian dust is a major source of particulate matter in New Zealand, particularly in remote alpine locations; however, locally derived dust is also important. Metal pollutants, including Pb, Cu and Sn, were enriched in the samples by approximately 15 times and up to >100 times expected natural concentrations, confirming that metal pollution is a ubiquitous component of the atmosphere, even in relatively remote locations. Moreover, pollutants were highly enriched in otherwise clean air, i.e. during and following rainfall. Additionally, high concentrations of elements naturally enriched in sea water, e.g. Sr, Ba and Rb, were deposited alongside mineral dust, reflecting the oceanic origin of air influencing the site and the role of sea spray in contributing aerosol to the atmosphere. These elements experienced the greatest enrichment during rainfall, implying sea spray and pollution become relatively important during otherwise clean air conditions.

  8. 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.

  9. 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.

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

    PubMed

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

    2011-10-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2007-01-01

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

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  14. 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

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

    SciTech Connect

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

    1985-01-01

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

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

    PubMed

    Phalen, Robert N; Coleman, Ted

    2012-08-01

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

  17. 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

  18. 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

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

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

  20. Annual Patterns and Sources of Light-Absorbing Aerosols over Central Greenland

    NASA Astrophysics Data System (ADS)

    Hu, J.; Bergin, M. H.; Dibb, J. E.; Sheridan, P. J.; Ogren, J. A.

    2014-12-01

    The Arctic region has proven to be more responsive to recent changes in climate than other parts of the Earth. A key component of the Arctic climate is the Greenland ice sheet (GIS), which has the potential to dramatically influence sea level, depending on the amount of melting that occurs, as well as climate, through shifts in the regional radiation balance. Light-absorbing aerosols from biomass burning, fossil fuel combustion, and dust sources can potentially have a significant impact on the radiation balance of the GIS; however, in order to better understand their impact, it is important to first understand the annual trends of light-absorbing aerosols and their sources over the ice sheet. With this in mind, aerosol properties including the wavelength dependent aerosol light scattering and absorption coefficients have been continuously measured at Summit, Greenland since the spring of 2011. These measurements will be used to calculate the multi-wavelength single-scattering albedo (ω0) and absorption Ångström exponent, identify annual patterns of aerosols over the GIS and how they vary from year to year, detect events of high absorption, and determine the sources of the aerosols. Preliminary findings indicate that the aerosols have an absorption Ångström exponent of approximately 1, which is characteristic of black carbon (BC). Absorption and scattering coefficients are higher in the spring and summer (March-September) and consequently lower in the fall and winter (September-March). Absorption and single-scattering albedo are averaged over the sunlit months of April-August and are found to be highest and lowest, respectively, in the year of 2012, corresponding to the year of record melt extent over the GIS.

  1. 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.

  2. 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

  3. 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

  4. 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

  5. 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

  6. Fossil and modern sources of aerosol carbon in the Netherlands - A year-long radiocarbon study

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike; Monaco, Mattia; Kappetijn, Arthur; Meijer, Harro A. J.; Szidat, Sönke; Röckmann, Thomas

    2013-04-01

    Measurement of the radioactive carbon isotope 14C in aerosols can provide a direct estimate of the contribution of fossil fuel sources to aerosol carbon. In aerosol science, measurements of 14C/12C ratios are usually reported as fraction modern (fm). The radiocarbon signature gives a clear distinction between 'modern' carbon sources (fm around 1.1-1.2 for biomass burning and around 1.05 for biogenic secondary organic aerosol) and 'fossil' carbon sources (fm =0 for primary and secondary formation from fossil fuel combustion). Due to the high cost of 14C analyses very few long-term studies have been conducted to date. The data that will be presented offer a unique insight into the seasonal variation of source contributions to the carbonaceous aerosol in a highly industrialized region. High volume filter samples have been collected roughly twice per month from February 2011 - July 2012 at Cabauw, a rural location in the Netherlands surrounded by major urban centers and highways. This site provides a regional background aerosol contamination in the Netherlands. We report measurements of fm for total carbon (TC), organic carbon (OC), water insoluble OC (WIOC) and thermally refractory carbon (RC) as a proxy for elemental carbon. The fraction modern of OC lies between 0.65 - 1 and shows only a moderate seasonal variation with highest values in the spring and lowest values in the summer. Elemental carbon is generally dominated by fossil fuel emissions, but shows a distinct seasonal variation with higher contribution of modern sources from November - Mai. This contribution is attributed to wood combustion. It is low when air masses arrive from the ocean and high for air masses with European continental origin, pointing to a main source outside the Netherlands. Water soluble organic carbon is dominated by modern sources throughout the year. For TC concentrations between 1.2 and 8 μg/m3, fm(TC) increases with TC concentration. A Keeling plot implies that synoptic scale

  7. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

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

  9. 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.

  10. 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

  11. 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%.

  12. 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

  13. 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.

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

    NASA Astrophysics Data System (ADS)

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

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

  15. 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.

  16. Impacts of sources and aging on submicrometer aerosol properties in the marine boundary layer across the Gulf of Maine

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D.; Onasch, T. B.; Worsnop, D.; Baynard, T.; de Gouw, J. A.; Goldan, P. D.; Kuster, W. C.; Williams, E.; Roberts, J. M.; Lerner, B.; Stohl, A.; Pettersson, A.; Lovejoy, E. R.

    2006-12-01

    Measurements were made on board the NOAA RV Ronald H. Brown during the second New England Air Quality Study (NEAQS 2004) to determine the source of the aerosol in the region and how sources and aging processes affect submicrometer aerosol chemical composition and optical properties. Using the Lagrangian particle dispersion model FLEXPART in combination with gas phase tracer compounds, local (urban), regional (NE U.S. urban corridor of Washington, D.C.; New York; and Boston), and distant (midwest industries and North American forest fires) sources were identified. Submicrometer aerosol measured near the source region (Boston Harbor) had a molar equivalence ratio near one with respect to NH4+, NO3-, and SO4=, had a large mass fraction of particulate organic matter (POM) relative to SO4=, and had relatively unoxidized POM. As distance from the source region increased, the submicrometer aerosol measured in the marine boundary layer became more acidic and had a lower POM mass fraction, and the POM became more oxidized. The relative humidity dependence of light extinction reflected the change in aerosol composition being lower for the near-source aerosol and higher for the more processed aerosol. A factor analysis performed on a combined data set of aerosol and gas phase parameters showed that the POM measured during the experiment was predominantly of secondary anthropogenic origin.

  17. Characterization of sources for southern African aerosols through fatty acid and trajectory analyses

    NASA Astrophysics Data System (ADS)

    Billmark, Kaycie A.; Swap, Robert J.; Macko, Stephen A.

    2003-07-01

    Biogeochemical cycles in southern Africa are affected by emissions from extensive biomass burning. Emitted trace gases and aerosols frequently accumulate and recirculate in the well-defined synoptic pattern that persists for long time periods over southern Africa. The role of organic aerosols during atmospheric transport and the influence of neighboring air masses on biogeochemical dynamics in this nutrient-limited region are insufficiently studied. The Southern African Regional Science Initiative (SAFARI 2000) was conducted in part to investigate the impacts of this large-scale transport and deposition of increasingly anthropogenic emissions on southern African biogeochemical cycling. This study explores the understanding of regional atmospheric transport through the identification of chemical biomarkers to describe aerosols collected during the SAFARI 2000 dry season research campaign. Total suspended particulate aerosol samples were collected diurnally for a period of two weeks in Mongu, Zambia. Mongu is bordered by the Zambezi River on the west and the Miombo woodland savanna in all other directions. It also lies on the northern extent of the Kalahari Desert. This region is characterized by high biomass burning emissions of river floodplain grasses and woodland savanna during the dry season. Fatty acids were extracted from the collected aerosols and analyzed using gas chromatography. The resultant fatty acid compositions were examined for temporal patterns and trends. Furthermore, these results were compared to both synoptic meteorological patterns over the region, as well as to modeled air parcel trajectories, to gain insight into changes in aerosol composition resulting from changes in atmospheric transports from regions of different vegetation. The results of these analyses confirm that abundances of fatty acids are dependent on local and synoptic meteorology and can thus be used as an additional geochemical tracer to better describe aerosol sources and

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

    SciTech Connect

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

    1980-08-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-10-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2012-02-01

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

  1. Pulmonary function and clearance after prolonged sulfuric acid aerosol exposure

    SciTech Connect

    Ives, P.J. ); Gerrity, T.R.; DeWitt, P.; Folinsbee, L.J. )

    1991-03-15

    The authors studied pulmonary function and clearance responses after a 4 H exposure to 75-100 {mu}g/m{sup 3} sulfuric acid aerosol (SAA). Healthy subjects, who exercised for 30 min/H at ventilation of about 25 L/min, were exposed once to clean air and once to SAA. Oral hygiene and acidic juice gargle were used to minimize oral ammonia. Lung function tests, including spirometry, plethysmography, and partial flow-volume (PEFV) curves were performed before and after exposure. Clearance of 99m-Technetium labeled iron oxide was assessed after each exposure. The first moment of fractional tracheobronchial retention (M1TBR), after correcting for 24 H retention and normalizing to time zero, was used as an index of clearance. There were no significant changes in lung volumes, airways resistance, or maximum expiratory flows after SAA exposure. Flow at 40% of total lung capacity on PEFV curves decreased 17% (NS) after SAA exposure. Tracheobronchial clearance was accelerated after a single exposure to SAA; M1TBR decreased from 73 {plus minus} 5 min (air) to 69 {plus minus} 5 min (SAA). These results suggest that acute prolonged exposure to low levels of SAA has minimal effects on lung mechanics in healthy subjects but does produce a modest acceleration of particle clearance.

  2. 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

  3. 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...

  4. 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.

  5. 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.

  6. 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.

  7. Sources of carbonaceous aerosol in the free troposphere

    NASA Astrophysics Data System (ADS)

    Timonen, H.; Jaffe, D. A.; Wigder, N.; Hee, J.; Gao, H.; Pitzman, L.; Cary, R. A.

    2014-08-01

    In this study concentrations of organic (OC) and elemental carbon (EC) from free tropospheric (FT) fine particulate matter (PM) were measured from March to September, 2012 with a Semi-Continuous OC/EC carbon aerosol analyzer at the top of Mt. Bachelor (2.8 km a.s.l) in Central Oregon, U.S. The average concentrations of OC and EC in the FT were low (OC: 1.87 ± 6.10, EC: 0.07 ± 0.26 μg m-3; average ± SD) but much higher during specific pollution episodes. During springtime the highest OC and EC concentrations were measured for dry free tropospheric air masses, whereas during summertime the highest OC and EC concentrations were typically measured for more humid air masses that were uplifted from the boundary layer (BL). The highest OC and EC concentrations were measured during biomass burning episodes (3 h average OC: up to 146.0 μg m-3, EC up to 5.5 μg m-3). Elevated OC and EC concentrations were also measured during Asian Long Range Transport (LRT) episodes (OC: up to 3.6 μg m-3, EC up to 1.1 μg m-3). In addition, between episodes, an increase in OC was seen in the afternoon, possibly due to SOA formation. This SOA can then be exported to the FT via diurnal ventilation of the BL. For Asian LRT episodes the OC/EC ratios varied between 8 and 34, with an average of 17.9. For local biomass burning emissions OC/EC ratios were between 25 and 30. Higher OC/EC ratios (30-40) were observed for the biomass burning plumes originating from longer distances, possibly due to SOA formation.

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

    NASA Astrophysics Data System (ADS)

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

    2012-01-01

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

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

    PubMed

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

    2014-01-15

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

  10. 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.

  11. The ambient organic aerosol soluble in water: Measurements, chemical characterization, and an investigation of sources

    NASA Astrophysics Data System (ADS)

    Sullivan, Amy P.

    This thesis characterizes the ambient fine organic carbon (OC) aerosol and investigates its sources through the development and deployment of new analytical measurement techniques. Recognizing that OC is highly chemically complex, the approach was to develop methods capable of quantitatively measuring a large chemical fraction of the aerosol instead of specific chemical speciation. The focus is on organic compounds that are soluble in water (WSOC) since little is known about its chemical nature. The results from this thesis show that WSOC has mainly two sources: biomass burning and secondary organic aerosol (SOA). In urban areas, WSOC increases with plume age, and tracks other photochemically produced compounds. Chemical analysis of WSOC suggests that in urban Atlanta, the SOA is mainly small-chain aliphatic compounds indirectly linked to vehicle emissions. A method was first developed for quantitative on-line measurements of WSOC by extending the application of the Particle-into-Liquid Sampler (PILS) from inorganic to organic aerosol measurements. In this approach a PILS captures ambient particles into a flow of purified water, which is then forced through a liquid filter and the carbonaceous content quantified on-line by a Total Organic Carbon (TOC) analyzer. An instrument was first developed for ground-based measurements and then modified for airborne deployment. Ground-based measurements at the St. Louis - Midwest Supersite during the summer of 2003 showed that the fraction of OC that is water-soluble can have a highly diurnal pattern with WSOC to OC ratios reaching 0.80 during the day and lows of 0.40 during the night. During extended periods under stagnation pollution events, this pattern was well correlated with ozone concentrations. The results are consistent with formation of SOA. Airborne PILS-TOC measurements from the NOAA WP-3D during the New England Air Quality Study/Intercontinental Transport and Chemical Transformation (NEAQS/ITCT) 2004 program

  12. 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

  13. 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.

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

    PubMed

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

    2016-01-01

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

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

    PubMed

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

    2016-07-20

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

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

    PubMed

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

    2007-07-01

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

  17. 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...

  18. 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.

  19. Experimentation and modelling of mineral aerosol dissolution as source of transition metals in cloud droplets

    NASA Astrophysics Data System (ADS)

    Desboeufs, K.; Sofikitis, A.; Velay, J.; Losno, R.; Dulac, F.; Colin, J.

    2004-12-01

    Even at nano-molar concentrations, transition metals (TMI) could play an important role in the radical chemistry of the atmospheric liquid phase. For instance, cloud chemistry model calculations suggest that depletion of HOx by reactions between TMI and HO2/O2- radicals significantly slows down O3 production in polluted clouds. TMI are transferred into the liquid phase from aerosol particles by dissolution processes which can be a slow reaction. The dissolution kinetic of the solid phase thus competes with chemical kinetics in the homogeneous aqueous phase. It is therefore of importance to consider the evolution of TMI concentrations into cloud droplets in order to quantify the atmospheric impact of aerosols on the aqueous chemistry. Mineral particles including soil-derived particles and fly-ash are important sources of TMI in the troposphere.In order to parameterize the dissolution kinetic and concentrations of TMI from mineral particles into cloud droplets, we have conducted experimental laboratory simulations which mimic particles/water interactions occurring into droplets. These simulations were carried out in an open-flow reactor for typical atmospheric conditions (pH, ionic strength.). Data on TMI dissolution kinetic are provided for two generic kinds of mineral matrices from anthropogenic and natural sources: alumino-silicated and carbonaceous particles (dust, fly-ash, or urban particles). The concentrations of TMI released depend on pH, matrix type and particle-water contact time. The metals coming from carbonaceous particles are adsorbed impurities or salts and are very soluble with dissolution hardly dependent on pH. On the opposite, the metals dissolved from alumino-silicated particles are less soluble, notably the ones constitutive of the matrix network (Fe, Mn), and their dissolution is highly influenced by the pH. However, at a given pH, the results on the kinetic of dissolution emphasize that whatever the matrix, the TMI dissolution rates decrease

  20. 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).

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

    PubMed

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

    2015-09-01

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

  2. 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

  3. 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.

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

    PubMed

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

    2015-09-01

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

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

    PubMed

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

    2016-11-15

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

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

    PubMed

    Itahashi, Syuichi; Uno, Itsushi; Kim, Soontae

    2012-06-19

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

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

    PubMed

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

    2016-06-01

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

  8. 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.

  9. 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

    2016-05-25

    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.

  10. 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.

  11. 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

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  14. 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.

  15. Submicron Organic Aerosol Function Groups during the International Chemistry Experiment in the Arctic LOwer Troposphere (ICEALOT)

    NASA Astrophysics Data System (ADS)

    Russell, L. M.; Shaw, P. M.; Quinn, P. K.; Bates, T. S.

    2008-12-01

    Aerosol organic mass (OM) components are expected to have significant direct and indirect impacts on Arctic climate, especially during springtime Arctic haze. The chemical and physical properties of OM in Arctic aerosol remain largely unconstrained. The R/V Knorr traveled between Iceland and the Barents Sea during the ice-free months of March and April of 2008 and collected submicron particles on teflon filters for Fourier Transform Infrared (FTIR) spectroscopy to identify and quantify organic functional groups. Time series and composition are presented along with air mass back trajectories to indicate source regions. Early findings identify alcohols, alkanes, and carboxylic acids, with smaller amounts of amines, aromatics, alkenes and carbonyls. These data show the important contributions of organic oxygen and nitrogen in the Arctic region. Single particle analysis by Near-edge X-ray Absorption Fine Structure (NEXAFS) Scanning Transmission X- ray Microscopy (STXM) provides additional information about the distribution and morphology of the types of organic particles. Comparison to collocated simultaneous measurements by other techniques showed good agreement for OM and oxygenated organic fractions.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-11-01

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

  18. 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.

  19. 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.

  20. Burning of olive tree branches: a major organic aerosol source in the Mediterranean

    NASA Astrophysics Data System (ADS)

    Kostenidou, E.; Kaltsonoudis, C.; Tsiflikiotou, M.; Louvaris, E.; Russell, L. M.; Pandis, S. N.

