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Sample records for aerosol nr-pm1 species

  1. Effect of Vaporizer Temperature on Ambient Non-Refractory Submicron Aerosol Composition and Mass Spectra Measured by the Aerosol Mass Spectrometer

    EPA Science Inventory

    Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (Tvap) of 600oC in order to facilitate quantitative detection of non-refractory submicron (NR-PM1) species. By analogy with other thermal desorption instrument...

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

    SciTech Connect

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

    2015-04-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

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

    SciTech Connect

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

    2015-04-01

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

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

    DOE PAGES

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

    2015-04-01

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

  6. Size-resolved aerosol chemistry on Whistler Mountain, Canada with a High-Resolution Aerosol Mass Spectrometer during INTEX-B

    NASA Astrophysics Data System (ADS)

    Sun, Y.; Zhang, Q.; MacDonald, A. M.; Hayden, K.; Li, S. M.; Liggio, J.; Liu, P. S. K.; Anlauf, K. G.; Leaitch, W. R.; Cubison, M.; Worsnop, D.; van Donkelaar, A.; Martin, R. V.

    2008-12-01

    An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (elevation 2182 m-MSL), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ every 5 min. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m-3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed a~large accumulation mode peaking around 500-600 nm in Dva while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggest that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event

  7. New characteristics of submicron aerosols and factor analysis of combined organic and inorganic aerosol mass spectra during winter in Beijing

    NASA Astrophysics Data System (ADS)

    Zhang, J. K.; Ji, D. S.; Liu, Z. R.; Hu, B.; Wang, L. L.; Huang, X. J.; Wang, Y. S.

    2015-07-01

    In recent years, an increasing amount of attention has been paid to heavy haze pollution in Beijing, China. In addition to Beijing's population of approximately 20 million and its 5 million vehicles, nearby cities and provinces are host to hundreds of heavily polluting industries. In this study, a comparison between observations in January 2013 and January 2014 showed that non-refractory PM1 (NR-PM1) pollution was weaker in January 2014, which was primarily caused by variations in meteorological conditions. For the first time, positive matrix factorization (PMF) was applied to the merged high-resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer measurements in Beijing, and the sources and evolution of NR-PM1 in January 2014 were investigated. The two factors, NO3-OA1 and NO3-OA2, were primarily composed of ammonium nitrate, and each showed a different degree of oxidation and diurnal variation. The organic fraction of SO4-OA showed the highest degree of oxidation of all PMF factors. The hydrocarbon-like organic aerosol (OA) and cooking OA factors contained negligible amounts of inorganic species. The coal combustion OA factor contained a high contribution from chloride in its mass spectrum. The NR-PM1 composition showed significant variations in January 2014, in which the contribution of nitrate clearly increased during heavy pollution events. The most effective way to control fine particle pollution in Beijing is through joint prevention and control measures at the regional level, rather than a focus on an individual city, especially for severe haze events.

  8. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  9. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry. PMID:26348650

  10. ACTRIS ACSM intercomparison - Part I: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with Time-of-Flight ACSM (ToF-ACSM), High Resolution ToF Aerosol Mass Spectrometer (HR-ToF-AMS) and other co-located instruments

    NASA Astrophysics Data System (ADS)

    Crenn, V.; Sciare, J.; Croteau, P. L.; Verlhac, S.; Fröhlich, R.; Belis, C. A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artiñano, B.; Baisnée, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petit, J.-E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Estève, R.; Slowik, J. G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prévôt, A. S. H.; Jayne, J. T.; Favez, O.

    2015-07-01

    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for three weeks during the late fall-early winter period (November-December 2013). The first week was dedicated to tuning and calibration of each instrument whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual ACSM across all chemical families except for chloride for which three ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025) and were found to be of 9, 15, 19, 28 and 36 % for NR-PM1, nitrate, organic matter, sulfate and ammonium respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of ACSMs, detailed intercomparison results are presented as well as a discussion of some recommendations

  11. 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

  12. ACTRIS ACSM intercomparison - Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments

    NASA Astrophysics Data System (ADS)

    Crenn, V.; Sciare, J.; Croteau, P. L.; Verlhac, S.; Fröhlich, R.; Belis, C. A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artiñano, B.; Baisnée, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petit, J.-E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Estève, R.; Slowik, J. G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prévôt, A. S. H.; Jayne, J. T.; Favez, O.

    2015-12-01

    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall - early-winter period (November-December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some

  13. Characterization of near-highway submicron aerosols in New York City with a high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Lin, Y.-C.; Ng, N. L.; Jayne, J.; Massoli, P.; Williams, L. R.; Demerjian, K. L.

    2012-02-01

    Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML), equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE) - a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1) species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz) of gaseous pollutants (e.g. HCHO, NO2, NO, O3, and CO2, etc.), black carbon (BC), and particle number concentrations and size distributions. Particulate organics varied dramatically during periods with high traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA), a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate) and oxygenated OA (OOA) showed much smoother variations indicating minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60%) with HOA accounting for a major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ∼120 nm and 500 nm (vacuum aerodynamic diameter, Dva), respectively. OOA and inorganic species appear to be

  14. 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

  15. 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.

  16. A study of summer and winter highly time-resolved submicron aerosol composition measured at a suburban site in Prague

    NASA Astrophysics Data System (ADS)

    Kubelová, Lucie; Vodička, Petr; Schwarz, Jaroslav; Cusack, Michael; Makeš, Otakar; Ondráček, Jakub; Ždímal, Vladimír

    2015-10-01

    The variability of aerosol chemical composition and the impact of the origin of respective air masses were studied in high time resolution for selected periods of high and low levels of aerosol burden at a suburban station in Prague-Suchdol, Czech Republic in summer and winter. Ambient aerosol measurements were performed using the compact-Time of Flight-Aerosol Mass Spectrometer (c-ToF-AMS) and variations in concentration of the main species are discussed. The average mass concentrations for the main species were (summer; winter): organic matter (4.2 μg/m3; 8.4 μg/m3), SO42- (2.0 μg/m3; 4.4 μg/m3), NH4+ (1.2 μg/m3; 2.8 μg/m3), NO3- (0.8 μg/m3; 5.4 μg/m3) and Cl- (0.1 μg/m3; 0.23 μg/m3). We found an inverse relationship between non-refractory submicron particulate matter (NR-PM1) levels and the boundary layer height, mainly in winter. Furthermore, levels of pollution were influenced by the air mass origin, where cleaner maritime air masses resulted in lower aerosol levels compared to those of continental origin. Analysis of the diurnal variation of NR-PM1 showed minimum concentrations in the afternoon caused by dilution as a result of an increase in the boundary layer height. Most maximum concentrations of the main species occurred in the morning or night except sulphate which had a midday maximum, probably due to downdraft from upper boundary layer air and photochemical formation in the afternoon.