    2013-09-01

    Aerosol produced during the burning of olive tree branches was characterized with both direct source sampling (using a mobile smog chamber) and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8-10% black carbon (BC), 5% potassium, 3-4% sulfate, 2-3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA) consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O : C) ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034-0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O : C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs) such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF) was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%), HOA (hydrocarbon-like organic aerosol, 11.3%) and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.9 g kg-1. Assuming that half of the olive tree branches pruned is burned in Greece, 2300 ± 600 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in Mediterranean countries.

  1. Burning of olive tree branches: a major organic aerosol source in the Mediterranean

    NASA Astrophysics Data System (ADS)

    Kostenidou, E.; Kaltsonoudis, C.; Tsiflikiotou, M.; Louvaris, E.; Russell, L. M.; Pandis, S. N.

    2013-03-01

    Aerosol produced during the burning of olive tree branches was characterized with both direct source-sampling (using a mobile smog chamber) and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8-10% black carbon (BC), 5% potassium, 3-4% sulfate, 2-3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA) consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O:C) ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034-0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O:C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs) such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF) was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%), HOA (hydrocarbon-like organic aerosol, 11.3%) and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.2 g kg-1. Assuming that half of the olive tree branches pruned is burned in Greece 2280 ± 140 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in the Mediterranean countries.

  2. 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.

  3. Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site

    NASA Astrophysics Data System (ADS)

    Takahama, S.; Schwartz, R. E.; Russell, L. M.; MacDonald, A. M.; Sharma, S.; Leaitch, W. R.

    2011-07-01

    Ambient particles collected on teflon filters at the Peak of Whistler Mountain, British Columbia (2182 m a.s.l.) during spring and summer 2009 were measured by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFG). The project mean and standard deviation of organic aerosol mass concentrations (OM) for all samples was 3.2±3.3 (μg m-3). Measurements of aerosol mass fragments, size, and number concentrations were used to separate fossil-fuel combustion and burning and non-burning forest sources of the measured organic aerosol. The OM was composed of the same anthropogenic and non-burning forest components observed at Whistler mid-valley in the spring of 2008; during the 2009 campaign, biomass burning aerosol was additionally observed from fire episodes occurring between June and September. On average, organic hydroxyl, alkane, carboxylic acid, ketone, and primary amine groups represented 31 %±11 %, 34 %±9 %, 23 %±6 %, 6 %±7 %, and 6 %±3 % of OM, respectively. Ketones in aerosols were associated with burning and non-burning forest origins, and represented up to 27 % of the OM. The organic aerosol fraction resided almost entirely in the submicron fraction without significant diurnal variations. OM/OC mass ratios ranged mostly between 2.0 and 2.2 and O/C atomic ratios between 0.57 and 0.76, indicating that the organic aerosol reaching the site was highly aged and possibly formed through secondary formation processes.

  4. 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

  5. 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

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

    NASA Astrophysics Data System (ADS)

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

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

  7. 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

  8. Providing Size-Resolved Mixing State Inputs to Improve Aerosol Optics Models: Comparison of ACE-Asia Aerosol Chemical Measurements for Different Source Regions With Simultaneous Optical Measurements

    NASA Astrophysics Data System (ADS)

    Sullivan, R. C.; Poon, G.; Guazzotti, S.; Sodeman, D.; Holecek, J.; Spencer, M.; Prather, K.

    2005-12-01

    Measurements made of the aerodynamic size and chemical composition of single aerosol particles on board the R/V Ronald H. Brown sailing between Hawaii and the Sea of Japan during ACE-Asia in 2001 revealed a complex mixture of mineral dust, organic carbon, elemental carbon, sulfates, nitrates, chloride, ammonium, and sea salt. The air mass source regions included influences from the Pacific Ocean, Miyakejima volcano, Gobi and Taklimakan Deserts, Shanghai, Japan, and Korea. The particle composition sampled from each of these regions showed unique changes in the aerosol's mixing state. This complexity presents major challenges in accurately modeling the optical properties of the Asian aerosol. The degree of closure between the measured chemical and optical properties of this aerosol and those predicted by models has been presented by Quinn et al. [JGR, 109, D19S01, doi: 10.1029/2003JD004010, 2004]. Differences between measured and calculated aerosol absorption coefficients were partly attributed to the assumption of internally mixed homogeneous spheres for the aerosol population. Good correlations between measured and calculated aerosol mass and light scattering were found but relied on particle shapes not confirmed by measurements. To better our understanding of the relationship between aerosol chemistry and optical measurements, and provide more detailed inputs to improve the predictions of optical models, we present size-resolved single-particle mixing state results obtained by an ATOFMS for the seven air mass source regions described by Quinn et al. (2004). Our results do not support the assumption of a homogeneous internally mixed aerosol population for many of the source regions. Particular focus is given to the mixing state and chemical associations of sulfate, nitrate, chloride, ammonium, OC, EC, dust, and sea salt. We demonstrate the segregation of ammonium, sulfate, and nitrate within individual particles throughout the study and discuss the different

  9. 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.

  10. 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

  11. 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

  12. 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

  13. [Source apportionment of aerosol lead in Beijing using absolute principal component analysis].

    PubMed

    Li, Yu-wu; Liu, Xian-de; Li, Bing; Yang, Hong-xia; Dong, Shu-ping; Zhang, Ting; Guo, Jing

    2008-12-01

    From 18 September 2005 to 13 September 2006 in Beijing, 166 TSP samples were collected at three sites in southern suburb, downtown and northern suburb, respectively. Lead and other 28 elements were determined for those samples by ICP-AES and ICP-MS methods. The lead average concentration of one year in southern suburb, downtown and northern suburb was 179, 142 and 102 ng x m(-3), respectively. Source identification and apportionment were carried out using absolute principal component analysis (APCA) method. Five groups of sources were recognized. The sources are nonferrous metallurgy (55.6%), coal combustion (16.9%), construction dust (11.8%) and soil dust (10.2%), respectively. Major sources of aerosol lead in Beijing were from nonferrous metallurgy industry. Lead associated with coal combustion and other sources were evenly distributed over three sites. However, industrial leadwas apparently at different levels at three sites, higher in southern suburb and lower in northern suburb. The lead concentration originated from nonferrous metallurgy at three sites from southern suburb, downtown to northern suburb was 113, 77.0 and 44.2 ng x m(-3), respectively, implying that the major sources for industrial lead were from the south to the Beijing. There is considerable space for reduction of aerosol lead concentration in Beijing. The main object for lead pollution discharge reduction and environmental management measures should aim at nonferrous metallurgy, especially for the field of lead metallurgy located at the south area to the Beijing. The calculation result based on the same chemical analysis data also shows that major source for TSP in Beijing is of soil dust and construction dust, accounting for 72.3%. The other sources such as coal combustion and nonferrous metallurgy account for 13.4% and 9.5%, respectively.

  14. 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

  15. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

  17. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-08-01

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

  19. 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

  20. The source identification of ambient aerosols in Beijing, China by multivariate analysis coupled with {sup 14}C tracer

    SciTech Connect

    Xiaoyan Tang; Min Shao; Yuanhang Zhang

    1996-12-31

    Ambient aerosol is one of most important pollutants in China. This paper showed the results of aerosol sources of Beijing area revealed by combination of multivariate analysis models and 14C tracer measured on Accelerator Mass Spectrometry (AMS). The results indicated that the mass concentration of particulate (<100 (M)) didn`t increase rapidly, compared with economic development in Beijing city. The multivariate analysis showed that the predominant source was soil dust which contributed more than 50% to atmospheric particles. However, it would be a risk to conclude that the aerosol pollution from anthropogenic sources was less important in Beijing city based on above phenomenon. Due to lack of reliable tracers, it was very hard to distinguish coal burning from soil source. Thus, it was suspected that the soil source above might be the mixture of soil dust and coal burning. The 14C measurement showed that carbonaceous species of aerosol had quite different emission sources. For carbonaceous aerosols in Beijing, the contribution from fossil fuel to ambient particles was nearly 2/3, as the man-made activities ( coal-burning, etc.) increased, the fossil part would contribute more to atmospheric carbonaceous particles. For example, in downtown Beijing at space-heating seasons, the fossil fuel even contributed more than 95% to carbonaceous particles, which would be potential harmful to population. By using multivariate analysis together with 14C data, two important sources of aerosols in Beijing (soil and coal) combustion were more reliably distinguished, which was critical important for the assessment of aerosol problem in China.

  1. 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

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

    NASA Astrophysics Data System (ADS)

    Prather, K. A.

    2014-12-01

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

  3. Chemical information from the source function.

    PubMed

    Gatti, Carlo; Cargnoni, Fausto; Bertini, Luca

    2003-03-01

    The source function, which enables one to equate the value of the electron density at any point within a molecule to a sum of atomic contributions, has been applied to a number of cases. The source function is a model-independent, quantitative measure of the relative importance of an atom's or group's contribution to the density at any point in a system, and it represents a potentially interesting tool to provide chemical information. It is shown that the source contribution from H to the electron density rho(b) at the bond critical point in HX diatomics decreases with increasing X's electronegativity, and that this decrease is a result of significant changes in the Laplacian distribution within the H-basin. It is also demonstrated that the source function from Li to rho(b) in LiX diatomics is a more sensitive index of atomic transferability than it is the lithium atomic energy or population. The observed changes are such as to ensure a constant percentage source contribution from Li to rho(b) throughout the LiX series, rather than a constant source as one would expect in the limit of perfect atomic transferability. Application of the source function to planar lithium clusters has revealed that the source function clearly discriminates between a nonnuclear electron density maximum and a maximum associated to a nucleus, on the basis of the relative weight of the source contributions from the basin associated to the maximum and from the remaining basins in the cluster. The source function has also allowed for a classification of hydrogen bonds in terms of characteristic source contributions to the density at the H-bond critical point from the H involved in the H-bond, the H-donor D, and the H-acceptor A. The source contribution from the H appears as the most distinctive marker of the H-bond strength, being highly negative for isolated H-bonds, slightly negative for polarized assisted H-bonds, close to zero for resonance-assisted H-bonds, and largely positive for

  4. 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

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

    PubMed

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

    2016-07-19

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

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

    PubMed

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

    2016-07-19

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

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

    PubMed

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

    2014-08-01

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

  8. Relating aerosol absorption due to soot, organic carbon, and dust to emission sources determined from in-situ chemical measurements

    NASA Astrophysics Data System (ADS)

    Cazorla, A.; Bahadur, R.; Suski, K. J.; Cahill, J. F.; Chand, D.; Schmid, B.; Ramanathan, V.; Prather, K. A.

    2013-09-01

    Estimating the aerosol contribution to the global or regional radiative forcing can take advantage of the relationship between the spectral aerosol optical properties and the size and chemical composition of aerosol. Long term global optical measurements from observational networks or satellites can be used in such studies. Using in-situ chemical mixing state measurements can help us to constrain the limitations of such estimates. In this study, the Absorption Ångström Exponent (AAE) and the Scattering Ångström Exponent (SAE) derived from 10 operational AERONET sites in California are combined for deducing chemical speciation based on wavelength dependence of the optical properties. In addition, in-situ optical properties and single particle chemical composition measured during three aircraft field campaigns in California between 2010 and 2011 are combined in order to validate the methodology used for the estimates of aerosol chemistry using spectral optical properties. Results from this study indicate a dominance of mixed types in the classification leading to an underestimation of the primary sources, however secondary sources are better classified. The distinction between carbonaceous aerosols from fossil fuel and biomass burning origins is not clear, since their optical properties are similar. On the other hand, knowledge of the aerosol sources in California from chemical studies help to identify other misclassification such as the dust contribution.

  9. Global Aerosols

    Atmospheric Science Data Center

    2013-04-19

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-02-01

    The chemical content of the water soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to: (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for the period when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp < 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. The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m-3 for particles with 0.96 < dp < 1.5 μm to 73.9 ± 12.3 nmol m-3 for particles with dp < 0.49 μm, resulting in molar H / C ratios of 0.48 ± 0.05 to 0.92 ± 0.09 observed in combustion-related organic aerosol. The R-H was the most abundant group representing about 45% of measured total non-exchangeable organic hydrogen concentration followed by H-C-O (27%) and H-C-C= (26%). Levoglucosan, amines, ammonium and methanosulfonate were tentatively 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 aerosol and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from -26.81 ± 0.18‰ for the smallest particles to -25.93 ± 0.31‰ for the largest particles and the relative

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

    The chemical content of water-soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for periods when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp < 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 < dp < 3.0 μm to 73.9 ± 12.3 nmol m-3 for particles with dp < 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 -25.93 ± 0.31‰ for the largest

  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. 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.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  18. Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter

    NASA Astrophysics Data System (ADS)

    Hu, Weiwei; Hu, Min; Hu, Wei; Jimenez, Jose L.; Yuan, Bin; Chen, Wentai; Wang, Ming; Wu, Yusheng; Chen, Chen; Wang, Zhibin; Peng, Jianfei; Zeng, Limin; Shao, Min

    2016-02-01

    To investigate the seasonal characteristics of submicron aerosol (PM1) in Beijing urban areas, a high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) was utilized at an urban site in summer (August to September 2011) and winter (November to December 2010), coupled with multiple state of the art online instruments. The average mass concentrations of PM1 (60-84 µg m-3) and its chemical compositions in different campaigns of Beijing were relatively consistent in recent years. In summer, the daily variations of PM1 mass concentrations were stable and repeatable. Eighty-two percent of the PM1 mass concentration on average was composed of secondary species, where 62% is secondary inorganic aerosol and 20% secondary organic aerosol (SOA). In winter, PM1 mass concentrations changed dramatically because of the different meteorological conditions. The high average fraction (58%) of primary species in PM1 including primary organic aerosol (POA), black carbon, and chloride indicates primary emissions usually played a more important role in the winter. However, aqueous chemistry resulting in efficient secondary formation during occasional periods with high relative humidity may also contribute substantially to haze in winter. Results of past OA source apportionment studies in Beijing show 45-67% of OA in summer and 22-50% of OA in winter can be composed of SOA. Based on the source apportionment results, we found 45% POA in winter and 61% POA in summer are from nonfossil sources, contributed by cooking OA in both seasons and biomass burning OA (BBOA) in winter. Cooking OA, accounting for 13-24% of OA, is an important nonfossil carbon source in all years of Beijing and should not be neglected. The fossil sources of POA include hydrocarbon-like OA from vehicle emissions in both seasons and coal combustion OA (CCOA) in winter. The CCOA and BBOA were the two main contributors (57% of OA) for the highest OA concentrations (>100 µg m-3) in winter. The POA

  19. Oil Sands Operations in Alberta, Canada: A large source of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Liggio, J.; Li, S. M.; Hayden, K.; Taha, Y. M.; Stroud, C.; Darlington, A. L.; Drollette, B.; Gordon, M.; Lee, P.; Liu, P.; Leithead, A.; Moussa, S.; Wang, D.; O'Brien, J.; Mittermeier, R. L.; Brook, J.; Lu, G.; Staebler, R. M.; Han, Y.; Tokarek, T. W.; Osthoff, H. D.; Makar, P.; Zhang, J.; Plata, D.; Gentner, D. R.

    2015-12-01

    Little is known of the reaction products of emissions to the atmosphere from extraction of oil from unconventional sources in the oil sands (OS) region of Alberta, Canada. This study examines these reaction products, and in particular, the extent to which they form secondary organic aerosol (SOA), which can significantly contribute to regional particulate matter formation. An aircraft measurement campaign was conducted over the Athabasca oil sands region between August 13 and September 7, 2013. A broad suite of measurements were made during 22 flights, including organic aerosol mass and composition with a High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and organic aerosol gas-phase precursors by Proton Transfer Reaction (PTR) and off-line gas chromatography mass spectrometry. Large concentrations of organic aerosol were measured downwind of the OS region, which we show to be entirely secondary in nature. Laboratory experiments demonstrated that bitumen (the mined product) contains semi-volatile vapours in the C12-C18 range that will be emitted at ambient temperatures. When oxidized, these vapours form SOA with highly similar HR-ToF-AMS spectra to the SOA measured in the flights. Box modelling of the OS plume evolution indicated that the measured levels of traditional volatile organic compounds (VOCs) are not capable of accounting for the amount of SOA formed in OS plumes. This discrepancy is only reconciled in the model by including bitumen vapours along with their oxidation and condensation into the model. The concentration of bitumen vapours required to produce SOA matching observations is similar to that of traditional VOC precursors of SOA. It was further estimated that the cumulative SOA mass formation approximately 100 km downwind of the OS during these flights, and under these meteorological conditions was up to 82 tonnes/day. The combination of airborne measurements, laboratory experiments and box modelling indicated that semi

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

    PubMed

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

    2015-09-15

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

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

    PubMed

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

    2015-09-15

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

  2. 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.

  3. 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.

  4. Sea spray aerosol as a unique source of ice nucleating particles.

    PubMed

    DeMott, Paul J; Hill, Thomas C J; McCluskey, Christina S; Prather, Kimberly A; Collins, Douglas B; Sullivan, Ryan C; Ruppel, Matthew J; Mason, Ryan H; Irish, Victoria E; Lee, Taehyoung; Hwang, Chung Yeon; Rhee, Tae Siek; Snider, Jefferson R; McMeeking, Gavin R; Dhaniyala, Suresh; Lewis, Ernie R; Wentzell, Jeremy J B; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M; Ault, Andrew P; Axson, Jessica L; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M Dale; Deane, Grant B; Mayol-Bracero, Olga L; Grassian, Vicki H; Bertram, Timothy H; Bertram, Allan K; Moffett, Bruce F; Franc, Gary D

    2016-05-24

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

  5. Sea spray aerosol as a unique source of ice nucleating particles

    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

  6. 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.