  17. Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in Downtown Atlanta, Georgia

    NASA Astrophysics Data System (ADS)

    Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

    2013-12-01

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was recently developed to provide long-term real-time continuous measurements of ambient non-refractory (i.e., organic, sulfate, ammonium, nitrate, and chloride) submicron particulate matter (NR-PM1). Currently, there are a limited number of field studies that evaluate the long-term performance of the ACSM against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. The collocated measurements included a second ACSM, continuous and integrated sulfate, nitrate, and ammonium measurements, as well as a semi-continuous Sunset organic carbon/elemental carbon (OC/EC) analyzer, continuous tapered element oscillating microbalance (TEOM), 24 h integrated Federal Reference Method (FRM) filters, and continuous scanning electrical mobility system-mixing condensation particle counter (SEMS-MCPC). Intercomparison of the two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21); mass concentration for all chemical species agreed within ±27%, indicating that ACSM instruments are capable of stable and reproducible operation. Chemical constituents measured by the ACSM are also compared with those obtained from the continuous measurements from JST. Since the continuous measurement concentrations are adjusted to match the integrated filter measurements, these comparisons reflect the combined uncertainties of the ACSM, continuous, and filter measurements. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Differences between ACSM mass concentrations and the filter-adjusted JST continuous data are 5-27%, 4

  18. The impact of relative humidity on aerosol composition and evolution processes during wintertime in Beijing, China

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Wang, Zifa; Fu, Pingqing; Jiang, Qi; Yang, Ting; Li, Jie; Ge, Xinlei

    2013-10-01

    Non-refractory submicron aerosol (NR-PM1) species measured by an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) along with collocated gaseous species are used to investigate the impacts of relative humidity (RH) on aerosol composition and evolution processes during wintertime in Beijing, China. Aerosol species exhibit strong, yet different RH dependence between low and high RH levels. At low RH levels (<50%), all aerosol species increase linearly as a function of RH, among which organics present the largest mass increase rate at 11.4 μg m-3/10% RH. Because the particle liquid water predicted by E-AIM model is very low and the temperature is relatively constant, the enhancement of aerosol species is primarily due to the decrease of wind speed. While the rates of increase for most aerosol species are reduced at high RH levels (>50%), sulfate presents an even faster increasing rate, indicating the significant impact of liquid water on sulfate production. The RH dependence of organic aerosol (OA) components is also quite different. Among OA components, coal combustion OA (CCOA) presents the largest enhancement in both mass concentration and contribution as a function of RH. Our results elucidate the important roles of liquid water in aerosol processing at elevated RH levels, in particular affecting sulfate and CCOA via aqueous-phase reaction and gas-particle partitioning associated with water uptake, respectively. It is estimated that aqueous-phase processing can contribute more than 50% of secondary inorganic species production along with an increase of aerosol particle acidity during the fog periods. However, it appears not to significantly enhance secondary organic aerosol (SOA) formation and the oxidation degree of OA.

  19. Continuous measurements at the urban roadside in an Asian megacity by Aerosol Chemical Speciation Monitor (ACSM): particulate matter characteristics during fall and winter seasons in Hong Kong

    NASA Astrophysics Data System (ADS)

    Sun, C.; Lee, B. P.; Huang, D.; Jie Li, Y.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.

    2016-02-01

    Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 on the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found to be dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear mealtime concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during mealtimes, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and the influence of continental air masses.

  20. Continuous measurements at the urban roadside in an Asian Megacity by Aerosol Chemical Speciation Monitor (ACSM): particulate matter characteristics during fall and winter seasons in Hong Kong

    NASA Astrophysics Data System (ADS)

    Sun, C.; Lee, B. P.; Huang, D.; Li, Y. J.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.

    2015-07-01

    Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 at the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear meal-time concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during meal times, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a~lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and influence of continental air masses.

  1. Aged organic aerosol in the Eastern Mediterranean: the Finokalia aerosol measurement experiment-2008

    NASA Astrophysics Data System (ADS)

    Hildebrandt, L.; Engelhart, G. J.; Mohr, C.; Kostenidou, E.; Lanz, V. A.; Bougiatioti, A.; Decarlo, P. F.; Prévôt, A. S. H.; Baltensperger, U.; Mihalopoulos, N.; Donahue, N. M.; Pandis, S. N.

    2010-01-01

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

  2. Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment - 2008

    NASA Astrophysics Data System (ADS)

    Hildebrandt, L.; Engelhart, G. J.; Mohr, C.; Kostenidou, E.; Lanz, V. A.; Bougiatioti, A.; Decarlo, P. F.; Prevot, A. S. H.; Baltensperger, U.; Mihalopoulos, N.; Donahue, N. M.; Pandis, S. N.

    2010-05-01

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

  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. Characterization of near-highway submicron 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.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Lin, Y.-C.; Ng, N. L.; Jayne, J.; Massoli, P.; Williams, L. R.; Demerjian, K. L.

    2011-11-01

    Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML), equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE) - a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1) species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz) of gaseous pollutants (e.g., HCHO, NO2, NO, O3, and CO2, etc.), black carbon (BC), and particle number concentrations and size distributions. The particulate organics varied dramatically during periods with highest traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA), a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate) and oxygenated OA (OOA) showed much smoother variations - with minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60%) with HOA being the major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ~120 nm and 500 nm (vacuum aerodynamic diameter, Dva), respectively. OOA and inorganic species appear to be

  5. 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

  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. Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in downtown Atlanta, Georgia

    NASA Astrophysics Data System (ADS)

    Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

    2014-07-01

    Currently, there are a limited number of field studies that evaluate the long-term performance of the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. Intercomparison of two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21) indicating that ACSM instruments are capable of stable and reproducible operation. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the filter-adjusted continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Correlations of the ACSM NR-PM1 (non-refractory particulate matter with aerodynamic diameter less than or equal to 1 μm) plus elemental carbon (EC) with tapered element oscillating microbalance (TEOM) PM2.5 and Federal Reference Method (FRM) PM1 mass are strong with r2 > 0.7 and r2 > 0.8, respectively. Discrepancies might be attributed to evaporative losses of semi-volatile species from the filter measurements used to adjust the collocated continuous measurements. This suggests that adjusting the ambient aerosol continuous measurements with results from filter analysis introduced additional bias to the measurements. We also recommend to calibrate the ambient aerosol monitoring instruments using aerosol standards rather than gas-phase standards. The fitting approach for ACSM relative ionization for sulfate was shown to improve the comparisons between ACSM and collocated measurements in the absence of calibrated values, suggesting the importance of adding sulfate calibration into the ACSM calibration routine.

  8. The role of anthropogenic species in Biogenic aerosol formation

    EPA Science Inventory

    Isoprene is a widely recognized source of organic aerosol in the southeastern United States. Models have traditionally represented isoprene-derived aerosol as semivolatile species formed from the initial isoprene + OH reaction. Recent laboratory and field studies indicate later g...

  9. Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

    NASA Astrophysics Data System (ADS)

    Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Henne, S.; Herrmann, E.; Gysel, M.; Steinbacher, M.; Baltensperger, U.; Prévôt, A. S. H.

    2015-07-01

    Chemically resolved (organic, nitrate, sulphate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high altitude site Jungfraujoch (3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations shows that the highest (especially sulphate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence enabling the assessment of the composition for each. Most nitrate and part of the OA is injected from the regional PBL while sulphate is mainly produced in the FT. The south/north gradient of sulphate is also pronounced in FT air masses (sulphate mass fraction from the south: 45 %, from

  10. Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

    NASA Astrophysics Data System (ADS)

    Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Croteau, P. L.; Gysel, M.; Henne, S.; Herrmann, E.; Jayne, J. T.; Steinbacher, M.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

    2015-10-01

    Chemically resolved (organic, nitrate, sulfate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high-altitude site Jungfraujoch (JFJ; 3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations show that the highest (especially sulfate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ, while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long-range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small-scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence, enabling the assessment of the composition for each. Most nitrate and part of the OA are injected from the regional PBL, while sulfate is mainly produced in the FT. The south/north gradient of sulfate is also pronounced in FT air masses (sulfate mass fraction from the south: 45

  11. Time- and size-resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes

    NASA Astrophysics Data System (ADS)

    Zhang, Qi; Canagaratna, Manjula R.; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis

    2005-04-01

    An Aerodyne aerosol mass spectrometer (AMS) was deployed at the Pittsburgh Environmental Protection Agency Supersite from 7 to 22 September 2002 as part of the Pittsburgh Air Quality Study (PAQS). The main objectives of this deployment were to characterize the concentrations, size distributions, and temporal variations of nonrefractory (NR) chemical species in submicron particles (approximately PM1) and to further develop and evaluate the AMS. Reasonably good agreement was observed on particle concentrations, composition, and size distributions between the AMS data and measurements from collocated instruments (given the difference between the PM1 and PM2.5 size cuts), including TEOM, semicontinuous sulfate, 2-hour- and 24-hour-averaged organic carbon, SMPS, 4-hour-averaged ammonium, and micro-orifice uniform deposit impactor. Total NR-PM1 mass concentration in Pittsburgh accumulates over periods of several days punctuated with rapid cleaning due to rain or air mass changes. Sulfate and organics are the major NR-PM1 components while the concentrations of nitrate and chloride are generally low. Significant amounts of ammonium, which most of the time are consistent with sulfate present as ammonium sulfate, are also present in particles. However, there are periods when the aerosols are relatively acidic and more than 50% of sulfate is estimated to be in the form of ammonium bisulfate. No major enhancement of the organic concentration is observed during these acidic periods, which suggests that acid-catalyzed SOA formation was not an important process during this study. Size distributions of particulate sulfate, ammonium, organics, and nitrate vary on timescales of hours to days, showing unimodal, bimodal and even trimodal characteristics. The accumulation mode (peaking around 350-600 nm in vacuum aerodynamic diameter for the mass distributions) and the ultrafine mode (<100 nm) are observed most frequently. The accumulation mode is dominated by sulfate that appears to

  12. 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

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

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2010-12-01

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

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

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2011-06-01

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

  15. The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition

    NASA Astrophysics Data System (ADS)

    Docherty, K. S.; Aiken, A. C.; Huffman, J. A.; Ulbrich, I. M.; Decarlo, P. F.; Sueper, D.; Worsnop, D. R.; Snyder, D. C.; Grover, B. D.; Eatough, D. J.; Goldstein, A. H.; Ziemann, P. J.; Jimenez, J. L.

    2011-02-01

    Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate sources and chemical composition of fine particles (PMf) in the inland region of Southern California. This paper briefly summarizes the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July-15 August) and provides detailed intercomparisons of complementary measurements and average PMf composition during this period. Daily meteorology and gas-phase species concentrations were highly repetitive with meteorological and gas-phase species concentrations displaying clear diurnal cycles and weekday/weekend contrast, with organic aerosol (OA) being the single largest component contributing approximately one-third of PMf mass. In contrast with historical characterizations of OA in the region, several independent source apportionment efforts attributed the vast majority (~80%) of OA mass during SOAR-1 to secondary organic aerosol (SOA). Given the collocation of complementary aerosol measurements combined with a dominance of SOA during SOAR-1, this paper presents new results on intercomparisons among several complementary measurements and on PMf composition during this period. Total non-refractory submicron (NR-PM1) measurements from a high-resolution aerosol mass spectrometer (HR-AMS) are compared with measurements by tapered element oscillating microbalances (TEOM) including a filter dynamics measurement system (TEOMFDMS). NR-PM1 is highly correlated with PM2.5 TEOMFDMS measurements and accounts for the bulk of PM2.5 mass with the remainder contributed primarily by refractory material. In contrast, measurements from a heated TEOM show substantial losses of semi-volatile material, including ammonium nitrate and semi-volatile organic material. Speciated HR-AMS measurements are also consistent and highly correlated with several complementary measurements, including those of a collocated compact AMS

  16. 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

  17. Results and code predictions for ABCOVE (aerosol behavior code validation and evaluation) aerosol code validation: Test AB6 with two aerosol species. [LMFBR

    SciTech Connect

    Hilliard, R K; McCormack, J C; Muhlestein, L D

    1984-12-01

    A program for aerosol behavior code validation and evaluation (ABCOVE) has been developed in accordance with the LMFBR Safety Program Plan. The ABCOVE program is a cooperative effort between the USDOE, the USNRC, and their contractor organizations currently involved in aerosol code development, testing or application. The second large-scale test in the ABCOVE program, AB6, was performed in the 850-m/sup 3/ CSTF vessel with a two-species test aerosol. The test conditions simulated the release of a fission product aerosol, NaI, in the presence of a sodium spray fire. Five organizations made pretest predictions of aerosol behavior using seven computer codes. Three of the codes (QUICKM, MAEROS and CONTAIN) were discrete, multiple species codes, while four (HAA-3, HAA-4, HAARM-3 and SOFIA) were log-normal codes which assume uniform coagglomeration of different aerosol species. Detailed test results are presented and compared with the code predictions for seven key aerosol behavior parameters.