  7. Toxicological evaluation of realistic emission source aerosols (TERESA)--power plant studies: assessment of breathing pattern.

    PubMed

    Diaz, Edgar A; Lemos, Miriam; Coull, Brent; Long, Mark S; Rohr, Annette C; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Godleski, John J

    2011-08-01

    Our approach to study multi-pollutant aerosols isolates a single emissions source, evaluates the toxicity of primary and secondary particles derived from this source, and simulates chemical reactions that occur in the atmosphere after emission. Three U.S. coal-fired power plants utilizing different coals and with different emission controls were evaluated. Secondary organic aerosol (SOA) derived from α-pinene and/or ammonia was added in some experiments. Male Sprague-Dawley rats were exposed for 6 h to filtered air or different atmospheric mixtures. Scenarios studied at each plant included the following: primary particles (P); secondary (oxidized) particles (PO); oxidized particles + SOA (POS); and oxidized and neutralized particles + SOA (PONS); additional control scenarios were also studied. Continuous respiratory data were obtained during exposures using whole body plethysmography chambers. Of the 12 respiratory outcomes assessed, each had statistically significant changes at some plant and with some of the 4 scenarios. The most robust outcomes were found with exposure to the PO scenario (increased respiratory frequency with decreases in inspiratory and expiratory time); and the PONS scenario (decreased peak expiratory flow and expiratory flow at 50%). PONS findings were most strongly associated with ammonium, neutralized sulfate, and elemental carbon (EC) in univariate analyses, but only with EC in multivariate analyses. Control scenario O (oxidized without primary particles) had similar changes to PO. Adjusted R(2) analyses showed that scenario was a better predictor of respiratory responses than individual components, suggesting that the complex atmospheric mixture was responsible for respiratory effects.

  8. Elemental analysis of aerosols in Tehran's atmosphere using PIXE and identification of pollution sources.

    PubMed

    Esmaili, N; Khashman, S; Lamehi-Rachti, M; Agha Aligol, D; Shokouhi, F; Oliaiy, P; Farmahini Farahani, M

    2014-11-01

    In this study, the proton-induced X-ray emission (PIXE) technique has been applied to measure the elemental composition and concentrations of particulate matter of 220 samples of aerosols in Tehran's atmosphere within a 450-day time interval starting from March 2009 and ending in June 2010, covering all four seasons. PIXE analysis shows the samples are comprised of various elements including Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, and Pb. Also, to obtain more information about the sources of pollution and to identify the major sources of urban particulate matter, principal component analysis (PCA) was used. Furthermore, micro-PIXE was performed to study individual aerosols in some samples. Results revealed that the concentration of elements originating from vehicle emissions increases three times in winter; whereas the concentration of elements with soil origin remains constant. Based on wind rose maps, it is inferred that the high concentrations of the elements Al, Si, K, Ca, Ti, Mn, and Fe are associated with natural dust brought by winds into Tehran from the west.

  9. 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

  10. 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).

  11. 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.

  12. 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.

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

    DOE PAGES

    Woody, Matthew C.; Baker, Kirk R.; Hayes, Patrick L.; Jimenez, Jose L.; Koo, Bonyoung; Pye, Havala O. T.

    2016-03-29

    Community Multiscale Air Quality (CMAQ) model simulations utilizing the traditional organic aerosol (OA) treatment (CMAQ-AE6) and a volatility basis set (VBS) treatment for OA (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of OA in southern California. Traditionally, CMAQ treats primary organic aerosol (POA) as nonvolatile and uses a two-product framework to represent secondary organic aerosol (SOA) formation. CMAQ-VBS instead treats POA asmore » semivolatile and lumps OA using volatility bins spaced an order of magnitude apart. The CMAQ-VBS approach underpredicted organic carbon (OC) at IMPROVE and CSN sites to a greater degree than CMAQ-AE6 due to the semivolatile POA treatment. However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA, indicated that CMAQ-VBS better represented the diurnal profile and primary/secondary split of OA. CMAQ-VBS SOA underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate for SOA) concentration by a factor of 5.2, representing a considerable improvement to CMAQ-AE6 SOA predictions (factor of 24 lower than AMS). We use two new methods, one based on species ratios (SOA/ΔCO and SOA/Ox) and another on a simplified SOA parameterization, to apportion the SOA underprediction for CMAQ-VBS to slow photochemical oxidation (estimated as 1.5 ×  lower than observed at Pasadena using −log(NOx : NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2 ×  for Pasadena), and low emissions or excessive dispersion for the Pasadena site (estimated to be 1.6 to 2.3 ×  too low/excessive). The first and third factors are common to CMAQ-AE6, while the intrinsic SOA formation

  14. 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

  15. 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

  16. 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.

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

    PubMed Central

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

    2012-01-01

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

  18. 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

  19. Atmospheric Aerosol Source-Receptor Relationships: The Role of Coal-Fired Power Plants

    SciTech Connect

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2005-12-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of March 2005 through August 2005. Significant progress was made this project period on the source characterization, source apportionment, and deterministic modeling activities. This report highlights new data on road dust, vegetative detritus and motor vehicle emissions. For example, the results show significant differences in the composition in urban and rural road dust. A comparison of the organic of the fine particulate matter in the tunnel with the ambient provides clear evidence of the significant contribution of vehicle emissions to ambient PM. The source profiles developed from this work are being used by the source-receptor modeling activities. The report presents results on the spatial distribution of PMF-factors. The results can be grouped into three different categories: regional sources, local sources, or potentially both regional and local sources. Examples of the regional sources are the sulfate and selenium PMF-factors which most likely-represent coal fired power plants. Examples of local sources are the specialty steel and lead factors. There is reasonable correspondence between these apportionments and data from the EPA TRI and AIRS emission inventories. Detailed comparisons between PMCAMx predictions and measurements by the STN and IMPROVE measurements in the Eastern US are presented. Comparisons were made for the major aerosol components and PM{sub 2.5} mass in July 2001, October 2001, January 2002, and April 2002. The results are encouraging with average fraction biases for most species less than 0.25. The improvement of the model performance during the last two years was mainly due to the comparison of the model predictions with the continuous measurements in the Pittsburgh Supersite. Major improvements have included the descriptions: of ammonia emissions (CMU inventory), night time nitrate chemistry, EC emissions and their diurnal

  20. Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site

    NASA Astrophysics Data System (ADS)

    Takahama, S.; Schwartz, R. E.; Russell, L. M.; MacDonald, A. M.; Sharma, S.; Leaitch, W. R.

    2011-01-01

    Ambient particles collected on teflon filters at the Peak of Whistler Mountain, British Columbia (2182 m a.s.l.) during spring and summer 2009 were measured by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFG). The project mean and standard deviation of organic aerosol mass concentrations (OM) for all samples was 3.2±3.3 (μg m-3). The OM was dominated by regional forest sources, burning, and non-burning that occurred mostly during June-September. On average, organic hydroxyl, alkane, carboxylic acid, ketone, and amine, groups represented 31%±11%, 34%±9%, 23%±6%, 6%±7%, and 6%±3% of OM, respectively. Ketone groups were associated with the forest aerosols and represented up to 27% of the OM in these aerosols. Additional measurements of aerosol mass fragments, size, and number concentrations were used to separate fossil-fuel combustion and burning and non-burning forest sources of the measured organic aerosol. The OM concentrations observed at Whistler Peak during this campaign were higher than those measured during a shorter period in the spring of 2008 at a site in Whistler valley, over one km lower than the peak location. The 2009 campaign was largely influenced by the wildfire emissions that were absent during the 2008 campaign.

  1. Molecular marker analysis as a guide to the sources of fine organic aerosols

    SciTech Connect

    Rogge, W.F.; Cass, G.R.; Hildemann, L.M.; Mazurek, M.A.; Simoneit, B.R.T.

    1992-07-01

    The molecular composition of fine particulate (D{sub p} {ge} 2 {mu}m) organic aerosol emissions from the most important sources in the Los Angeles area has been determined. Likewise, ambient concentration patterns for more than 80 single organic compounds have been measured at four urban sites (West Los Angeles, Downtown Los Angeles, Pasadena, and Rubidoux) and at one remote offshore site (San Nicolas Island). It has been found that cholesterol serves as a marker compound for emissions from charbroilers and other meat cooking operations. Vehicular exhaust being emitted from diesel and gasoline powered engines can be traced in the Los Angeles atmosphere using fossil petroleum marker compounds such as steranes and pentacyclic triterpanes (e.g., hopanes). Biogenic fine particle emission sources such as plant fragments abraded from leaf surfaces by wind and weather can be traced in the urban atmosphere. Using distinct and specific source organic tracers or assemblages of organic compounds characteristic for the sources considered it is possible to estimate the influence of different source types at any urban site where atmospheric data are available.

  2. Molecular marker analysis as a guide to the sources of fine organic aerosols

    SciTech Connect

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

    1992-07-01

    The molecular composition of fine particulate (D[sub p] [ge] 2 [mu]m) organic aerosol emissions from the most important sources in the Los Angeles area has been determined. Likewise, ambient concentration patterns for more than 80 single organic compounds have been measured at four urban sites (West Los Angeles, Downtown Los Angeles, Pasadena, and Rubidoux) and at one remote offshore site (San Nicolas Island). It has been found that cholesterol serves as a marker compound for emissions from charbroilers and other meat cooking operations. Vehicular exhaust being emitted from diesel and gasoline powered engines can be traced in the Los Angeles atmosphere using fossil petroleum marker compounds such as steranes and pentacyclic triterpanes (e.g., hopanes). Biogenic fine particle emission sources such as plant fragments abraded from leaf surfaces by wind and weather can be traced in the urban atmosphere. Using distinct and specific source organic tracers or assemblages of organic compounds characteristic for the sources considered it is possible to estimate the influence of different source types at any urban site where atmospheric data are available.

  3. 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

  4. 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

  5. Chemically-Resolved Volatility Measurements of Organic Aerosol from Different Sources

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Docherty, K. S.; Mohr, C.; Ulbrich, I. M.; Ziemann, P. J.; Onasch, T. B.; Jimenez, J. L.

    2009-04-01

    A newly modified fast temperature-stepping thermodenuder (TD) was coupled to a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) for rapid quantification 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 a-pinene and gasoline vapor. Almost all atmospheric models represent POA as non-volatile, with no allowance for evaporation upon heating or dilution, or condensation upon cooling. Our results indicate that all OAs observed show semi-volatile behavior and that most POAs are 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 BBOA because of its 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 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 less volatile.

  6. 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.

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

    NASA Technical Reports Server (NTRS)

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

    2000-01-01

    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 degrees. 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.

  8. 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.

  9. Fatty acids on continental sulfate aerosol particles

    NASA Astrophysics Data System (ADS)

    Tervahattu, H.; Juhanoja, J.; Vaida, V.; Tuck, A. F.; Niemi, J. V.; Kupiainen, K.; Kulmala, M.; VehkamäKi, H.

    2005-03-01

    Surface analyses of atmospheric aerosols from different continental sources, such as forest fires and coal and straw burning, show that organic surfactants are found on such aerosols. The predominant organic species detected by time-of-flight secondary ion mass spectrometry on the sulfate aerosols are fatty acids of different carbon chain length up to the C32 acid. These observations are consistent with literature accounts of functional group analysis of bulk samples, but this is the first direct evidence of fatty acid films on the surface of sulfate aerosols. Surface analysis leads to the conclusion that fatty acid films on continental aerosols may be more common than has been previously suggested.

  10. 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

  11. Spatially and Temporally Refined Sources of Black Carbon Aerosols in the Arctic in spring

    NASA Astrophysics Data System (ADS)

    Qi, L.; Li, Q.; Mao, Y.; Chen, Y.; Randerson, J. T.; Wang, Q.; Hao, W. M.

    2014-12-01

    Black carbon (BC) aerosols play a substantial role in the rapid warming of the Arctic. We systematically evaluate the simulation of BC vertical profile (ARCTAS and ARCPAC flights), surface concentrations and concentrations in snow (Doherty et al., 2010) in the Arctic in spring using a global chemical transport model GEOS-Chem. We also provide highly spatially (2° lat ×2.5° lon) and temporally resolved source estimates of surface BC concentrations using GEOS-Chem adjoint. Results showed that the vertical profiles of BC agree with the aircraft observations from surface to 10 km within 50%. The monthly mean regional averaged BC concentrations in snow in Alaska, Arctic Ocean, Canada, Greenland and Russia agree with the observations within 40%, while the mean BC concentrations in snow in Svalbard and Norway agree with the observations within a factor of 3 because of inaccurate simulation of snow precipitation in GEOS5. We found Asian anthropogenic sources contributed 20-50% of BC concentrations through troposphere and in snow in the Arctic and are the major contributors in most regions. Adjoint analysis showed that BC concentrations of about 10 ng/m3 (30-100% of the total Asian contribution) observed at the surface stations are attributed to emissions emitted by Asian anthropogenic sources 30 days before the observation, and these background BC aerosols were transported to the station by circum-polar-vortex. Previous source estimates that repeated identified Europe as the major contributor of BC in the Arctic only trace back for 5 to 10 days and do not capture the background contribution from Asia. Russian biomass burning is important in mid-troposphere and accounts for 60% of total BC at 4-5 km. The relative contribution from different sources estimated by the adjoint of GEOS-Chem agrees with the forward estimate within 10%. Moreover, the adjoint analysis enables us to pinpoint the major sources to grid box level. Results showed that for surface observations

  12. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

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

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

    PubMed

    McNeill, V Faye

    2015-02-01

    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.

  15. Photochemistry at interfaces: a source of radicals impacting on aerosol formation and properties

    NASA Astrophysics Data System (ADS)

    George, C.; D'anna, B.; Monge, M.; Dupart, Y.

    2011-12-01

    Recent findings confirm the presence of light absorbing organic material (HULIS, biomass burning particles, PAHs) in atmospheric aerosols... but also at the air/ocean interface. The presence of such light absorbing material allows photosensitised processes to occur. The latter may be sources of radicals in the troposphere that may alter its oxidation capacity (as for instance through the formation of HONO) or change the pathways leading to particle formation and ageing. We will exemplify such processes by presenting new data on the generation of radicals from dust particles or at the air/sea interface leading to particle formation in presence of SO2. These are recent findings that are questioning our current understanding of tropospheric photochemistry.

  16. 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

  17. 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

  18. 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.

  19. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA)-power plant studies: assessment of cellular responses

    PubMed Central

    Godleski, John J.; Diaz, Edgar A.; Lemos, Miriam; Long, Mark; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Coull, Brent

    2013-01-01

    The Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA) project assessed primary and secondary particulate by simulating the chemical reactions that a plume from a source might undergo during atmospheric transport and added other atmospheric constituents that might interact with it. Three coal-fired power plants with different coal and different emission controls were used. Male Sprague-Dawley rats were exposed for 6 h to either filtered air or aged aerosol from the power plant. Four exposure scenarios were studied: primary particles (P); primary + secondary (oxidized) particles (PO); primary + secondary (oxidized) particles + SOA (POS); and primary + secondary (oxidized) particles neutralized + SOA (PONS). Exposure concentrations varied by scenario to a maximum concentration of 257.1 ± 10.0 µg/m3. Twenty-four hours after exposure, pulmonary cellular responses were assessed by bronchoalveolar lavage (BAL), complete blood count (CBC), and histopathology. Exposure to the PONS and POS scenarios produced significant increases in BAL total cells and macrophage numbers at two plants. The PONS and P scenarios were associated with significant increases in BAL neutrophils and the presence of occasional neutrophils and increased macrophages in the airways and alveoli of exposed animals. Univariate analyses and random forest analyses showed that increases in total cell count and macrophage cell count were significantly associated with neutralized sulfate and several correlated measurements. Increases in neutrophils in BAL were associated with zinc. There were no significant differences in CBC parameters or blood vessel wall thickness by histopathology. The association between neutrophils increases and zinc raises the possibility that metals play a role in this response. PMID:21466245

  20. Tracing impacts of local and regional emission sources on the aerosols over Central Himalayan region during GVAX

    NASA Astrophysics Data System (ADS)

    Sahai, Shivraj; Sagar, Ram; Pant, P.; Krishna Moorthy, K.; Venkata Phanikumar, Devulapalli; Dumka, Umesh Chandra; Pant, Vimlesh; Singh, Narendra; Kotamarthi, V. R.; Naja, Manish; Satheesh, S. K.

    2012-07-01

    -range transport impact, available satellite products over the Indo-Gangetic Plain (IGP) of relevance to biomass burning (Carbon monoxide, Aerosol Optical Depth, Fire products, etc) have been exploited to relate to the observed aerosol physical properties during GVAX. The findings are expected to reveal the linkages between local and regional emission sources (biomass burning in particular) and atmospheric perturbations.

  1. 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.

  2. 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

  3. 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. PMID:19204485

  4. 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.