  18. 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

  19. Photoreactivity of condensed species on Titan's aerosols analogues

    NASA Astrophysics Data System (ADS)

    Fleury, Benjamin; Gudipati, Murthy; Carrasco, Nathalie

    2016-10-01

    Titan's aerosols formation is initiated in the upper atmospheric layers at about 1000 km by the dissociation and the ionization of N2 and CH4 by the VUV solar photons [1]. Then, they aggregate and sediment to the surface. The temperatures of the stratosphere and the troposphere [3] (measured by the HASI instrument onboard the Huygens probe [2]) allow the condensation of many volatile organics on the solid aerosols, forming organic ice coating on the aerosol polymers. We will present an experimental study simulating this process and discuss the photoreactivity of condensed species on Titan's aerosols analogues in the atmosphere and on the surface. We demonstrated experimentally that the organic aerosols, which cover the Titan's surface, drive the photoreactivity of condensed species such as acetylene when they are irradiated with long wavelength photons (λ > 300 nm). This result highlights that Titan's surface remains active despite the absorption of the most energetic photons by the atmosphere.AcknowledgmentsThis work is supported by NASA Solar System Workings grant " Photochemistry in Titan's Lower Atmosphere". The research work has been carried out at the Jet Propulsion Laboratory, California Institute of Technology under a contract with the National Aeronautics and Space Administration. NC acknowledges the European Research Council for their financial support (ERC Starting Grant PRIMCHEM, grant agreement n°636829).References[1] Waite, J. H., et al., The process of Tholin formation in Titan's upper atmosphere, (2007), Science 316, 870-875.[2] Fulchignoni, M., et al., In situ measurements of the physical characteristics of Titan's environment, (2005), Nature 438, 785-791[3] Lavvas, P., et al., Condensation in Titan's atmosphere at the Huygens landing site, (2011), Icarus 215, 732-750.

  20. Condensational growth and trace species scavenging in stratospheric sulfuric acid/water aerosol droplets

    NASA Technical Reports Server (NTRS)

    Tompson, Robert V., Jr.

    1991-01-01

    Stratospheric aerosols play a significant role in the environment. The composition of aerosols is believed to be a liquid solution of sulfuric acid and water with numerous trace species. Of these trace species, ozone in particular was recognized as being very important in its role of shielding the environment from harmful ultraviolet radiation. Also among the trace species are HCl and ClONO2, the so called chlorine reservoir species and various oxides of nitrogen. The quantity of stratospheric aerosol and its particle size distribution determines, to a large degree, the chemistry present in the stratosphere. Aerosols experience 3 types of growth: nucleation, condensation, and coagulation. The application of condensation investigations to the specific problem of stratospheric aerosols is discussed.

  1. An aerosol climatology for a rapidly growing arid region (southern Arizona): Major aerosol species and remotely sensed aerosol properties

    PubMed Central

    Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.

    2014-01-01

    This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March–May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls. PMID:24707452

  2. Characteristics of Carbonaceous and Ionic Species and Direct Aerosol Forcing of the Aerosols over Gosan, Jeju, Korea

    NASA Astrophysics Data System (ADS)

    Kim, N.; Kim, Y.; Kang, C.

    2010-12-01

    Geophysical Research, 109, D21201, doi:10.1029/2004JD004945. Khan, A.J. , Li, J., Dutkiewicz, V.A., and Husain, L. (2010) Elemental carbon and sulfate aerosols over a rural mountain site in the northeastern United States: Regional emissions and implications for climate change, Atmospheric Environment, 44, 2364-2371. Kim, N.K., Park, H.-J., and Kim, Y.P. (2009) Chemical composition change in TSP due to dust storm at Gosan, Korea: Do the concentrations of anthropogenic species increase due to dust storm?, Water, Air, & Soil Pollution, 204, 165-175.

  3. Outdoor and indoor aerosol size, number, mass and compositional dynamics at an urban background site during warm season

    NASA Astrophysics Data System (ADS)

    Talbot, N.; Kubelova, L.; Makes, O.; Cusack, M.; Ondracek, J.; Vodička, P.; Schwarz, J.; Zdimal, V.

    2016-04-01

    This paper describes the use of a unique valve switching system that allowed for high temporal resolution indoor and outdoor data to be collected concurrently from online C-ToF-AMS, SMPS and OC/EC, and offline BLPI measurements. The results reveal near real-time dynamic aerosol behaviour along a migration path from an outdoor to indoor environment. An outdoor reduction in NR-PM1 mass concentration occurred daily from AM (06:00-12:00) to PM (12:00-18:00). SO4 (26%-37%) [AM/PM] increased proportionally during afternoons at the expense of NO3 (18%-7%). The influences of mixing height, temperature and solar radiation were considered against the mean mass concentration loss for each species. Losses were then calculated according to species via a basic input/output model. NO3 lost the most mass during afternoon periods, which we attribute to the accelerated dissociation of NH4NO3 through increasing temperature and decreasing relative humidity. Indoor/outdoor (I/O) ratios varied from 0.46 for <40 nm to 0.65 for >100 nm. These ratios were calculated using average SMPS PNC measurements over the full campaign and corroborated using a novel technique of calculating I/O penetration ratios through the indoor migration of particles during a new particle formation event. This ratio was then used to observe changes in indoor composition relative to those outdoors. Indoor sampling was carried out in an undisturbed room with no known sources. Indoor concentrations were found to be proportional to those outdoors, with organic matter [2.7 μg/m3] and SO4 [1.7 μg/m3] being the most prominent species. These results are indicative of fairly rapid aerosol penetration, a source-free indoor environment and small afternoon I/O temperature gradients. Fine fraction NO3 was observed indoors in both real-time AMS PM1 and off-line BLPI measurements. Greater mass concentration losses were observed from filter measurements, highlighting an important time dependency factor when investigating semi

  4. The Effect of Inlet Aspiration of Aerosol Odd-nitrogen Species on NOy Budget Determination.

    NASA Astrophysics Data System (ADS)

    Knapp, D. J.; Rogers, D. C.; Weinheimer, A. J.; Montzka, D.; Flocke, F. M.; Zheng, W.; Wennberg, P.; Crounse, J.; McCabe, D.; Decarlo, P.; Dunlea, E.; Aiken, A.; Jimenez, J.; Blake, D.

    2007-12-01

    During the MILAGRO/MIRAGE-MEX campaign in March 2006, the NCAR chemiluminescence NOx, NOy, O3 instrument was flown aboard the NSF C-130 in and around the Mexico City Metropolitan Area (MCMA) to sample the urban pollution plume. The NOy instrument sampled ambient air from an aft-facing inlet extended on a pylon from the bottom of the aircraft, in a continuously aspirated flow of about 1 SLM. The sample flow entrained small aerosols which is understood from a practical perspective, but until this time had not been quantified for this inlet configuration. During flights close to MCMA, relatively high values of ammonium nitrate aerosol (5.2 ppbv equivalent mixing ratio) were measured by the University of Colorado AMS instrument coincidently with high NOy readings (5.5 ppbv) from the NCAR NOy instrument. Subsequent analysis of the NOy partitioning resulted in a component NOy deficiency of 15 - 40 percent, based on independent but concomitantly measured major NOy species: NOx, PANs, HNO3, alkyl nitrates and aerosol NH4NO3. The aspiration efficiency of small aerosols from the NOy inlet was modeled using the Fluent aerodynamic model. The amount of aerosol NH4NO3 and HNO3 on fine dust were calculated based on the determined aspiration efficiencies for a range of aerosol masses, and the potential contribution of these species to the NOy budget was determined. Systematic aspiration of an unknown amount of these aerosols may at least partially explain historic examples of missing NOy.

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

    NASA Astrophysics Data System (ADS)

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

    2005-07-01

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

  6. Local and remote impacts of aerosol species on Indian summer monsoon rainfall in a GCM

    NASA Astrophysics Data System (ADS)

    Guo, Liang; Turner, Andrew; Highwood, Eleanor

    2016-04-01

    The HadGEM2 AGCM is used to determine the most important anthropogenic aerosols in the Indian monsoon using experiments in which observed trends in individual aerosol species are imposed. Sulphur dioxide (SD) emissions are shown to impact rainfall more strongly than black carbon (BC) aerosols, causing reduced rainfall especially over northern India. Significant perturbations due to BC are not noted until its emissions are scaled up in a sensitivity test, in which rainfall increases over northern India as a result of the Elevated Heat Pump mechanism, enhancing convection during the pre-monsoon and bringing forward the monsoon onset. Secondly, the impact of anthropogenic aerosols is compared to that of increasing greenhouse-gas concentrations and observed sea-surface temperature (SST) warming. The tropospheric temperature gradient driving the monsoon shows weakening when forced by either SD or imposed SST trends. However the observed SST trend is dominated by warming in the deep tropics; when the component of SST trend related to aerosol emissions is removed, further warming is found in the extratropical northern hemisphere that tends to offset monsoon weakening. This suggests caution is needed when using SST forcing as a proxy for greenhouse warming. Finally, aerosol emissions are decomposed into those from the Indian region and those elsewhere, in pairs of experiments with SD and BC. Both local and remote aerosol emissions are found to lead to rainfall changes over India; for SD, remote aerosols contribute around 75% of the rainfall decrease over India, while for BC the remote forcing is even more dominant.

  7. Aerosol-halogen interaction: Change of physico-chemical properties of SOA by naturally released halogen species

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Krüger, H.; Platt, U.; Schmitt-Kopplin, P.; Zetzsch, C.

    2011-12-01

    Reactive halogen species are released by various sources like photo-activated sea-salt aerosol or salt pans and salt lakes. These heterogeneous release mechanisms have been overlooked so far, although their potential of interaction with organic aerosols like Secondary Organic Aerosol (SOA), Biomass Burning Organic Aerosol (BBOA) or Atmospheric Humic LIke Substances (HULIS) is completely unknown. Such reactions can constitute sources of gaseous organo-halogen compounds or halogenated organic particles in the atmospheric boundary layer. To study the interaction of organic aerosols with reactive halogen species (RHS), SOA was produced from α-pinene, catechol and guaiacol using an aerosol smog-chamber. The model SOAs were characterized in detail using a variety of physico-chemical methods (Ofner et al., 2011). Those aerosols were exposed to molecular halogens in the presence of UV/VIS irradiation and to halogens, released from simulated natural halogen sources like salt pans, in order to study the complex aerosol-halogen interaction. The heterogeneous reaction of RHS with those model aerosols leads to different gaseous species like CO2, CO and small reactive/toxic molecules like phosgene (COCl2). Hydrogen containing groups on the aerosol particles are destroyed to form HCl or HBr, and a significant formation of C-Br bonds could be verified in the particle phase. Carbonyl containing functional groups of the aerosol are strongly affected by the halogenation process. While changes of functional groups and gaseous species were visible using FTIR spectroscopy, optical properties were studied using Diffuse Reflectance UV/VIS spectroscopy. Overall, the optical properties of the processed organic aerosols are significantly changed. While chlorine causes a "bleaching" of the aerosol particles, bromine shifts the maximum of UV/VIS absorption to the red end of the UV/VIS spectrum. Further physico-chemical changes were recognized according to the aerosol size-distributions or the

  8. Effects of aerosol species on atmospheric visibility in Kaohsiung City, Taiwan

    SciTech Connect

    Chang-Gai Lee; Chung-Shin Yuan; Jui-Cheng Chang; Ching Yuan

    2005-07-01

    Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During the study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition of Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 {mu}m, corresponding with the wavelength region of visible light, which accounted for {approximately} 72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH{sub 4}){sup 2}SO{sub 4}, NH{sub 4}NO{sub 3}, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein. 35 refs., 10 figs., 4 tabs.

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  10. Soluble species in the Arctic summer troposphere - acidic gases, aerosols, and precipitation

    SciTech Connect

    Talbot, R.W.; Vijgen, A.S.; Harriss, R.C. Old Dominion Univ., Norfolk, VA )

    1992-10-01

    The large-scale spatial distribution from 0.15-to 6 km altitude in the North American Arctic troposphere of several soluble acidic gases and major aerosol species during the summertime is reported. The distribution is found to be compositionally consistent on a large spatial scale. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases while acidic sulfate aerosols dominate the particulate phase. There appears to be a surface source of NH3 over the pack ice which may originate from decay of dead marine organisms on the ice surface, evolution from surface ocean waters in open ice leads, or release from rotting sea ice. At low altitude over the pack ice this NH34 appears to partially neutralize aerosol acidity. Over sub-Arctic tundra in southeastern Alaska, inputs of marine biogenic sulfur from the Bering Sea appear to be an important source of boundary layer aerosol SO4(2-). The rainwater acidity over the tundra is typical of remote regions. 61 refs.

  11. Soluble species in the Arctic summer troposphere - Acidic gases, aerosols, and precipitation

    NASA Technical Reports Server (NTRS)

    Talbot, R. W.; Vijgen, A. S.; Harriss, R. C.