  5. On the sources of bias in aerosol optical depth retrieval in the UV range

    NASA Astrophysics Data System (ADS)

    Arola, Antti; Koskela, Tapani

    2004-04-01

    In this paper we discuss and evaluate the systematic sources of bias in aerosol optical depth (AOD) values in the UV range due to (1) the entrance of diffuse light into the finite field of view, (2) diurnal atmospheric changes of ozone under urban conditions, (3) the influence of omitting the effect of NO2 absorption, and (4) stray light of a single monochromator. These error sources have been neglected before in Brewer AOD retrieval. However, if these bias estimates are added together, it appears likely that the main reason for the recent results, that is, an AOD wavelength dependency that is in contradiction to the Ångstrom law, lies in the omitted sources of systematic error in the AOD retrieval. For instance, the estimated negative bias in AOD difference between 306.3 and 320.1 nm is ˜0.0772, while between 310.1 and 320.1 nm it is ˜0.0346. If the true Ångstrom α was 1 and the AOD at 320.1 was 0.5, then the actual difference between 306.3 and 320.1 nm would be positive and equal to 0.022, while between 310.1 and 320.1 nm it would be 0.016. Therefore the neglected source of bias can mask this difference and result in a negative Ångstrom exponent (AE) value. In addition to these sources of bias, we also discuss other potential sources of uncertainty that have been previously neglected.

  6. Fossil and Nonfossil Sources of Organic and Elemental Carbon Aerosols in the Outflow from Northeast China.

    PubMed

    Zhang, Yan-Lin; Kawamura, Kimitaka; Agrios, Konstantinos; Lee, Meehye; Salazar, Gary; Szidat, Sönke

    2016-06-21

    Source quantification of carbonaceous aerosols in the Chinese outflow regions still remains uncertain despite their high mass concentrations. Here, we unambiguously quantified fossil and nonfossil contributions to elemental carbon (EC) and organic carbon (OC) of total suspended particles (TSP) from a regional receptor site in the outflow of Northeast China using radiocarbon measurement. OC and EC concentrations were lower in summer, representing mainly marine air, than in other seasons, when air masses mostly traveled over continental regions in Mongolia and northeast China. The annual-mean contribution from fossil-fuel combustion to EC was 76 ± 11% (0.1-1.3 μg m(-3)). The remaining 24 ± 11% (0.03-0.42 μg m(-3)) was attributed to biomass burning, with slightly higher contribution in the cold period (∼31%) compared to the warm period (∼21%) because of enhanced emissions from regional biomass combustion sources in China. OC was generally dominated by nonfossil sources, with an annual average of 66 ± 11% (0.5-2.8 μg m(-3)), approximately half of which was apportioned to primary biomass-burning sources (34 ± 6%). In winter, OC almost equally originated from primary OC (POC) emissions and secondary OC (SOC) formation from fossil fuel and biomass-burning sources. In contrast, summertime OC was dominated by primary biogenic emissions as well as secondary production from biogenic and biomass-burning sources, but fossil-derived SOC was the smallest contributor. Distinction of POC and SOC was performed using primary POC-to-EC emission ratios separated for fossil and nonfossil emissions. PMID:27203471

  7. 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...

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

    NASA Astrophysics Data System (ADS)

    Herich, Hanna; Hüglin, Christoph; Buchmann, Brigitte

    2010-05-01

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

  9. 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.

  10. Source and long-term behavior of transuranic aerosols in the WIPP environment.

    PubMed

    Thakur, P; Lemons, B G

    2016-10-01

    Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard. PMID:27394421

  11. 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.

  12. Source and long-term behavior of transuranic aerosols in the WIPP environment.

    PubMed

    Thakur, P; Lemons, B G

    2016-10-01

    Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

  13. Yearly trend of dicarboxylic acids in organic aerosols from south of Sweden and source attribution

    NASA Astrophysics Data System (ADS)

    Hyder, Murtaza; Genberg, Johan; Sandahl, Margareta; Swietlicki, Erik; Jönsson, Jan Åke

    2012-09-01

    Seven aliphatic dicarboxylic acids (C3-C9) along with phthalic acid, pinic acid and pinonic acid were determined in 35 aerosol (PM10) samples collected over the year at Vavihill sampling station in south of Sweden. Mixture of dichloromethane and methanol (ratio 1:3) was preferred over water for extraction of samples and extraction was assisted by ultrasonic agitation. Analytes were derivatized using N,O-bis(trimethylsilyl)trifluoroacetamide (BSTFA) containing 1% trimethylsilyl chloride and analyzed using gas chromatography/mass spectrometry. Among studied analytes, azelaic acid was found maximum with an average concentration of 6.0 ± 3.6 ng m-3 and minimum concentration was found for pimelic acid (1.06 ± 0.63 ng m-3). A correlation coefficients analysis was used for defining the possible sources of analytes. Higher dicarboxylic acids (C7-C9) showed a strong correlation with each other (correlation coefficients (r) range, 0.96-0.97). Pinic and pinonic acids showed an increase in concentration during summer. Lower carbon number dicarboxylic acids (C3-C6) and phthalic acid were found strongly correlated, but showed a poor correlation with higher carbon number dicarboxylic acids (C7-C9), suggesting a different source for them. Biomass burning, vehicle exhaust, photo-oxidation of volatile organic compounds (natural and anthropogenic emissions) were possible sources for dicarboxylic acids.

  14. Premonsoon aerosol optical properties from AERONET retrievals and its probable source fields in Eastern India urban environment (Kolkata): evaluating spatial variability and its comparison with MODIS retrievals.

    NASA Astrophysics Data System (ADS)

    B, P.; Verma, S.

    2015-12-01

    Aerosol characteristics were examined using Aerosol Robotic Network (AERONET) and MODIS retrievals (Moderate Resolution Imaging Spectroradiometer) during the period, February to June 2009 in Eastern India, Kolkata (KOL). AERONET retrievals results for the study period manifested an aerosol optical depth - AOD (Angstrom exponent - α) in the range 0.65 - 0.81 (0.66 - 0.97) with an intermittent influence of dust. A substantial dominance of finer (coarser) particles were found in February (April) and an equal dominance of both in June. Aerosol size distribution (ASD) revealed a high volume in fine mode during June and that in April for the coarse mode. A few areas of in and around KOL, Odisha, and Sikkim influenced AOD ascertained using the Potential source contribution function (PSCF). Cluster analysis revealed preferred pathway as continental during February and both continental and marine during March to June. Episodic days identified for dust occurrence was examined and was further corroborated by MODIS Rapid response images. Further, comparative results of seven collateral AERONET sites in India, revealed a high AOD (α) at KOL during February to May (March and April) with Fine mode - FM (Coarse mode - CM) AOD of KOL being high during March and April (February to April) than other locations. Single scattering albedo (SSA) at 0.67 μm at KOL was slightly lower during February and March, with being equivalent and or higher than other sites during April to June. Comparison of AERONET - MODIS AOD at 0.55 µm for KOL (entire study period) for the collateral days revealed underestimation of MODIS during February to April and overestimation during May and June than AERONET. AERONET - MODIS AOD comparison for seven locations, during low (February) and high (June) aerosol loading, showed good agreement for few stations and divulged discrepancy for other sites.

  15. Sources of carbonaceous aerosols over the United States and implications for natural visibility

    NASA Astrophysics Data System (ADS)

    Park, Rokjin J.; Jacob, Daniel J.; Chin, Mian; Martin, Randall V.

    2003-06-01

    We use a global three-dimensional model (GEOS-CHEM) to better quantify the sources of elemental carbon (EC) and organic carbon (OC) aerosols in the United States through simulation of year-round observations for 1998 at a network of 45 sites (Interagency Monitoring of Protected Visual Environments (IMPROVE)). Simulation with our best a priori understanding of sources, including global satellite data to constrain fire emissions, captures most of the variance in the observations (R2 = 0.84 for EC, 0.67 for OC) with a low bias of 15% for EC and 26% for OC. Multiple linear regression to fit the IMPROVE data yields best estimates of 1998 U.S. sources of 0.60 Tg year-1 EC and 0.52 Tg year-1 OC from fossil fuel; 0.07 Tg year-1 EC and 0.89 Tg year-1 OC from biofuel; 0.08 Tg year-1 EC and 0.60 Tg year-1 OC from wildfires; and 1.10 Tg year-1 OC from vegetation. We find that fires in Mexico and Canada contributed 40-70% of annual mean natural EC in the United States for 1998 and 20-30% of annual mean natural OC. Transpacific transport from Asian pollution sources amounted to less than 10% of the natural EC and less than 2% of the natural OC; in contrast to ozone, we find that intercontinental transport of anthropogenic carbonaceous aerosols does not enhance significantly the natural background. IMPROVE observations and model simulations for the summer of 1995 show that Canadian fire emissions can produce large events of elevated EC and OC in the southeastern United States. Our best estimates of mean natural concentrations of EC and OC in the United States, using a model simulation with climatological monthly mean fire emissions, are 2-3 times higher than the default values recommended by the U.S. Environmental Protection Agency for visibility calculations, except for OC in the eastern United States (16% lower).

  16. Emission source functions in heavy ion collisions

    NASA Astrophysics Data System (ADS)

    Shapoval, V. M.; Sinyukov, Yu. M.; Karpenko, Iu. A.

    2013-12-01

    Three-dimensional pion and kaon emission source functions are extracted from hydrokinetic model (HKM) simulations of central Au+Au collisions at the top Relativistic Heavy Ion Collider (RHIC) energy sNN=200 GeV. The model describes well the experimental data, previously obtained by the PHENIX and STAR collaborations using the imaging technique. In particular, the HKM reproduces the non-Gaussian heavy tails of the source function in the pair transverse momentum (out) and beam (long) directions, observed in the pion case and practically absent for kaons. The role of rescatterings and long-lived resonance decays in forming the mentioned long-range tails is investigated. The particle rescattering contribution to the out tail seems to be dominating. The model calculations also show substantial relative emission times between pions (with mean value 13 fm/c in the longitudinally comoving system), including those coming from resonance decays and rescatterings. A prediction is made for the source functions in Large Hadron Collider (LHC) Pb+Pb collisions at sNN=2.76 TeV, which are still not extracted from the measured correlation functions.

  17. 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

  18. 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.

  19. 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.

  20. 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

  1. 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

  2. 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

  3. 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

  4. 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).

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  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.

    2014-12-01

    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

  7. Acute lung function responses to ambient acid aerosol exposures in children

    SciTech Connect

    Raizenne, M.E.; Burnett, R.T.; Stern, B.; Franklin, C.A.; Spengler, J.D.

    1989-02-01

    We examined the relationship between lung function changes and ambient acid aerosol episodes in children attending a residential summer camp. Young females (112) performed daily spirometry, and 96 were assessed on one occasion for airway hyperresponsiveness using a methacholine bronchoprovocation test. Air quality measurements were performed on site and four distinct acid aerosol episodes were observed during the 41-day study. The maximum values observed during the 41-day study were: O/sub 3/ at 143 ppb; H/sub 2/SO/sub 4/ at 47.7 micrograms/m/sup 3/; and (H+) at 550 nmole/m/sup 3/. Maximum decrements of 3.5 and 7% for FEV1 and PEF, respectively, were observed to be associated with the air pollution episodes. There was some evidence of a differential lung function response to the episodes where children with a positive response to a methacholine challenge had larger decrements compared to their nonresponsive counterparts.

  8. Acute lung function responses to ambient acid aerosol exposures in children.

    PubMed

    Raizenne, M E; Burnett, R T; Stern, B; Franklin, C A; Spengler, J D

    1989-02-01

    We examined the relationship between lung function changes and ambient acid aerosol episodes in children attending a residential summer camp. Young females (112) performed daily spirometry, and 96 were assessed on one occasion for airway hyperresponsiveness using a methacholine bronchoprovocation test. Air quality measurements were performed on site and four distinct acid aerosol episodes were observed during the 41-day study. The maximum values observed during the 41-day study were: O3 at 143 ppb; H2SO4 at 47.7 micrograms/m3; and [H+] at 550 nmole/m3. Maximum decrements of 3.5 and 7% for FEV1 and PEF, respectively, were observed to be associated with the air pollution episodes. There was some evidence of a differential lung function response to the episodes where children with a positive response to a methacholine challenge had larger decrements compared to their nonresponsive counterparts.

  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. 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.

  12. 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

  13. Source attribution of aerosol size distributions and model evaluation using Whistler Mountain measurements and GEOS-Chem-TOMAS simulations

    NASA Astrophysics Data System (ADS)

    D'Andrea, S. D.; Ng, J. Y.; Kodros, J. K.; Atwood, S. A.; Wheeler, M. J.; Macdonald, A. M.; Leaitch, W. R.; Pierce, J. R.

    2015-09-01

    Remote and free tropospheric aerosols represent a large fraction of the climatic influence of aerosols; however, aerosol in these regions is less characterized than those polluted boundary layers. We evaluate aerosol size distributions predicted by the GEOS-Chem-TOMAS global chemical transport model with online aerosol microphysics using measurements from the peak of Whistler Mountain, BC, Canada (2182 m a.s.l.). We evaluate the model for predictions of aerosol number, size and composition during periods of free tropospheric (FT) and boundary-layer (BL) influence at "coarse" 4° × 5° and "nested" 0.5° × 0.667° resolutions by developing simple FT/BL filtering techniques. We find that using temperature as a proxy for upslope flow (BL influence) improved the model measurement comparisons. The best threshold temperature was around 2 °C for the coarse simulations and around 6 °C for the nested simulations, with temperatures warmer than the threshold indicating boundary-layer air. Additionally, the site was increasingly likely to be in-cloud when the measured RH was above 90 %, so we do not compare the modeled and measured size distributions during these periods. With the inclusion of these temperature and RH filtering techniques, the model-measurement comparisons improved significantly. The slope of the regression for N80 (the total number of particles with particle diameter, Dp > 80 nm) in the nested simulations increased from 0.09 to 0.65, R2 increased from 0.04 to 0.46, and log-mean bias improved from 0.95 to 0.07. We also perform simulations at the nested resolution without Asian anthropogenic (AA) emissions and without biomass-burning (BB) emissions to quantify the contribution of these sources to aerosols at Whistler Peak (through comparison with simulations with these emissions on). The long-range transport of AA aerosol was found to be significant throughout all particle number concentrations, and increased the number of particles larger than 80 nm (N80

  14. Source attribution of aerosol size distributions and model evaluation using Whistler Mountain measurements and GEOS-Chem-TOMAS simulations

    NASA Astrophysics Data System (ADS)

    D'Andrea, S. D.; Ng, J. Y.; Kodros, J. K.; Atwood, S. A.; Wheeler, M. J.; Macdonald, A. M.; Leaitch, W. R.; Pierce, J. R.

    2016-01-01

    Remote and free-tropospheric aerosols represent a large fraction of the climatic influence of aerosols; however, aerosol in these regions is less characterized than those polluted boundary layers. We evaluate aerosol size distributions predicted by the GEOS-Chem-TOMAS global chemical transport model with online aerosol microphysics using measurements from the peak of Whistler Mountain, British Columbia, Canada (2182 m a.s.l., hereafter referred to as Whistler Peak). We evaluate the model for predictions of aerosol number, size, and composition during periods of free-tropospheric (FT) and boundary-layer (BL) influence at "coarse" 4° × 5° and "nested" 0.5° × 0.667° resolutions by developing simple FT/BL filtering techniques. We find that using temperature as a proxy for upslope flow (BL influence) improved the model-measurement comparisons. The best threshold temperature was around 2 °C for the coarse simulations and around 6 °C for the nested simulations, with temperatures warmer than the threshold indicating boundary-layer air. Additionally, the site was increasingly likely to be in cloud when the measured relative humidity (RH) was above 90 %, so we do not compare the modeled and measured size distributions during these periods. With the inclusion of these temperature and RH filtering techniques, the model-measurement comparisons improved significantly. The slope of the regression for N80 (the total number of particles with particle diameter, Dp, > 80 nm) in the nested simulations increased from 0.09 to 0.65, R2 increased from 0.04 to 0.46, and log-mean bias improved from 0.95 to 0.07. We also perform simulations at the nested resolution without Asian anthropogenic emissions and without biomass-burning emissions to quantify the contribution of these sources to aerosols at Whistler Peak (through comparison with simulations with these emissions on). The long-range transport of Asian anthropogenic aerosol was found to be significant throughout all particle

  15. [Pollution Characteristics and Sources of Carbonaceous Aerosol in PM2.5 During Winter in Guanzhong Area].

    PubMed

    Tian, Peng-shan; Cao, Jun-ji; Han, Yong-ming; Zhang, Ning-ning; Zhang, Rong; Liu, Sui-xin

    2016-02-15

    To study the characteristics and sources of carbonaceous aerosol in PM2.5 during winter in Guanzhong area, PM2.5 samples were collected from December 2012 to February 2013 in Xi'an, Baoji, Weinan and Qinling, and then organic carbon (OC) and elemental carbon (EC) were analyzed following the thermal/optical reflection protocol. The average concentrations of OC in the four sites were 47.8, 45.8, 31.2 and 37.0 microg x m(-3), respectively, while EC concentrations were 8.5, 6.7, 7.6 and 5.7 microg x m(-3), respectively. Total carbonaceous aerosol (TCA) accounted for 36.4%, 46.2%, 36.9% and 33.4% of PM2.5, respectively. OC was strongly correlated with EC in Xi'an (R2 = 0.93) and Qinling (R2 = 0.91), while weakly correlated in Baoji (R2 = 0.58) and Weinan (R2 = 0.62), which indicated that OC and EC had more similar sources or higher mixing degree in the former two sites. All OC/EC ratios exceeded 2.0, which indicated the formation of secondary organic carbon (SOC). In Xi'an, Baoji, Weinan and Qinling, SOC accounted for 21.6%, 40.3%, 23.2% and 27.8% of OC, respectively. Positive matrix factorization (PMF) was used to analyze the sources of carbonaceous aerosol and four sources were obtained. Coal burning was the major source, contributing 45.3%-47.9% in Guanzhong area. Gasoline vehicle and biomass burning were the minor sources, contributing 26.1%-33.1% and 14.3%-20.1% respectively. In addition, diesel vehicle also had some contribution to carbonaceous aerosol.