    1992-01-01

    The large-scale spatial distribution from 0.15-to 6 km altitude in the North American Arctic troposphere of several soluble acidic gases and major aerosol species during the summertime is reported. The distribution is found to be compositionally consistent on a large spatial scale. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases while acidic sulfate aerosols dominate the particulate phase. There appears to be a surface source of NH3 over the pack ice which may originate from decay of dead marine organisms on the ice surface, evolution from surface ocean waters in open ice leads, or release from rotting sea ice. At low altitude over the pack ice this NH34 appears to partially neutralize aerosol acidity. Over sub-Arctic tundra in southeastern Alaska, inputs of marine biogenic sulfur from the Bering Sea appear to be an important source of boundary layer aerosol SO4(2-). The rainwater acidity over the tundra is typical of remote regions.

  12. Experiment to Characterize Aircraft Volatile Aerosol and Trace-Species Emissions (EXCAVATE)

    NASA Technical Reports Server (NTRS)

    Anderson, B. E.; Branham, H.-S.; Hudgins, C. H.; Plant, J. V.; Ballenthin, J. O.; Miller, T. M.; Viggiano, A. A.; Blake, D. R.; Boudries, H.; Canagaratna, M.

    2005-01-01

    The Experiment to Characterize Aircraft Volatile and Trace Species Emissions (EXCAVATE) was conducted at Langley Research Center (LaRC) in January 2002 and focused upon assaying the production of aerosols and aerosol precursors by a modern commercial aircraft, the Langley B757, during ground-based operation. Remaining uncertainty in the postcombustion fate of jet fuel sulfur contaminants, the need for data to test new theories of particle formation and growth within engine exhaust plumes, and the need for observations to develop air quality models for predicting pollution levels in airport terminal areas were the primary factors motivating the experiment. NASA's Atmospheric Effects of Aviation Project (AEAP) and the Ultra Effect Engine Technology (UEET) Program sponsored the experiment which had the specific objectives of determining ion densities; the fraction of fuel S converted from S(IV) to S(VI); the concentration and speciation of volatile aerosols and black carbon; and gas-phase concentrations of long-chain hydrocarbon and PAH species, all as functions of engine power, fuel composition, and plume age.

  13. Daily variation of organic aerosol concentration and composition in Seoul, Korea during KORUS pre-campaign

    NASA Astrophysics Data System (ADS)

    Shin, H. J.; Lee, J.; Choi, A. Y.; Park, S. M.; Park, J. S.; Song, I. H.; Hong, Y. D.

    2015-12-01

    Daily variation of Organic Aerosol (OA) as well as organic tracer compounds have been observed in aerosol samples collected during KORUS-AQ (Korea-US Air Quality Study) pre-campaign (From May 18 to June 12) in Seoul, Korea. NR-PM1 bounded OA was measured by HR-TOF-AMS (Aerodyne) and the temporal variation, composition of OA by family group characterization, and oxidation state of OA was studied. And to distinguish the source characteristics (such as HOA, COA, NOA, SV-OOA, LV-OOA, etc…) of the organic, AMS-PMF model will be used.For the observation of organic tracer compounds, solvent extractable fractions were analyzed by GC-MS. More than 80 organic compounds were detected in the aerosol samples and grouped by source characterized classes, including vehicular emission tracers, biomass burning tracers, coal emission tracers, secondary organic aerosol (SOA) tracers. The main objective of this study is evaluation of the validity of OA fractionation based on the AMS measurement. So, we will compare daily variation of OA composition measured by AMS with daily variation of organic tracer compounds. Further, we will specify source characteristics estimated using AMS-PMF model by comparing the results of source apportionment of OA using PMF of organic tracer compounds.

  14. Soluble species in the Arctic summer troposphere: Acidic gases, aerosols, and precipitation

    NASA Astrophysics Data System (ADS)

    Talbot, R. W.; Vijgen, A. S.; Harriss, R. C.

    1992-10-01

    We report here the distribution of selected acidic gases and aerosol species in the North American Arctic and sub-Arctic summer troposphere. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases and acidic sulfate aerosols dominating the particulate phase. Our data show that the acidic gas and aerosol composition is uniform on a large spatial scale. There appears to be a surface source of NH4+ over the Arctic Ocean pack ice which may reflect release of NH3 from decay of dead marine organisms on the ice surface near ice leads, release from rotting sea ice, or an upward flux from surface ocean waters in open ice leads. This NH3 appears to partially neutralize aerosol acidity in the boundary layer. Over sub-Arctic tundra in southwestern Alaska inputs of marine biogenic sulfur from the nearby Bering Sea appear to be an important source of boundary layer aerosol SO42-. While there were only minor effects on aerosol chemistry over the tundra from sea salt, the rainwater chemistry showed influence from marine aerosols which were apparently incorporated into air masses during frontal passages moving inland from the Bering Sea. The rainwater acidity over the tundra (pH 4.69) is typical of remote regions. The principal acidity components are H2SO4 and carboxylic acids, especially HCOOH. The carboxylic acids appear to have a strong continental biogenic source, but hydrocarbons of marine origin and emissions from forest fires may also be important. The wet deposition fluxes of NO3--N and SO42--S over sub-Arctic tundra during July-August 1988 were 2.1 and 2.4 mmol m-2 yr-1. Wet deposition of NO3- was nearly 3 times higher than the average NOy deposition flux, which is believed to represent primarily dry deposition of HNO3 (Bakwin et al., this issue). Our measurements indicate that the mid-troposphere in the Arctic is generally contaminated with low levels of anthropogenic pollutants even in summer when direct atmospheric coupling

  15. 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

  16. Measurements of trace gas species and aerosols at three Siberian stations

    NASA Astrophysics Data System (ADS)

    Arshinov, Mikhail Yu.; Belan, Boris D.; Davydov, Denis K.; Kozlov, Artem V.; Ivlev, Georgii A.; Pestunov, Dmitrii A.; Tolmachev, Gennadii N.; Fofonov, Alexander V.