  16. A new source of Southern Ocean and Antarctic aerosol from tropospheric polar cell chemistry of sea ice emissions

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Robinson, A. D.; Harris, N. R. P.; Keywood, M.; Ward, J.; Galbally, I.; Molloy, S.; Thomas, A.; Wilson, S. R.

    2014-12-01

    The Antarctic region is a pristine environment with minimal anthropogenic influence. Aerosol measurements in this environment allow the study of natural aerosols and polar atmospheric dynamics. Measurements in this region have been limited primarily to continental and coastal locations where permanent stations exist, with a handful of measurements in the sea ice region. The MAPS campaign (Measurements of Aerosols and Precursors during SIPEXII) occurred as part of SIPEX II (Sea Ice Physics and Ecosystems eXperiment II) voyage in Spring, 2012, and produced the first Antarctic pack-ice focused aerosol dataset aimed at characterizing new particle formation processes off the coast of East Antarctica (~65°S, 120°E). Numerous atmospheric parameters and species were measured, including the number of aerosol particles in the 3-10 nm size range, the range associated with nucleating particle formation. A latitudinal transect through the sea ice identified the Polar Front from sudden changes in nucleating particle concentrations, averaging 51cm-3 north of the front in the Ferrel cell, and 766 cm-3 south of the front, in the Polar cell region. The Polar Front location was also confirmed by meteorological and back-trajectory data. Background aerosol populations in the Polar cell fluctuated significantly but displayed no growth indicators, suggesting transport. Back-trajectories revealed that air parcels often descended from the free-troposphere within the previous 24-48 hrs. It is proposed that particle formation occurs in the free troposphere from precursors uplifted at the polar front region which, being a sea-ice/ocean region, is a significant precursor source. After tropospheric formation, populations descending at the poles are transported northward and reach the sea ice surface, missing continental stations. Current measurements of Antarctic aerosol suggest very low loading which may be explained by these circulation patterns and may underestimate total regional loading

  17. Sources of aerosol as determined from elemental composition and size distributions in Beijing

    NASA Astrophysics Data System (ADS)

    Zhang, Wenjie; Zhuang, Guoshun; Guo, Jinghua; Xu, Dongqun; Wang, Wei; Baumgardner, Darrel; Wu, Zhiyuan; Yang, Wen

    2010-02-01

    consistent to other researches. Most of the elements in coarse fractions showed higher concentrations in the nighttime than those in the daytime. In addition, most peaks of accumulation modes showed higher in daytime than those in nighttime, and/or showed tendency to increase to larger sizes. Taking into account the properties of aerosols coming from different sources in the winter, the direction from which air masses are transported affects the characteristics of the particles, i.e. cleaner air from the northwest and more polluted air from the south. There were also similar variations in potassium and manganese, indicating waste incineration as a common source.

  18. Long-term aerosol measurements in Gran Canaria, Canary Islands: Particle concentration, sources and elemental composition

    NASA Astrophysics Data System (ADS)

    Gelado-Caballero, MaríA. D.; López-GarcíA, Patricia; Prieto, Sandra; Patey, Matthew D.; Collado, Cayetano; HéRnáNdez-Brito, José J.

    2012-02-01

    There are very few sets of long-term measurements of aerosol concentrations over the North Atlantic Ocean, yet such data is invaluable in quantifying atmospheric dust inputs to this ocean region. We present an 8-year record of total suspended particles (TSP) collected at three stations on Gran Canaria Island, Spain (Taliarte at sea level, Tafira 269 m above sea level (a.s.l.) and Pico de la Gorra 1930 m a.s.l.). Using wet and dry deposition measurements, the mean dust flux was calculated at 42.3 mg m-2 d-1. Air mass back trajectories (HYSPLIT, NOAA) suggested that the Sahara desert is the major source of African dust (dominant during 32-50% of days), while the Sahel desert was the major source only 2-10% of the time (maximum in summer). Elemental composition ratios of African samples indicate that, despite the homogeneity of the dust in collected samples, some signatures of the bedrocks can still be detected. Differences were found for the Sahel, Central Sahara and North of Sahara regions in Ti/Al, Mg/Al and Ca/Al ratios, respectively. Elements often associated with pollution (Pb, Cd, Ni, Zn) appeared to share a common origin, while Cu may have a predominantly local source, as suggested by a decrease in the enrichment factor (EF) of Cu during dust events. The inter-annual variability of dust concentrations is investigated in this work. During winter, African dust concentration measurements at the Pico de la Gorra station were found to correlate with the North Atlantic Oscillation (NAO) index.

  19. Quantitative evaluation of emission control of primary and secondary organic aerosol sources during Beijing 2008 Olympics

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

    To explore the primary and secondary sources of fine organic particles after the aggressive implementation of air pollution controls during 2008 Beijing Olympic Games, 12-h PM2.5 concentrations were measured at one urban and one upwind rural site during the CAREBeijing-2008 (Campaigns of Air quality REsearch in Beijing and surrounding region) summer field campaign. The PM2.5 concentrations were 72.5±43.6μg m3 and 64.3±36.2μg m-3 at the urban site and rural site, respectively, which were the lowest in recent years due to the implementation of drastic control measures and favorable weather conditions. Five primary and four secondary fine organic particle sources were quantified using a CMB (chemical mass balance) model and tracer-yield method. Compared with previous studies in Beijing, the contribution of vehicle emission increased, with diesel engines contributing 16.2±5.9% and 14.5±4.1% to the total organic carbon (OC) concentrations and gasoline vehicles accounting for 10.3±8.7% and 7.9±6.2% of the OC concentrations at two sites. Due to the implementation of emission control measures, the OC concentrations from important primary sources have been reduced, and secondary formation has become an important contributor to fine organic aerosols. Compared with the non-controlled period, primary vehicle contributions were reduced by 30% and 24% in the urban and regional area, and reductions in the contribution from coal combustion were 57% and 7%, respectively. These results demonstrate the emission control measures significantly alleviated the primary organic particle pollution in and around Beijing. However, the control effectiveness of secondary organic particles was not significant.

  20. 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

  1. 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

  2. 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.

  3. 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

  4. Carbon dioxide accumulation during small animal, whole body plethysmography: effects on ventilation, indices of airway function, and aerosol deposition.

    PubMed

    Kimmel, Edgar C; Whitehead, Gregory S; Reboulet, James E; Carpenter, Robert L

    2002-01-01

    Barometric (whole body) plethysmography is used to examine changes in ventilation and breathing pattern in unrestrained animals during exposure to therapeutic or toxic aerosols. Whole body plethysmographs (WBP) may be operated with a bias flow in order to maintain an adequate supply of oxygen and remove expired CO(2). However, some aerosol generation and delivery methods may require operation of the WBP without bias flow, which would artificially deplete aerosol concentration. Under these conditions, expired CO(2) accumulates in the plethysmograph and stimulates ventilation, increasing total aerosol deposition, shifting regional deposition, and significantly altering some airway function indices. We characterized these effects in guinea pigs using a commercially available 4.5-L WBP, with and without a 1 L/min bias flow. CO(2)-induced changes in breathing frequency (f), tidal volume (Vt), minute ventilation (Ve), and indices of airway function -- including enhanced pause (penh), flow derived parameter (FDP), and respiratory duty cycle -- were measured. Without bias flow, CO(2) in the plethysmograph increased steadily to 5.4% after 30 min compared to a steady state 0.9% with bias flow. This resulted in a moderate suppression of f, and significant increases in Vt and Ve by factors of 1.5 and 1.4, respectively. Changes in regional deposition were stimulated for 300 mg/m(3) polydisperse aerosols with mass median aerodynamic diameters of 0.3, 1, 3, or 7 microm and geometric standard deviations of 1.7. Percent increase in aerosol deposition from CO(2) inhalation ranged from 24% to 90%, by mass, depending on aerosol size distribution and respiratory tract region. In addition, fractional deposition shifted toward the pulmonary region. Empirical indices of airway constriction, penh and FDP, also were increased significantly to 1.7 and 1.3 times their respective baseline values. The study quantifies the effect of inadvertent coexposure to CO(2) on ventilation, aerosol

  5. Development of an aerosol dispersion test to detect early changes in lung function

    SciTech Connect

    McCawley, M.; Lippmann, M.

    1988-07-01

    The dispersion of a 0.5 micron aerosol bolus during tidal breathing differs significantly (p less than 0.0001) between a group of smokers (with approximately 20 pack-years average exposure) and a comparable group of nonsmokers. Their mean differences in standard respiratory function indexes from spirometry (forced vital capacity (FVC), forced expiratory volume in one second (FEV1), mean forced expiratory flow during the middle half of the FVC (FEF25-75)) were smaller and not statistically significant. The test is simple to perform and may be done as quickly as spirometry but without using a forced exhalation. Comparison of the coefficients of variation for the dispersion test and FEV1 indicate that the aerosol dispersion test may be useful in epidemiologic investigations either by reducing the required population size or increasing the level of confidence.

  6. Photodegradation of Secondary Organic Aerosol Particles as a Source of Small, Oxygenated Volatile Organic Compounds.

    PubMed

    Malecha, Kurtis T; Nizkorodov, Sergey A

    2016-09-20

    We investigated the photodegradation of secondary organic aerosol (SOA) particles by near-UV radiation and photoproduction of oxygenated volatile organic compounds (OVOCs) from various types of SOA. We used a smog chamber to generate SOA from α-pinene, guaiacol, isoprene, tetradecane, and 1,3,5-trimethylbenzene under high-NOx, low-NOx, or ozone oxidation conditions. The SOA particles were collected on a substrate, and the resulting material was exposed to several mW of near-UV radiation (λ ∼ 300 nm) from a light-emitting diode. Various OVOCs, including acetic acid, formic acid, acetaldehyde, and acetone were observed during photodegradation, and their SOA-mass-normalized fluxes were estimated with a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). All the SOA, with the exception of guaiacol SOA, emitted OVOCs upon irradiation. Based on the measured OVOC emission rates, we estimate that SOA particles would lose at least ∼1% of their mass over a 24 h period during summertime conditions in Los Angeles, California. This condensed-phase photochemical process may produce a few Tg/year of gaseous formic acid, the amount comparable to its primary sources. The condensed-phase SOA photodegradation processes could therefore measurably affect the budgets of both particulate and gaseous atmospheric organic compounds on a global scale. PMID:27547987

  7. Photodegradation of Secondary Organic Aerosol Particles as a Source of Small, Oxygenated Volatile Organic Compounds.

    PubMed

    Malecha, Kurtis T; Nizkorodov, Sergey A

    2016-09-20

    We investigated the photodegradation of secondary organic aerosol (SOA) particles by near-UV radiation and photoproduction of oxygenated volatile organic compounds (OVOCs) from various types of SOA. We used a smog chamber to generate SOA from α-pinene, guaiacol, isoprene, tetradecane, and 1,3,5-trimethylbenzene under high-NOx, low-NOx, or ozone oxidation conditions. The SOA particles were collected on a substrate, and the resulting material was exposed to several mW of near-UV radiation (λ ∼ 300 nm) from a light-emitting diode. Various OVOCs, including acetic acid, formic acid, acetaldehyde, and acetone were observed during photodegradation, and their SOA-mass-normalized fluxes were estimated with a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). All the SOA, with the exception of guaiacol SOA, emitted OVOCs upon irradiation. Based on the measured OVOC emission rates, we estimate that SOA particles would lose at least ∼1% of their mass over a 24 h period during summertime conditions in Los Angeles, California. This condensed-phase photochemical process may produce a few Tg/year of gaseous formic acid, the amount comparable to its primary sources. The condensed-phase SOA photodegradation processes could therefore measurably affect the budgets of both particulate and gaseous atmospheric organic compounds on a global scale.

  8. The toxicological evaluation of realistic emissions of source aerosols study: statistical methods.

    PubMed

    Coull, Brent A; Wellenius, Gregory A; Gonzalez-Flecha, Beatriz; Diaz, Edgar; Koutrakis, Petros; Godleski, John J

    2011-08-01

    The Toxicological Evaluation of Realistic Emissions of Source Aerosols (TERESA) study involved withdrawal, aging, and atmospheric transformation of emissions of three coal-fired power plants. Toxicological evaluations were carried out in rats exposed to different emission scenarios with extensive exposure characterization. Data generated had multiple levels of resolution: exposure, scenario, and constituent chemical composition. Here, we outline a multilayered approach to analyze the associations between exposure and health effects beginning with standard ANOVA models that treat exposure as a categorical variable. The model assessed differences in exposure effects across scenarios (by plant). To assess unadjusted associations between pollutant concentrations and health, univariate analyses were conducted using the difference between the response means under exposed and control conditions and a single constituent concentration as the predictor. Then, a novel multivariate analysis of exposure composition and health was used based on Random Forests(™), a recent extension of classification and regression trees that were applied to the outcome differences. For each exposure constituent, this approach yielded a nonparametric measure of the importance of that constituent in predicting differences in response on a given day, controlling for the other measured constituent concentrations in the model. Finally, an R(2) analysis compared the relative importance of exposure scenario, plant, and constituent concentrations on each outcome. Peak expiratory flow (PEF) is used to demonstrate how the multiple levels of the analysis complement each other to assess constituents most strongly associated with health effects.

  9. ATMOSPHERIC AEROSOL SOURCE-RECEPTOR RELATIONSHIPS: THE ROLE OF COAL-FIRED POWER PLANTS

    SciTech Connect

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2005-04-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of September 2004 through February 2005. Significant progress was made this project period on the analysis of ambient data, source apportionment, and deterministic modeling activities. The major experimental achievement this project period was the characterization of the mercury and fine particle emissions from two modern, large, commercial pulverized coal boilers. This testing completes the field work component of the Source Characterization Activity. This report highlights results from mercury emission measurements made using a dilution sampler. The measurements clearly indicate that mercury is being transformed from an oxidized to an elemental state within the dilution. However, wall effects are significant making it difficult to determine whether or not these changes occur in the gas phase or due to some interaction with the sampler walls. This report also presents results from an analysis that uses spherical aluminum silicate (SAS) particles as a marker for primary PM{sub 2.5} emitted from coal combustion. Primary emissions from coal combustion contribute only a small fraction of the PM{sub 2.5} mass (less than 1.5% in the summer and less than 3% in the winter) at the Pittsburgh site. Ambient SAS concentrations also appear to be reasonably spatially homogeneous. Finally, SAS emission factors measured at pilot-scale are consistent with measurements made at full-scale. This report also presents results from applying the Unmix and PMF models to estimate the contribution of different sources to the PM{sub 2.5} mass concentrations in Pittsburgh using aerosol composition information. Comparison of the two models shows similar source composition and contribution for five factors: crustal material, nitrate, an Fe, Mn, and Zn factor, specialty steel production, and a cadmium factor. PMF found several additional factors. Comparison between source contributions

  10. 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

  11. Using multidimensional gas chromatography to group secondary organic aerosol species by functionality

    NASA Astrophysics Data System (ADS)

    Flores, Rosa M.; Doskey, Paul V.

    2014-10-01

    A carbon number-functionality grid (CNFG) for a complex mixture of secondary organic aerosol (SOA) precursors and oxidation products was developed from the theoretical retention index diagram of a multidimensional gas chromatographic (GC × 2GC) analysis of a mixture of SOA precursors and derivatized oxidation products. In the GC × 2GC analysis, comprehensive separation of the complex mixture was achieved by diverting the modulated effluent from a polar primary column into 2 polar secondary columns. Column stationary phases spanned the widest range of selectivity of commercially available GC analytic columns. In general, separation of the species by the polar primary column was by the number of carbon atoms in the molecule (when the homologous series of reference compounds was selected to have molecular volumes and functionalities similar to the target analytes) and the polar secondary columns provided additional separation according to functionality. An algebraic transformation of the Abraham solvation parameter model was used to estimate linear retention indices of solutes relative to elution of a homologous series of methyl diesters on the primary and secondary columns to develop the theoretical GC × 2GC retention diagram. Retention indices of many of the oxidation products of SOA precursors were estimated for derivatized forms of the solutes. The GC stationary phases selected for the primary column [(50%-Trifluoropropyl)-methylpolysiloxane] and secondary columns (90% Cyanopropyl Polysilphenylene-siloxane and Polyethylene Glycol in a Sol-Gel matrix) provided a theoretical separation of 33 SOA precursors and 98 derivatized oxidation products into 35 groups by molecular volume and functionality. Comprehensive analysis of extracts of vapor and aerosol samples containing semivolatile SOA precursors and oxidation products, respectively, is best accomplished by (1) separating the complex mixture of the vapor and underivatized aerosol extracts with a (50

  12. Survey of aerosol optical properties measured as a function of wavelength with multiple photoacoustic instruments in Sacramento during the CARES campaign

    NASA Astrophysics Data System (ADS)

    Dubey, M. K.; Flowers, B. A.; Arnott, W. P.; Mazzoleni, C.; Lack, D. A.; Gyawali, M. S.; Gorkowski, K.; Fast, J. D.; Zaveri, R. A.; Hubbe, J.; Aiken, A. C.