    2014-05-01

    Siberia is of great importance to understand the climate change due to it covers about 10% of Earth's land surface and it has the largest area to be studied under the Pan-Eurasian Experiment (PEEX). In the overview done by Kulmala et al. (2011) authors arrived at a conclusion that continuous and comprehensive measurements of GHGs and aerosols over Siberia are still lacking. Understanding the importance of this problem, in recent years the Institute of Atmospheric Optics SB RAS established several monitoring stations for continuous measurements of aerosol and trace gas species to fill up this gap. In this paper we present some results of continuous measurements of trace gas species and aerosols carried out at three stations located in West Siberia. The first one is a so-called TOR-station located in the scientific campus of Tomsk (56° 28'41"N, 85° 03'15"E), the second one is the Base Experimental Complex (BEC, 56° 28'49"N, 85° 06'08"E) - in the eastern suburbs of Tomsk, and the third one is Fonovaya Observatory (56° 25'07"N, 84° 04'27"E) - in a rural area 60 km west of Tomsk. All equipment of the stations is fully automated and can be monitored via Internet. Gas analyzers are hourly calibrated against standard gas mixtures, micro-flux gas sources, or gas generators, depending on the instrument type and the gas to be detected. Aerosol measurements carried out continuously from March 2010 enabled a frequency and seasonal dependency of the new particle formation (NPF) events to be revealed. NPF events in Siberia are more often observed during spring (from March to May) and early autumn (secondary frequency peak in September). On average, NPF evens took place on 23-28 % of all days. This work was funded by Presidium of RAS (Program No. 4), Brunch of Geology, Geophysics and Mining Sciences of RAS (Program No. 5), Interdisciplinary integration projects of Siberian Branch of RAS (No. 35, No. 70, No. 131), Russian Foundation for Basic Research (grants No 14

  17. Evaporation Kinetics of Organic Aerosols: Species-wise Measurements and Estimates

    NASA Astrophysics Data System (ADS)

    Zhang, H.; Worton, D. R.; Shen, S.; Nah, T.; Wilson, K. R.; Goldstein, A. H.

    2014-12-01

    A large fraction of atmospheric fine particulate matters (PM2.5) are organic aerosols (OA) that can form from primary emission (primary OA) or oxidation of more volatile organic compounds (secondary OA). Most OA are semi-volatile that can evaporate from particle phase to gas phase. OA evaporation strongly impacts aerosol mass loading, aerosol oxidation state, and aerosol properties in the atmosphere. In this study, we use four semi-volatile long-chain n-alkanes (n-octadecane, n-eicosane, n-docosane, and n-tetracosane) and α-pinene-derived OA as surrogates for primary and secondary OA, respectively. The evaporation of these OA components was examined in a flow reactor. Two soft ionization mass spectrometry techniques were used to measure evaporation kinetics of individual OA constituents: on-line direct analysis in real time-mass spectrometry (DART-MS) (used for secondary OA) and off-line two-dimensional gas chromatograph coupled to a high-resolution time-of-flight mass spectrometer (GC×GC/HTOF-MS) with vacuum ultraviolet (VUV) photoionization (used for primary OA). The semi-volatile n-alkanes can be oxidized in both phases, following different reaction schemes and leading to multigenerational oxygenated products with different isomeric distributions. Here the evaporation kinetic of primary OA surrogates was determined based on chemical analysis and kinetic simulations. The evaporation of α-pinene-derived OA was characterized based on the DART-MS mass spectra change upon heating. Results for both systems suggest slow evaporation compared to the gas-particle partitioning theory, especially when the OA are solid. The species-wise measurements using novel techniques provide insights into the detailed evaporation kinetics for atmospheric relevant systems.

  18. Water-Soluble Organic Species in Biomass Burning Aerosols in Southern Africa: Their Chemical Identification and Spatial Distribution

    NASA Astrophysics Data System (ADS)

    Gao, S.; Hegg, D. A.; Hobbs, P. V.; Kirchstetter, T. W.; Magi, B.

    2001-12-01

    During the SAFARI-2000 field campaign, 14 aerosol samples were collected from an aircraft in plumes from biomass fires (under both flaming and smoldering conditions), at various distances from the fire source. Also collected were 36 aerosol samples in haze layers ranging from the surface to 16,000 feet, some of which could be associated with specific fires. The samples were collected on teflon membrane filters (lower size limit of about 30nm in diameter) which were analyzed for total aerosol mass loading and chemical composition using several analytical techniques. Particular effort was made to speciate the water-soluble portion of the aerosol organics. Seven organic acids and seven carbohydrate species (and their possible stereoisomers) were identified and quantified, along with three inorganic anions and five inorganic cations. The identified organic species accounted for up to 32% of the total aerosol mass; compared with concurrent total carbon and organic carbon measurements, the identified organics constituted at least 5% to 30% of the mass of the total aerosol organics. A number of conspicuous spatial distribution patterns were observed for these species. For instance, using K+ to correct for dilution, it was found that gluconate, oxalate, succinate, and glutarate, along with sulfate and nitrate, all increased significantly in mass concentration from the fire source going downwind. This suggests secondary formation of these species during aerosol aging. On the other hand, formate and acetate showed decreasing trends downwind, probably due to the loss of these volatile species to the gas phase. Another striking pattern is that anhydrosugars (e.g. levoglucosan) had the highest aerosol mass fraction near smoldering fires but a very low fraction in the haze layers, whereas, dicarboxylic acids showed an almost opposite trend. This implies possible chemical reaction processes converting intermediate organic products, such as levoglucosan, to smaller products like

  19. Determination of the passing efficiency for aerosol chemical species through a typical aircraft-mounted, diffuser-type aerosol inlet system

    NASA Astrophysics Data System (ADS)

    Sheridan, Patrick J.; Norton, Richard B.

    1998-04-01

    To assess the particle transmission efficiency of a conventional aircraft-mounted, diffuser-type inlet (CI), a new design inlet containing an internal filter basket assembly (aerosol filter inlet, or AFI) was constructed. All interior surfaces of the AFI were covered with filter material, and air was actively pulled through these filter walls during aerosol sampling. The AFI was demonstrated in the laboratory to trap nearly all particles entering its nozzle orifice, so it was considered usable as a baseline to judge the performance of other inlets. Wind tunnel studies were conducted at three different wind velocities that approximated typical research aircraft speeds. As wind velocity increased, particle transmission through the CI relative to the AFI decreased, as evidenced by chemical analysis of the filter deposits. Aircraft studies of the two inlets showed that particle transmission varied significantly with the measured species. Typical coarse-particle species such as Ca++, Mg++, Na+ and K+ showed 50-90% mass losses through a conventional diffuser-type inlet/curved intake tube system. Predominantly fine particle species such as SO4= and NH4+ passed the CI system with much higher efficiencies, with aerosol mass losses of 0-26% for most flights. Since the AFI traps nearly all particles aspirated into its nozzle orifice, these values indicate that on average, 80-90% of the SO4= and NH4+ aerosol mass passes through the CI and curved intake tube during airborne sampling. This finding suggests that the capability to sample fine (i.e., submicrometer) aerosols from aircraft is perhaps not as bad as has been previously reported, given that adequate attention is paid to inlet design, location, and orientation issues.