    2010-12-01

    The goal of the Carbonaceous Aerosols and Radiative Effects Study (CARES) in Central California was to develop scientific knowledge on the life cycle of black carbon and organic aerosols in a mixed urban and forested region. The focus was to improve mechanisms by which carbonaceous aerosols are produced and modified and how they alter their optical properties. To achieve this we deployed ten photoacoustic instruments at ground sites (T0 in Sacramento, and T1 in Cool) and on aircraft (DOE-G1 and NOAA-P3) to measure aerosol absorption and scattering as a function of wavelength. Optical properties were measured at 1064, 871, 780, 532, 405, 375 and 355 nm. Analysis of optical properties over this wide spectral range is being used to attribute the contributions of black, brown and organic carbon as it mixes with other aerosol constituents. Diurnal variations of optical properties measured at T0 reflect urban sources while those at T1 are influenced by local biogenic emissions mixed with transported urban emissions. We present optical evidence of particle nucleation and secondary organic formation at the ground sites. Airborne observations on the G-1 are used to gain a regional perspective and also test for self-consistency and/or performances of instruments. We focus on the inter-comparison flight on 18th June, 2010 where photoacoustic data from the NOAA-P3 (Calnex) and G-1 instruments are compared. Our data are combined with measurements of tracers (e.g. CO 2 and CO) and output from WRF-models to gain a predictive understanding of radiative forcing by carbonaceous aerosols in a mixed urban and forested regime.

  13. 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.

  14. 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.

  15. 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.

  16. 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).

  17. Investigation of sources of atmospheric aerosol at a hot spot area in Dhaka, Bangladesh.

    PubMed

    Begum, Bilkis A; Biswas, Swapan K; Kim, Eugene; Hopke, Philip K; Khaliquzzaman, Mohammed

    2005-02-01

    Samples of fine and coarse fractions of airborne particulate matter were collected at the Farm Gate area in Dhaka from July 2001 to March 2002. Dhaka is a hot spot area with very high pollutant concentrations because of the proximity of major roadways. The samples were collected using a "Gent" stacked filter unit in two fractions of 0- to 2.2-microm and 2.2- to 10-microm sizes. The samples were analyzed for elemental concentrations by particle-induced X-ray excitation (PIXE) and for black carbon by reflectivity methods, respectively. The data were analyzed by positive matrix factorization (PMF) to identify the possible sources of atmospheric aerosols in this area. Six sources were found for both the coarse and fine PM fractions. The data sets were also analyzed by an expanded model to explore additional sources. Seven and six factors were obtained for coarse and fine PM fractions, respectively, in these analyses. The identified sources are motor vehicle, soil dust, emissions from construction activities, sea salt, biomass burning/brick kiln, resuspended/fugitive Pb, and two-stroke engines. From the expanded modeling, approximately 50% of the total PM2.2 mass can be attributed to motor vehicles, including two-stroke engine vehicle in this hot spot in Dhaka, whereas the PMF modeling indicates that 45% of the total PM2.2 mass is from motor vehicles. The PMF2 and expanded models could resolve approximately 4% and 3% of the total PM2.2 mass as resuspended/fugitive Pb, respectively. Although, Pb has been eliminated from gasoline in Bangladesh since July 1999, there still may be substantial amounts of accumulated lead in the dust near roadways as well as fugitive Pb emissions from battery reclaimation and other industries. Soil dust is the largest component of the coarse particle fraction (PM2.2-10) accounting for approximately 71% of the total PM2.2-10 mass in the expanded model, whereas from the PMF modeling, the dust (undifferentiated) contribution is approximately 49%.

  18. 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.

  19. The effect of local sources on particle size and chemical composition and their role in aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Portin, H.; Leskinen, A.; Hao, L.; Kortelainen, A.; Miettinen, P.; Jaatinen, A.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.; Komppula, M.

    2013-12-01

    The effects of local pollutant sources and particle chemical composition on aerosol-cloud interactions were investigated by measuring cloud interstitial and total aerosol size distributions, particle chemical composition and hygroscopic growth factors and cloud droplet size distributions on an observation tower, with a special focus on comparing clean air masses with those affected by local sources. The polluted air masses contained more particles than the clean air masses in all size classes, excluding the accumulation mode. This was caused by cloud processing, which was also observed for the polluted air but to a lesser extent. Some, mostly minor, differences in the particle chemical composition between the air masses were observed. The average size and number concentration of activating particles were quite similar for both air masses, producing average droplet populations with only minor distinctions. As a case study, a long cloud event was analyzed in detail regarding emissions from local sources, including a paper mill and a heating plant. Clear differences in the total and accumulation mode particle concentrations, particle hygroscopicity and chemical composition during the cloud event were observed. Particularly, larger particles, higher hygroscopicities and elevated amounts of inorganic constituents, especially SO4, were linked with the pollutant plumes. In the air masses affected by traffic and domestic wood combustion, a bimodal particle hygroscopicity distribution was observed, indicating externally mixed aerosol. The variable conditions during the event had a clear impact on cloud droplet formation.

  20. Aerosol-derived lung morphometry: comparisons with a lung model and lung function indexes.

    PubMed

    Blanchard, J D; Heyder, J; O'Donnell, C R; Brain, J D

    1991-10-01

    This study evaluated the ability of aerosol-derived lung morphometry to noninvasively probe airway and acinar dimensions. Effective air-space diameters (EAD) were calculated from the time-dependent gravitational losses of 1-microns particles from inhaled aerosol boluses during breath holding. In 17 males [33 +/- 7 (SD) yr] the relationship between EAD and volumetric penetration of the bolus into the lungs (Vp) could be expressed by the linear power-law function, log (EAD) alpha beta log (Vp). Our EAD values were consistent with Weibel's symmetric lung model A for small airways and more distal air spaces. As lung volume increased from 57 to 87% of total lung capacity (TLC), EAD at Vp of 160 and 550 cm3 increased 70 and 41%, respectively. At 57% TLC, log (EAD) at 160 cm3 was significantly correlated with airway resistance (r = -0.57, P less than 0.0204) but not with forced expired flow between 25 and 75% of vital capacity. Log (EAD) at 400 cm3 was correlated with deposition of 1-micron particles (r = -0.73, P less than 0.0009). We conclude that aerosol-derived lung morphometry is a responsive noninvasive probe of peripheral air-space diameters. PMID:1757343

  1. Aerosol assisted chemical vapour deposition of Cu-ZnO composite from single source precursors.

    PubMed

    Shahid, Muhammad; Mazhar, Muhammad; Hamid, Mazhar; O'Brien, Paul; Malik, Mohammad A; Helliwell, Madeleine; Raftery, James

    2009-07-28

    Two heterobimetallic precursors [Zn(TFA)3(micro-OH)Cu3(dmae)3Cl].THF (1) and [Zn(TFA)4Cu3(dmae)4] (2) [dmae=N,N-dimethylaminoethanolate and TFA=trifluoroacetate], have been synthesized and characterized by their melting points, elemental analysis, FT-IR spectroscopy, mass spectrometry, TGA and single crystal X-ray diffraction methods. Both complexes were used to deposit thin films of Cu-ZnO composite on glass substrates by aerosol assisted chemical vapor deposition (AACVD) method. The films were characterized by "scotch tape" test for adhesion, thickness measurement as a function of temperature, EDX for composition, SEM for surface morphology and XRD for crystalline phases. Thin film deposition studies at 250, 325, 400, 475 degrees C indicated the increase in thickness with temperature reaching a maximum at 400 degrees C and then decreasing. EDX and PXRD results showed the uniform distribution of cubic metallic copper and hexagonal zinc oxide phases which make them useful for nanocatalysis on structured surfaces. PMID:19587992

  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. Air ion measurements as a source of information about atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Hõrrak, Urmas; Mirme, Aadu; Salm, Jaan; Tamm, Eduard; Tammet, Hannes

    The mobility spectra of air ions recorded in the course of routine atmospheric electric measurements contain information about atmospheric aerosols. The mobility spectrum of air ions is correlated with the size spectrum of aerosol particles. Two procedures of conversion (and conversion errors) are considered in this paper assuming the steady state of charge distribution. The first procedure uses the fraction model of the aerosol particle size distribution and algebraic solution of the conversion problem. The second procedure uses the parametric KL model of the particle size distribution and the least square fitting of the mobility measurements. The procedures were tested using simultaneous side-by-side measurements of air ion mobilities and aerosol particle size distributions at a rural site during a monthly period. The comparison of results shows a promising agreement between the measured and calculated size spectra in the common size range. A supplementary information about nanometer particles was obtained from air ion measurements.

  4. 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.

  5. 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

  6. 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.

  7. Variability and Sources of Tropospheric Aerosols Over the North Atlantic in Fall: A Model Analysis in Support of the NASA NAAMES Earth-Venture Suborbital-2 Mission

    NASA Astrophysics Data System (ADS)

    Liu, H.; Moore, R.; Hostetler, C. A.; Ferrare, R. A.; Fairlie, T. D.; Hu, Y.; Chen, G.; Johnson, M. S.; Gantt, B.; Jaegle, L.

    2015-12-01

    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, with the first field deployment in November 2015. 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. As a pre-mission analysis, we examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during November 2008 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 (MERRA at 2°×2.5° horizontal resolution) from the NASA Global Modeling 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, 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 surface aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. Simulations indicate that, along the NAAMES nominal ship and flight tracks (40°W, 40-57°N), episodic pollution transport associated with frontal passages occurs at both the surface and free troposphere, with periods of relatively unperturbed marine air as indicated by

  8. Contribution of residential wood combustion and other sources to hourly winter aerosol in Northern Sweden determined by positive matrix factorization

    NASA Astrophysics Data System (ADS)

    Krecl, P.; Hedberg Larsson, E.; Ström, J.; Johansson, C.

    2008-07-01

    The combined effect of residential wood combustion (RWC) emissions with stable atmospheric conditions, which frequently occurs in Northern Sweden during wintertime, can deteriorate the air quality even in small towns. To estimate the contribution of RWC to the total atmospheric aerosol loading, positive matrix factorization (PMF) was applied to hourly mean particle number size distributions measured in a residential area in Lycksele during winter 2005/2006. The sources were identified based on the particle number size distribution profiles of the PMF factors, the diurnal contributions patterns estimated by PMF for both weekends and weekdays, and correlation of the modeled particle number concentration per factor with measured aerosol mass concentrations (PM10, PM1, and light-absorbing carbon MLAC) Through these analyses, the factors were identified as local traffic (factor 1), local RWC (factor 2), and local RWC plus long-range transport (LRT) of aerosols (factor 3). In some occasions, the PMF model could not separate the contributions of local RWC from background concentrations since their particle number size distributions partially overlapped. As a consequence, we report the contribution of RWC as a range of values, being the minimum determined by factor 2 and the possible maximum as the contributions of both factors 2 and 3. A multiple linear regression (MLR) of observed PM10, PM1, total particle number, and MLAC concentrations is carried out to determine the source contribution to these aerosol variables. The results reveal RWC is an important source of atmospheric particles in the size range 25 606 nm (44 57%), PM10 (36 82%), PM1 (31 83%), and MLAC (40 76%) mass concentrations in the winter season. The contribution from RWC is especially large on weekends between 18:00 LT and midnight whereas local traffic emissions show similar contributions every day.

  9. 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.

  10. 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. PMID:24344569

  11. Measurement of fragmentation and functionalization pathways in the multistep heterogeneous oxidation of organic aerosol

    SciTech Connect

    Kroll, Jesse H.; Smith, Jared D.; Che, Dung L.; Kessler, Sean H.; Worsnop, Douglas R.; Wilson, Kevin R.

    2009-03-10

    The competition between the addition of polar, oxygen-containing functional groups (functionalization) and the cleavage of C-C bonds (fragmentation) has a governing influence on the change in volatility of organic species upon atmospheric oxidation, and hence on the loading of tropospheric organic aerosol. However the branching between these two channels is generally poorly constrained for oxidized organics. Here we determine functionalization/fragmentation branching ratios for organics spanning a range of oxidation levels, using the heterogeneous oxidation of squalane (C30H62) as a model system. Squalane particles are exposed to high concentrations of OH in a flow reactor, and measurements of particle mass and elemental ratios enable the determination of absolute elemental composition (number of oxygen, carbon, and hydrogen atoms) of the oxidized particles. At low OH exposures, the oxygen content of the organics increases, indicating that functionalization dominates, whereas at higher exposures the amount of carbon in the particles decreases, indicating the increasing importance of fragmentation processes. Once the organics are moderately oxidized (O/C~;;0.4), fragmentation completely dominates, and the increase in O/C ratio upon further oxidation is due to the loss of carbon rather than the addition of oxygen. These results suggest that fragmentation reactions may be key steps in the atmospheric formation and evolution of oxygenated organic aerosol (OOA).

  12. 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.

  13. 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

  14. 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

  15. 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.

  16. 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.

  17. [Research on source profile of aerosol organic compounds in leather plant].

    PubMed

    Wang, Bo-Guang; Zhou, Yan; Feng, Zhi-Cheng; Liu, Hui-Xuan

    2009-04-15

    Through investigating current air pollution condition for PM10 in every factories of different style leather plants in Pearl River Delta, characteristic profile of semi-volatile organic compounds in PM10 emitted from leather factories and their contents were researched by using ultrasonic and gas chromatography and mass spectrum technology. The 6 types of organic compounds containing 46 species in total were found in the collected samples, including phenyl compounds, alcohols, PAHs, acids, esters and amides. The concentrations of PM10 in leather tanning plant, leather dying plant and man-made leather plant were 678.5, 454.5, 498.6 microgm x m(-3) respectively, and concentration of organic compounds in PM10 were 10.04, 6.89, 14.21 microg x m(-3) in sequence. The more important type of pollutants in each leather plants had higher contribution to total organic mass as follows, esters and amides in tanning plants profile account for 43.47% and 36.51% respectively; esters and alcohols in dying plants profiles account for 52.52% and 16.16% respectively; esters and amide in man-made leather plant have the highest content and account for 57.07% and 24.17% respectively. In the aerosol organic source profiles of tested leather plants, 9-octadecenamide was the abundant important species with the weight of 26.15% in tanning plant, and Bis(2-ethylhexyl) phthalate was up to 44.19% in the dying plant, and Bis(2-ethylhexyl) maleate and 1-hydroxy-piperidine had obviously higher weight in man-made plant than the other two plants.

  18. 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; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

    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

  19. 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

  20. 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

  1. 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.

    2013-09-01

    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 photo-oxidation of dilute gasoline and diesel motor vehicle exhaust. In half of the experiments POA was present in the chamber at the onset of photo-oxidation. In these experiments positive matrix factorization (PMF) was used to determine separate POA and SOA factors from aerosol mass spectrometer data. A two-factor solution, with one POA factor and one SOA factor, was sufficient to describe the organic aerosol in all but one experiment. In the other half of the experiments, POA was not present at the onset of photo-oxidation; these experiments are considered "pure SOA" experiments. The POA mass spectrum was similar to the mass spectra of the hydrocarbon-like organic aerosol factor determined from ambient datasets with one exception, a diesel vehicle equipped with a diesel oxidation catalyst. The SOA in all experiments had a constant composition over the course of photo-oxidation, and did not appear to age with continued oxidation. The SOA mass spectra for the various gasoline and diesel vehicles were similar to each other, but markedly different than ambient oxidized organic aerosol factors. Van Krevelen analysis of the POA and SOA factors for gasoline and diesel experiments reveal slopes of -0.68 and -0.43, respectively. This suggests that the oxidation chemistry in these experiments is a combination of carboxylic acid and alcohol/peroxide formation, consistent with ambient oxidation chemistry. These experiments also provide insight to the mixing behavior of the POA and SOA. Analysis of the time series of the POA factor concentration and a basis-set model both indicate that for all but one of the vehicles tested here, the POA and SOA seem to mix and form a single organic aerosol phase.

  2. 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.

  3. 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.

  4. 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.; 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 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

  5. 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.

  6. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

  7. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a. PMID:25766014

  8. 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.

  9. 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

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

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2011-02-01

    Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM1 mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (Dva) and an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00-02:00 p.m. EST due to photochemical production. The average (±σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012 (±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62 (±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified two primary OA (POA) sources, traffic and cooking, and three secondary OA (SOA) components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63), a less oxidized, semi-volatile SV-OOA (O/C = 0.38) and a unique nitrogen-enriched OA (NOA; N/C = 0.053) characterized with prominent CxH2x + 2N+ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that organic nitrogen

  11. 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.

  12. 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

  13. Composition and source apportionment of surfactants in atmospheric aerosols of urban and semi-urban areas in Malaysia.

    PubMed

    Wahid, Nurul Bahiyah Abd; Latif, Mohd Talib; Suratman, Suhaimi

    2013-06-01

    This study was conducted to determine the composition and source apportionment of surfactant in atmospheric aerosols around urban and semi-urban areas in Malaysia based on ionic compositions. Colorimetric analysis was undertaken to determine the concentrations of anionic surfactants as Methylene Blue Active Substances (MBAS) and cationic surfactants as Disulphine Blue Active Substances (DBAS) using a UV spectrophotometer. Ionic compositions were determined using ion chromatography for cations (Na(+), NH4(+), K(+), Mg(2+), Ca(2+)) and anions (F(-), Cl(-), NO3(-), SO4(2-)). Principle component analysis (PCA) combined with multiple linear regression (MLR) were used to identify the source apportionment of MBAS and DBAS. Results indicated that the concentrations of surfactants at both sampling sites were dominated by MBAS rather than DBAS especially in fine mode aerosols during the southwest monsoon. Three main sources of surfactants were identified from PCA-MLR analysis for MBAS in fine mode samples particularly in Kuala Lumpur, dominated by motor vehicles, followed by soil/road dust and sea spray. Besides, for MBAS in coarse mode, biomass burning/sea spray were the dominant source followed by motor vehicles/road dust and building material. PMID:23336924

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

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2010-10-01

    peaking around local lunch and dinner times. In addition, NOA is characterized with prominent CxH2x+2N+ peaks likely from amine compounds. Our results indicate that cooking-related activities are a major source of POA in NYC, releasing comparable amounts of POA as traffic emissions. POA=HOA+COA) on average accounts for ~30% of the total OA mass during this study while SOA dominates the OA composition with SV-OOA and LV-OOA on average accounting for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC involves a~continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that nitrogen-containing organic species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving acid-base chemistry. Analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD) indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.

  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, 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

  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, 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

  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. 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.

  20. Sources and characteristics of carbonaceous aerosols at Agra "World heritage site" and Delhi "capital city of India".

    PubMed

    Pipal, A S; Tiwari, S; Satsangi, P G; Taneja, Ajay; Bisht, D S; Srivastava, A K; Srivastava, M K

    2014-01-01

    Agra, one of the oldest cities "World Heritage site", and Delhi, the capital city of India are both located in the border of Indo-Gangetic Plains (IGP) and heavily loaded with atmospheric aerosols due to tourist place, anthropogenic activities, and its topography, respectively. Therefore, there is need for monitoring of atmospheric aerosols to perceive the scenario and effects of particles over northern part of India. The present study was carried out at Agra (AGR) as well as Delhi (DEL) during winter period from November 2011 to February 2012 of fine particulate (PM₂.₅: d < 2.5 μm) as well as associated carbonaceous aerosols. PM₂.₅ was collected at both places using medium volume air sampler (offline measurement) and analyzed for organic carbon (OC) and elemental carbon (EC). Also, simultaneously, black carbon (BC) was measured (online) at DEL. The average mass concentration of PM₂.₅ was 165.42 ± 119.46 μg m(-3) at AGR while at DEL it was 211.67 ± 41.94 μg m(-3) which is ~27% higher at DEL than AGR whereas the BC mass concentration was 10.60 μg m(-3). The PM₂.₅ was substantially higher than the annual standard stipulated by central pollution control board and United States Environmental Protection Agency standards. The average concentrations of OC and EC were 69.96 ± 34.42 and 9.53 ± 7.27 μm m(-3), respectively. Total carbon (TC) was 79.01 ± 38.98 μg m(-3) at AGR, while it was 50.11 ± 11.93 (OC), 10.67 ± 3.56 μg m(-3) (EC), and 60.78 ± 14.56 μg m(-3) (TC) at DEL. The OC/EC ratio was 13.75 at (AGR) and 5.45 at (DEL). The higher OC/EC ratio at Agra indicates that the formation of secondary organic aerosol which emitted from variable primary sources. Significant correlation between PM₂.₅ and its carbonaceous species were observed indicating similarity in sources at both sites. The average concentrations of secondary organic carbon (SOC) and primary organic carbon (POC) at AGR were 48.16 and 26

  1. Sources and characteristics of carbonaceous aerosols at Agra "World heritage site" and Delhi "capital city of India".

    PubMed

    Pipal, A S; Tiwari, S; Satsangi, P G; Taneja, Ajay; Bisht, D S; Srivastava, A K; Srivastava, M K

    2014-01-01

    Agra, one of the oldest cities "World Heritage site", and Delhi, the capital city of India are both located in the border of Indo-Gangetic Plains (IGP) and heavily loaded with atmospheric aerosols due to tourist place, anthropogenic activities, and its topography, respectively. Therefore, there is need for monitoring of atmospheric aerosols to perceive the scenario and effects of particles over northern part of India. The present study was carried out at Agra (AGR) as well as Delhi (DEL) during winter period from November 2011 to February 2012 of fine particulate (PM₂.₅: d < 2.5 μm) as well as associated carbonaceous aerosols. PM₂.₅ was collected at both places using medium volume air sampler (offline measurement) and analyzed for organic carbon (OC) and elemental carbon (EC). Also, simultaneously, black carbon (BC) was measured (online) at DEL. The average mass concentration of PM₂.₅ was 165.42 ± 119.46 μg m(-3) at AGR while at DEL it was 211.67 ± 41.94 μg m(-3) which is ~27% higher at DEL than AGR whereas the BC mass concentration was 10.60 μg m(-3). The PM₂.₅ was substantially higher than the annual standard stipulated by central pollution control board and United States Environmental Protection Agency standards. The average concentrations of OC and EC were 69.96 ± 34.42 and 9.53 ± 7.27 μm m(-3), respectively. Total carbon (TC) was 79.01 ± 38.98 μg m(-3) at AGR, while it was 50.11 ± 11.93 (OC), 10.67 ± 3.56 μg m(-3) (EC), and 60.78 ± 14.56 μg m(-3) (TC) at DEL. The OC/EC ratio was 13.75 at (AGR) and 5.45 at (DEL). The higher OC/EC ratio at Agra indicates that the formation of secondary organic aerosol which emitted from variable primary sources. Significant correlation between PM₂.₅ and its carbonaceous species were observed indicating similarity in sources at both sites. The average concentrations of secondary organic carbon (SOC) and primary organic carbon (POC) at AGR were 48.16 and 26

  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. 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.

  4. 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...

  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. The hydrogen-sulfur correlation, by PIXE plus PESA, and aerosol source identification

    NASA Astrophysics Data System (ADS)

    Cahill, Thomas A.; Eldred, Robert A.; Wallace, Don; Kusko, Bruce H.

    1987-03-01

    The use of hydrogen-free thin teflon filters for particulate sampling has allowed us to simultaneously measure sulfur (and other elements) by PIXE and hydrogen by PESA. Particulate hydrogen in nonvolatile forms (since all analyses are in vacuum) is an important component of aerosols, totalling typically about {1}/{3} of all atoms. The hydrogen is measured at the same time as PIXE by placing a surface barrier detector at 30° in the forward direction, allowing the (p, p) kinematic energy shift to safely resolve hydrogen from the unresolved peaks of C, N, O, and heavier elements. The method is absolute and simple, with no important corrections. Sensitivity on 400 {μg}/{cm 2} teflon filters is about 5 {ng}/{cm 2} H in 100s. This technique was introduced to the National Park Service 31 station network in June. 1984, and immediately proved enormously valuable in separating natural aerosols from anthropogenic aerosols. For example, at Great Smoky NP, the H/S correlation was excellent, > 0.90, while the molar ratio was 10:1 (note: (NH 4) 2SO 4) has a ratio 8:1), while at North Cascades NP, there was essentially no correlation and the {H}/{S} molar ratio was 37:1. In the former, most hydrogen is tied to presumably anthropogenic sulfur species, while at North Cascades NP, the converse is true. Evidence of H 2SO 4) aerosols from Arctic studies will also be shown.

  7. 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...

  8. SOURCE APPORTIONMENT OF PRIMARY AND SECONDARY CARBONACEOUS AEROSOL IN THE UNITED STATES USING MODELS AND MEASUREMENTS

    EPA Science Inventory

    In this presentation, three diagnostic evaluation methods of model performance for carbonaceous aerosol are reviewed. The EC-tracer method is used to distinguish primary and secondary carbon, radiocarbon data are used to distinguish fossil-fuel and contemporary carbon, and organ...

  9. Characterization and source apportionment of aerosol light extinction in Chengdu, southwest China

    NASA Astrophysics Data System (ADS)

    Tao, Jun; Zhang, Leiming; Cao, Junji; Hsu, Shih-Chieh; Xia, Xiangao; Zhang, Zhisheng; Lin, Zejian; Cheng, Tiantao; Zhang, Renjian

    2014-10-01

    To investigate aerosol properties in the Sichuan Basin of China, field aerosol sampling was carried out in Chengdu, China during four one-month periods, each in a different season in 2011. Aerosol scattering coefficient (bsp) at dry (RH<40%) and wet (40% < RH<90%) conditions and aerosol absorption coefficient (bap) were measured. Additionally, daily PM2.5 and PM10 samples were also collected. PM2.5 samples were subject to chemical analysis for various chemical components including major water-soluble ions, organic and elemental carbon (OC and EC), trace elements, as well as anhydrosugar Levoglucosan (LG) and Mannosan (MN). A multiple linear regression analysis was applied to the measured dry bsp against (NH4)2SO4, NH4NO3, organic mass (OM), fine soil (FS), and coarse mass (CM, PM2.5-10), and to the measured bap against EC in all the four seasons to evaluate the impact of individual chemical components of PM2.5 and CM on aerosol light extinction (bext = bsp + bap). Mass scattering efficiency (MSE) and mass absorption efficiency (MAE) of the individual chemical components of PM2.5 were estimated based on seasonal regression equations and were then used for estimating bext. The annual bsp, bap and single scattering albedo (SSA) at dry conditions were 456 ± 237 Mm-1, 96 ± 48 Mm-1 and 0.82 ± 0.05, respectively. The annual average bsp at ambient conditions estimated through hygroscopic curve of aerosol (f(RH)) was 763 ± 415 Mm-1, which was 1.7 times of the dry bsp. The annual average SSA at ambient conditions also increased to 0.88 ± 0.04. The estimated dry bext was only 2 ± 9% higher than the measurements and the estimated ambient bext from individual chemical components was only 1 ± 10% lower, on an annual basis, than that estimated from using f(RH). Secondary inorganic aerosols, coal combustion, biomass burning, iron and steel industry, Mo-related industry, soil dust, and CM to bext were estimated to account for 41 ± 19%, 18 ± 12%, 14 ± 13%, 13 ± 11%, 5

  10. Source and variation of carbonaceous aerosols at Mount Tai, North China: Results from a semi-continuous instrument

    NASA Astrophysics Data System (ADS)

    Wang, Zhe; Wang, Tao; Gao, Rui; Xue, Likun; Guo, Jia; Zhou, Yang; Nie, Wei; Wang, Xinfeng; Xu, Pengju; Gao, Jian; Zhou, Xuehua; Wang, Wenxing; Zhang, Qingzhu

    2011-03-01

    Carbonaceous aerosols were measured with a semi-continuous thermal-optical OC/EC analyzer at the summit of Mount Tai (1532.7 m a.s.l) in north China during spring and summer of 2007. Non-volatile organic carbon (NVOC) and elemental carbon (EC) showed high concentrations with mean values of 6.07, 1.77 and 5.05, 0.99 μg m -3 in spring and summer, respectively. The mean concentration of semi-volatile organic carbon (SVOC) was 6.26 μg m -3 in spring and 13.33 μg m -3 in summer, contributing 51 and 72% to total organic carbon (TOC), respectively. Different measurement methods for EC were compared, and a good agreement between optical and thermal methods was found. Due to volatilization of SVOC during sampling, the integrated filter measurement without denuder and backup absorbent tended to underestimate TOC compared to semi-continuous measurement. Principal component analysis (PCA) and hierarchical cluster analysis (HCA) results indicated that the observed carbonaceous aerosols at Mount Tai were mostly contributed by the transport of aged aerosols in the planetary boundary layer (PBL) mixed with combined sources. Also, the influence of emissions from Korea was observed at Mount Tai, as well as biomass burning. Cloud processing contributed to elevated SVOC concentrations, and the formation of secondary organic aerosol (SOA) through photochemistry and cloud processing were both enhanced in summer. Clean air masses from the free troposphere reduced carbonaceous concentrations, and the regional background condition with 2.13 ± 1.05 μg m -3 of NVOC, 0.43 ± 0.29 μg m -3 of EC, and 2.40 to 6.80 μg m -3 of SVOC (for spring and summer, respectively) were suggested for the North China Plain.

  11. Air pollution of Moscow by the carbon monoxide and aerosols, boundary layer parameters and estimation of the CO sources intensity.

    NASA Astrophysics Data System (ADS)

    Rakitin, V.; Fokeeva, E.; Kuznetsov, R.; Emilenko, A.; Kopeikin, V.

    2009-04-01

    The results of measurements of the carbon monoxide total content, the soot and submicron aerosols content are given for the period 2005-2008 over Moscow. Two identical grating spectrometers of medium resolution (0,2sm-1) are used with appropriate solar tracking systems, one of which is located outside the city at Zvenigorod Scientific Station (ZSS 56oN, 38oE, 60km West from Moscow in the rural zone) and the other one is inside a city center. This method makes possible to determine the characteristics of anthropogenic pollution, urban part of the CO content. Some simultaneously measurements of aerosols content, the CO column and CO background concentrations in Moscow, autumn 2007 are presented. Nephelometer and quartz filters for soot sampling were used for aerosols measurements. Correlations coefficients between aerosols, CO background concentration and urban part of the CO content were obtained. Permanent sounding of boundary layer was carried out using acoustic locator (SODAR) LATAN-3. Applications of SODAR data (profile of wind speed and inversion height) makes possible to forecast of air pollution situations in megacities area. We obtained the correlation coefficients for the urban part of the CO content with the wind speed for cold and warm seasons. Analysis results of measurements demonstrated preeminent influence of the wind in certain boundary layer (up to 500m) upon the CO extension. The intensity of CO sources in Moscow was estimated. The systematization of CO diurnal variations for different meteorological conditions was performed. Comparing our results with the results of the earlier measurements period (1993-2005), we found out that the urban part of the CO content in the surface air layer over the city did not increase in spite of more than tripled number of motor-vehicles in Moscow. So using the applications of this spectroscopic method we can obtain the air pollution trend from the averaged air pollution measured values.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. 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

  19. A new description of Titan's aerosol optical properties from the analysis of VIMS Emission Phase Function observations

    NASA Astrophysics Data System (ADS)

    Rodriguez, Sebastien; Maltagliati, Luca; Sotin, Christophe; Rannou, Pascal; Bézard, Bruno; Cornet, Thomas

    2016-10-01

    The Huygens probe gave unprecedented information on the properties of Titan's aerosols (vertical distribution, opacity as a function of wavelength, phase function, single scattering albedo) by in-situ measurements (Tomasko et al. 2008). Being the only existing in-situ atmospheric probing for Titan, this aerosol model currently is the reference for many Titan studies (e.g. by being applied as physical input in radiative transfer models of the atmosphere). Recently a reanalysis of the DISR dataset, corroborated by data from the Downward-Looking Visible Spectrometer (DLVS), was carried out by the same group (Doose et al. 2016), leading to significant changes to the indications given by Tomasko et al. (2008).Here we present the analysis of the Emission Phase Function observation (EPF) performed by VIMS during the Cassini flyby T88 (November 2012). An EPF observes the same spot on the surface (and thus the same atmosphere) with the same emergence angle but with different incidence angles. In this way, our EPF allows, for the first time, to have direct information on the phase function of Titan's aerosols, as well as on other important physical parameters of the aerosols as the behavior of their extinction as a function of wavelength and the single scattering albedo (also as a function of wavelength) for the whole VIMS range (0.8-5.2 μm). The T88 EPF is composed of 25 VIMS datacubes spanning a scattering angle range approximately from 0°to 70°.We used the radiative transfer model described in Hirtzig et al. (2013) as baseline, updated with improved methane (+ related isotopes) spectroscopy. By changing the aerosol description in the model, we found the combination of aerosol optical parameters that fits best a constant aerosol column density over the whole set of the VIMS datacubes. We confirmed that the new results from Doose et al. (2016) do improve the fit for what concerns the vertical profile and the extinction as a function of wavelength. However, a different

  20. A new description of Titan's aerosol optical properties from the analysis of VIMS Emission Phase Function observations

    NASA Astrophysics Data System (ADS)

    Maltagliati, Luca; Rodriguez, Sebastien; Sotin, Christophe; Rannou, Pascal; Bezard, Bruno; Cornet, Thomas

    2016-06-01

    The Huygens probe gave unprecedented information on the properties of Titan's aerosols (vertical distribution, opacity as a function of wavelength, phase function, single scattering albedo) by in-situ measurements (Tomasko et al. 2008). Being the only existing in-situ atmospheric probing for Titan, this aerosol model currently is the reference for many Titan studies (e.g. by being applied as physical input in radiative transfer models of the atmosphere). Recently a reanalysis of the DISR dataset, corroborated by data from the Downward-Looking Visible Spectrometer (DLVS), was carried out by the same group (Doose et al. 2016), leading to significant changes to the indications given by Tomasko et al. (2008). Here we present the analysis of the Emission Phase Function observation (EPF) performed by VIMS during the Cassini flyby T88 (November 2012). An EPF observes the same spot on the surface (and thus the same atmosphere) with the same emergence angle but with different incidence angles. In this way, our EPF allows, for the first time, to have direct information on the phase function of Titan's aerosols, as well as on other important physical parameters of the aerosols as the behavior of their extinction as a function of wavelength and the single scattering albedo (also as a function of wavelength) for the whole VIMS range (0.8-5.2 µm). The T88 EPF is composed of 25 VIMS datacubes spanning a scattering angle range approximately from 0°to 70°. We used the radiative transfer model described in Hirtzig et al. (2013) as baseline, updated with improved methane (+ related isotopes) spectroscopy. By changing the aerosol description in the model, we found the combination of aerosol optical parameters that fits best a constant aerosol column density over the whole set of the VIMS datacubes. We confirmed that the new results from Doose et al. (2016) do improve the fit for what concerns the vertical profile and the extinction as a function of wavelength. However, a different

  1. 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

  2. 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.

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

    PubMed

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

    2015-04-21

    A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends. PMID:25793355

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

    PubMed

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

    2015-04-21

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

  5. 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.

  6. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Perron, N.; Ciobanu, V. G.; Zotter, P.; Minguillón, M. C.; Wacker, L.; Prévôt, A. S. H.; Baltensperger, U.; Szidat, S.

    2012-11-01

    Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. The optimal strategy for 14C-based source apportionment of carbonaceous aerosols should follow an approach to subdivide TC into different carbonaceous aerosol fractions for individual 14C analyses, as these fractions may differ in their origins. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon measurements; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols

  7. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Perron, N.; Ciobanu, V. G.; Zotter, P.; Minguillón, M. C.; Wacker, L.; Prévôt, A. S. H.; Baltensperger, U.; Szidat, S.

    2012-07-01

    Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters, and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C, followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols like EUSAAR_2, compared to pure oxygen methods; and (4) S4 in O2 at 760 °C for recovery of the remaining EC. WINSOC was found to have a significantly higher fossil contribution than the water-soluble OC (WSOC). Moreover, the experimental results

  8. Organic compounds in urban aerosols from Gent, Belgium: Characterization, sources, and seasonal differences

    NASA Astrophysics Data System (ADS)

    KubáTová, Alena; Vermeylen, Reinhilde; Claeys, Magda; Cafmeyer, Jan; Maenhaut, Willy

    2002-11-01

    About 100 individual organic compounds were determined in urban aerosols collected at Gent, Belgium. The compounds were identified by gas chromatography-mass spectrometry, and quantitative data were obtained by gas chromatography-flame ionization detection. Measurements of the particulate mass and of organic and elemental carbon mass were also made. Aerosol samples from a winter and a summer campaign were analyzed in order to examine seasonal differences. The major part of the extractable and elutable organic carbon in both winter and summer aerosols was found to correspond to an unresolved complex mixture that is typical for car exhaust. The prevailing resolved organic compounds in both seasons were n-alkanes and fatty acids, but the distribution patterns of individual components within each class showed seasonal differences. The n-alkane pattern for summer aerosols was clearly affected by emissions from the vegetation, while that of fatty acids revealed a lower relative abundance of unsaturated fatty acids in summer than winter that can be related to more extensive atmospheric oxidation of unsaturated fatty acids during summer. Concentrations of dicarboxylic acids and related products that are believed to be oxidation products of hydrocarbons and fatty acids were highest in summer aerosols. Some individual compounds in the latter class could only be detected in summer samples and showed the highest concentrations on hot summer days that were characterized by maximum temperatures above 25°C and increased ozone concentrations. The latter compounds included novel, recently identified glutaric acid derivatives, namely, 3-isopropyl and 3-acetyl pentanedioic acid, likely originating from atmospheric oxidation of reactive monoterpene or sesquiterpene precursors that still need to be identified. Several compounds were found that are markers of wood combustion, including diterpenoic acids, lignin pyrolysis products, and levoglucosan. The quantitative results obtained for

  9. Aerosol composition and sources during high and low pollution periods in Ningbo, China

    NASA Astrophysics Data System (ADS)

    Xu, Jing-Sha; Xu, Hong-Hui; Xiao, Hang; Tong, Lei; Snape, Colin E.; Wang, Cheng-Jun; He, Jun

    2016-09-01

    Due to the rapid industrialization of the Yangtze River Delta (YRD) region in China, heavy air pollution episodes have occurred frequently over the past five years which are of great concern due to their environmental and health impacts. To investigate the chemical characteristics of the highly polluted aerosols in this region, a sampling campaign had been conducted in Ningbo from 3 December 2012 to 27 June 2013, during which a month long high pollution episode had been captured. Daily average PM2.5 concentrations during high and low pollution periods were 111 μg m-3 and 53 μg m-3, respectively. The most polluted day was 8 January 2013 with a PM2.5 concentration up to 175 μg m- 3. To understand the origin of the highly polluted aerosols, meteorological conditions, air mass backward trajectories, distribution of fire spots in surrounding areas and various categories of aerosol pollutants were analyzed, including trace metals, inorganic species, PAHs and anhydrosugars. Total metal concentrations were 3.8 and 1.6 μg m-3 for the high and low pollution episodes, respectively, accounting for 3.4% and 3.1% of the total PM2.5 mass. Total concentrations of ionic species accounted for more than 50.0% of the PM2.5 by mass, with dominant ions (nitrate, sulfate, ammonium) accounting for over 42.0% of the PM2.5 mass concentrations in both periods. During the high pollution episode, enhanced Cd-Pb and biomarker (levoglucosan, mannosan) levels indicated the contributions from coal combustion, traffic and biomass burning to fine aerosol PM2.5. The average diagnostic ratio of Fla/(Fla + Pyr) was 0.54 in high pollution episode, which was intermediate between that for wood (> 0.50) and coal combustion (0.58). BaP/Bpe was 0.49 and 0.30 for the highly and lightly polluted aerosols respectively, associated with the significant non-traffic emissions (< 0.60). In addition, stagnant weather conditions during the high pollution period and long-range transport of air masses from heavy

  10. 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

  11. Composition and major sources of organic compounds of aerosol particulate matter sampled during the ACE-Asia campaign

    NASA Astrophysics Data System (ADS)

    Simoneit, Bernd R. T.; Kobayashi, Minoru; Mochida, Michihiro; Kawamura, Kimitaka; Lee, Meehye; Lim, Ho-Jin; Turpin, Barbara J.; Komazaki, Yuichi

    2004-10-01

    The organic compound tracers of atmospheric particulate matter, as well as organic carbon (OC) and elemental carbon (EC), have been characterized for samples acquired during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) from Gosan, Jeju Island, Korea, from Sapporo, Japan, and from Chichi-jima Island in the western North Pacific, as well as on the National Oceanic and Atmospheric Administration R/V Ronald H. Brown. Total extracts were analyzed by gas chromatography-mass spectrometry to determine both polar and aliphatic compounds. Total particles, organic matter, and lipid and saccharide compounds were high during the Asian dust episode (early April 2001) compared to levels at other times. The organic matter can be apportioned to seven emission sources and to significant oxidation-producing secondary products during long-range transport. Terrestrial natural background compounds are vascular plant wax lipids derived from direct emission and as part of desert sand dust. Fossil fuel utilization is obvious and derives from petroleum product and coal combustion emissions. Saccharides are a major polar (water-soluble) carbonaceous fraction derived from soil resuspension (agricultural activities). Biomass-burning smoke is evident in all samples and seasons. It contributes up to 13% of the total compound mass as water-soluble constituents. Burning of refuse is another source of organic particles. Varying levels of marine-derived lipids are superimposed during aerosol transport over the ocean. Secondary oxidation products increase with increasing transport distance and time. The ACE-Asia aerosols are composed not only of desert dust but also of soil dust, smoke from biomass and refuse burning, and emissions from fossil fuel use in urban areas.

  12. Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona, Spain

    NASA Astrophysics Data System (ADS)

    Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.

    2013-04-01

    This study investigates the contribution of potential sources to the sub-micron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by Gas Chromatography-Mass Spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by Multivariate Curve Resolution-Alternating Least Squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin, three of secondary OA origin while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (Urban primary organic aerosol, Urban POA) contributed for 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA in RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation. Three Secondary Organic Aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO), i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols, showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, 16% and 7%, at UB and RS, respectively). By contrast, a SOA biogenic component attributed to α-pinene oxidation (SOA

  13. Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona (Spain) during SAPUSS

    NASA Astrophysics Data System (ADS)

    Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.

    2013-10-01

    This study investigates the contribution of potential sources to the submicron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). A total of 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by gas chromatography-mass spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by multivariate curve resolution-alternating least squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin and three of secondary OA origin, while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (urban primary organic aerosol, or POA Urban), mainly traffic emissions but also cigarette smoke, contributed 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA at RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation (REG.). Three secondary organic aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO) - i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols - showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, or 16% and 7%, at UB and RS, respectively

  14. Anthropogenic sources of aerosol particles in a football stadium: Real-time characterization of emissions from cigarette smoking, cooking, hand flares, and color smoke bombs by high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Faber, Peter; Drewnick, Frank; Veres, Patrick R.; Williams, Jonathan; Borrmann, Stephan

    2013-10-01

    Aerosol particles from several anthropogenic sources associated with football stadia including cooking, cigarette smoking, burning of color smoke bombs and hand flares were analyzed by high-resolution aerosol mass spectrometry. The physical and chemical characteristics of these different aerosols, in particular the organic fraction, were explored in laboratory studies to obtain robust references. These data were compared with field campaign results from a Bundesliga (German football league) match in the Coface Arena (Mainz, Germany) on 20th April 2012. The field measurement revealed a strongly elevated mass concentration of organic aerosols (OA) compared to background levels showing a temporal structure clearly related to the match. PMF analysis established that during the football match event cigarette smoke was the predominant component of submicron organic aerosol (67% of total OA). Cooking emissions from food outlets within the stadium correlated well with the sales figures of the catering stations and were also found to be of relevance (24% of total OA) especially in the period before kickoff. Pyrotechnics were not observed during this football match and no signatures of these sources were found in the mass spectra from the stadium measurements. All species that were elevated during the football match returned to their initial background levels within one hour after the match had finished. This demonstrates a good ventilation capacity of the open-topped Coface Arena.

  15. Chemical characterisation of atmospheric aerosols during a 2007 summer field campaign at Brasschaat, Belgium: sources and source processes, time series, diel variations, and temperature dependencies

    NASA Astrophysics Data System (ADS)

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

    2011-08-01

    Measurements of organic marker compounds and inorganic species were performed on PM2.5 aerosols from a Belgian forest site that is severely impacted by urban pollution ("De Inslag", Brasschaat, Belgium) during a 2007 summer period within the framework of the "Formation mechanisms, marker compounds, and source apportionment for biogenic atmospheric aerosols (BIOSOL)" project. The objectives of this study were to determine sources, source processes, time series, and diel variations of the organic species, and to explore the relationships between their concentrations and those of trace gases (O3, NO2, SO2, and CO2) or meteorological parameters (temperature, relative humidity, wind speed, and rain fall). The measured organic species included (i) low-molecular weight (MW) dicarboxylic acids (LMW DCAs), (ii) methanesulfonate (MSA), and (iii) terpenoic acids originating from the oxidation of α-pinene, β-pinene, d-limonene and Δ3-carene, and (iv) organosulfates related to secondary organic aerosol (SOA) from the oxidation of isoprene and α-pinene. The measurements of MSA, the LMW DCAs and selected inorganic species were done with ion chromatography (IC), while those of the terpenoic acids and organosulfates were performed using liquid chromatography with negative ion electrospray ionisation mass spectrometry [LC/(-)ESI-MS]. The organic tracers explained, on average, 5.3 % of the organic carbon (OC), of which 0.7 % was due to MSA, 3.4 % to LMW DCAs, and 1.2 % to organosulfates and terpenoic acids. The highest atmospheric concentrations of most species were observed during the first five days of the campaign, which were characterised by maximum day-time temperatures >22 °C. Most of the terpenoic acids and the organosulfates peaked during day-time, consistent with their photochemical origin, except the MW 295 α-pinene-related nitrooxy organosulfates and the terpenoic acids, cis-pinic, caric, and limonic acid. High concentrations of 3-methyl-1,2,3-butanetricarboxylic

  16. Ball Lightning Aerosol Electrochemical Power Source or A Cloud of Batteries

    NASA Astrophysics Data System (ADS)

    Meshcheryakov, Oleg

    2007-07-01

    Despite numerous attempts, an adequate theoretical and experimental simulation of ball lightning still remains incomplete. According to the model proposed here, the processes of electrochemical oxidation within separate aerosol particles are the basis for this phenomenon, and ball lightning is a cloud of composite nano or submicron particles, where each particle is a spontaneously formed nanobattery which is short-circuited by the surface discharge because it is of such a small size. As free discharge-shorted current loops, aerosol nanobatteries are exposed to a powerful mutual magnetic dipole dipole attraction. The gaseous products and thermal energy produced by each nanobattery as a result of the intra-particle self-sustaining electrochemical reactions, cause a mutual repulsion of these particles over short distances and prevent their aggregation, while a collectivization of the current loops of separate particles, due to the electric arc overlapping between adjacent particles, weakens their mutual magnetic attraction over short distances. Discharge currents in the range of several amperes to several thousand amperes as well as the pre-explosive mega ampere currents, generated in the reduction oxidation reactions and distributed between all the aerosol particles, explain both the magnetic attraction between the elements of the ball lightning substance and the impressive electromagnetic effects of ball lightning.

  17. The influence of continental sources of aerosols on the marine stratocumulus during FIRE IFO-1

    NASA Technical Reports Server (NTRS)

    Durkee, Philip A.

    1990-01-01

    The effects of aerosols on the microphysical characteristics of marine stratocumulus clouds can have a significant impact on climate processes through modification of cloud radiative properties. The effect of aerosols on clouds and the impact on climate processes have recently been discussed by several authors (Twomey et al., 1984; Coakley et al., 1987; Charlson et al., 1987). Of particular concern is the potential for observing variations of cloud characteristics that might be related to variations of available aerosols. The results of comparisons between aircraft-measured microphysical characteristics and satellite-detected radiative properties of marine stratocumulus clouds are presented. These results are extracted from Mineart (1988) and Durkee and Mineart (1989) where the analysis procedures and a full discussion of the observations are presented. Due to the space available, only a brief description of the results is presented. The satellite data used here are from the National Oceanic and Atmospheric Administration (NOAA) Advanced Very High Resolution Radiometer (AVHRR) collected at the Scripps Satellite Oceanography Facility. The AVHRR channel 1 (0.63 microns), channel 2 (0.86 microns), channel 3 (3.7 microns), and channel 4 (11 microns) data were used in the analysis. Cloud microphysical data were obtained by instruments on the NCAR Electra during cloud-penetrating missions in support of the field operations from 29 June to 19 July 1988.

  18. Ball Lightning–Aerosol Electrochemical Power Source or A Cloud of Batteries

    PubMed Central

    2007-01-01

    Despite numerous attempts, an adequate theoretical and experimental simulation of ball lightning still remains incomplete. According to the model proposed here, the processes of electrochemical oxidation within separate aerosol particles are the basis for this phenomenon, and ball lightning is a cloud of composite nano or submicron particles, where each particle is a spontaneously formed nanobattery which is short-circuited by the surface discharge because it is of such a small size. As free discharge-shorted current loops, aerosol nanobatteries are exposed to a powerful mutual magnetic dipole–dipole attraction. The gaseous products and thermal energy produced by each nanobattery as a result of the intra-particle self-sustaining electrochemical reactions, cause a mutual repulsion of these particles over short distances and prevent their aggregation, while a collectivization of the current loops of separate particles, due to the electric arc overlapping between adjacent particles, weakens their mutual magnetic attraction over short distances. Discharge currents in the range of several amperes to several thousand amperes as well as the pre-explosive mega ampere currents, generated in the reduction–oxidation reactions and distributed between all the aerosol particles, explain both the magnetic attraction between the elements of the ball lightning substance and the impressive electromagnetic effects of ball lightning.

  19. Chemical Composition and Sources of Aerosols in Finnish Arctic: 1964 - 2008

    NASA Astrophysics Data System (ADS)

    Husain, L.; Dutkiewicz, V. A.; Dejulio, A.; Ahmed, T.; Laing, J.; Hopke, P. K.; Paatero, J.; Viisanen, Y.

    2013-12-01

    BC particles strongly absorb solar radiation and impact the Earth's climate. In fact, BC may be the second largest contributor to global warming after greenhouses gases. However, the magnitude of the climate forcing by BC is quite uncertain, with a global average value estimated up to + 1.1W m-2 [Bond et al., 2013]. Direct long-term atmospheric measurements in the Arctic are required to evaluate the BC trends, variability and contributions from local as well as distant regional sources. Such information will permit the development of a strategy to minimize its impact on the climate. In this paper we report the measurements of concentrations of black carbon, [BC], SO4, methane sulfonic acid (MSA) and trace elements in filters collected weekly for 47 consecutive years at Kevo, Finland (69o 45' N and 27o 02' E) from 1964-2010. The data provides the longest record of direct measurement of these particulate species, and should be invaluable in assessing the impact of changes in emissions from nearby as well as distant sources. BC concentrations were determined in individual filters using thermal-optical and optical methods. The mean winter, spring, summer, and autumn [BC] were, 339, 199, 127, and 213 ngm-3, respectively. Annual [BC] decreased from 645 in 1965 to 82 ngm-3 in 2010, a nearly 8-fold decrease. There was a sharp decrease in concentrations after 1988, around the time of the collapse of the USSR. An overall decreasing trend was observed for all anthropogenic elements except lead where there was a decline that reflects the shift to unleaded gasoline. The 47-year complete data set will be analyzed by Positive Matrix Factorization (PMF). The receptor modeling results will be connected with back trajectory data in a Potential Source Contribution Function (PSCF) analysis to determine possible source areas. The combination of PMF and PSCF will identify sources and their geographic locations. Initial PSCF results with MSA show the Barents Sea and related areas as the