  20. Measurement of acidic aerosol species in eastern Europe: implications for air pollution epidemiology.

    PubMed Central

    Brauer, M; Dumyahn, T S; Spengler, J D; Gutschmidt, K; Heinrich, J; Wichmann, H E

    1995-01-01

    A large number of studies have indicated associations between particulate air pollution and adverse health outcomes. Wintertime air pollution in particular has been associated with increased mortality. Identification of causal constituents of inhalable particulate matter has been elusive, although one candidate has been the acidity of the aerosol. Here we report measurements of acidic aerosol species made for approximately 1.5 years in Erfurt, Germany, and Sokolov, Czech Republic. In both locations, the burning of high-sulfur coal is the primary source of ambient air pollution. Twenty-four-hour average measurements were made for PM10, [particulate matter with an aerodynamic diameter (da) < or = 10 microns], as well as fine particle (da < 2.5 microns) H+ and SO4(2-) for the entire study. Additionally, separate day and night measurements of fine particle H+, SO4(2-), NO3-, and NH4+ and the gases, SO2, HNO3, HONO, and NH3 were collected with an annular denuder/filter pack system over a 7-month (late winter-summer) period with additional measurements during pollution episodes the following winter. At both sites, 24-hr SO2 (mean concentrations of 52 micrograms/m3, with peak levels of > 585 micrograms/m3) and PM10 (mean concentration 60 micrograms m3) concentrations were quite high. However, aerosol SO4(2-) concentrations (mean concentration of approximately 10 micrograms/m3) were not as great as expected given the high SO2 concentrations, and acidity was very low (mean concentration of < 1 microgram/m3, with peak levels of only 7 micrograms/m3). Low acidity is likely to be the result of NH3 neutralization and slow conversion of SO2 to SO4(2-).(ABSTRACT TRUNCATED AT 250 WORDS) PMID:7656878

  1. Background error covariance with balance constraints for aerosol species and applications in variational data assimilation

    NASA Astrophysics Data System (ADS)

    Zang, Zengliang; Hao, Zilong; Li, Yi; Pan, Xiaobin; You, Wei; Li, Zhijin; Chen, Dan

    2016-08-01

    Balance constraints are important for background error covariance (BEC) in data assimilation to spread information between different variables and produce balance analysis fields. Using statistical regression, we develop a balance constraint for the BEC of aerosol variables and apply it to a three-dimensional variational data assimilation system in the WRF/Chem model; 1-month forecasts from the WRF/Chem model are employed for BEC statistics. The cross-correlations between the different species are generally high. The largest correlation occurs between elemental carbon and organic carbon with as large as 0.9. After using the balance constraints, the correlations between the unbalanced variables reduce to less than 0.2. A set of data assimilation and forecasting experiments is performed. In these experiments, surface PM2.5 concentrations and speciated concentrations along aircraft flight tracks are assimilated. The analysis increments with the balance constraints show spatial distributions more complex than those without the balance constraints, which is a consequence of the spreading of observation information across variables due to the balance constraints. The forecast skills with the balance constraints show substantial and durable improvements from the 2nd hour to the 16th hour compared with the forecast skills without the balance constraints. The results suggest that the developed balance constraints are important for the aerosol assimilation and forecasting.

  2. Acidic species and chloride depletion in coarse aerosol particles in the US east coast.

    PubMed

    Zhao, Yunliang; Gao, Yuan

    2008-12-15

    To investigate the interactions of water-soluble acidic species associated with coarse mode aerosol particles (1.8-10 microm) and chlorine depletion, ten sets of size-segregated aerosol samples were collected by a 10-stage Micro-Orifice Uniform Deposit Impactor (MOUDI) in Newark, New Jersey on the U.S. east coast. The samples were grouped into two categories according to the air-mass back trajectories and mass ratios of sodium to magnesium and calcium: Group I was primarily impacted by marine air mass and Group II was dominated by the continental air mass. In Group I, the concentrations of coarse mode nitrate and chloride depletion showed a strong correlation (R2=0.88). Without considering other cations, nitrate was found to account for all of the chloride depletion in coarse particles for most samples. The association of coarse mode nitrate with sea-salt particles is favored when the mass ratio of sodium to calcium is approximately equal to or greater than unity. Excess sulfate accounts for a maximum of 33% of chloride depletion in the coarse particles. Regarding chloride depletion in the different particle sizes, excess nitrate and sulfate account for 89% of the chloride depletion in the particle size range of 1.8-3.2 microm in the sample from July 13-14; all of the determined dicarboxylic acids and mono-carboxylic acids cannot compensate for the rest of the chloride depletion. In Group II, high percentages of chloride depletion were not observed. With nitrate being dominant in chlorine depletion observed at this location, N-containing species from pollution emissions may have profound impact on atmospheric composition through altering chlorine chemistry in this region. PMID:18973925

  3. Evaluation of multistep derivatization methods for identification and quantification of oxygenated species in organic aerosol.

    PubMed

    Flores, Rosa M; Doskey, Paul V

    2015-10-30

    Two, 3-step methods for derivatizing mono- and multi-functional species with carbonyl (CO), carboxylic acid (-COOH), and alcohol (-OH) moieties were compared and optimized. In Method 1, the CO, -COOH, and -OH moieties were converted (1) to methyloximes (R-CN-OCH3) with O-methylhydroxylamine hydrochloride (MHA), (2) to methyl esters (OC-R-OCH3) with (trimethylsilyl)diazomethane in methanol (TMSD/MeOH), and (3) to trimethylsilyl ethers [R-OSi(CH3)3] with N,O-bis(trimethylsilyl)-trifluoroacetamide (BSTFA) containing 1% trimethylchlorosilane (TMCS), respectively. Steps 1 and 3 of both methods were identical; however, in Step 2 of Method 2, -COOH moieties were derivatized with 10% (v/v) boron trifluoride (BF3) in MeOH or n-butanol (n-BuOH). The BF3/MeOH and BF3/n-BuOH were ineffective at converting species with more than 2-OH moieties. Average standard deviations for derivatization of 36 model compounds by the 3-step methods using TMSD/MeOH and BF3/(MeOH) were 7.4 and 14.8%, respectively. Average derivatization efficiencies for Methods 1 and 2 were 88.0 and 114%, respectively. Despite the lower average derivatization efficiency of Method 1, distinct advantages included a greater certainty of derivatization yield for the entire suite of mono- and multi-functional species and fewer processing steps for sequential derivatization. Detection limits for Method 1 using GC×GC-ToF-MS were 0.3-54pgm(-3). Approximately 100 oxygenated organic species were identified and quantified in aerosol filtered from 39m(3) of air in an urban location. Levels of species were 0.013-17ngm(-3) and were nearly all above the Method 1 limit of detection. PMID:26427323

  4. Halogen-induced organic aerosol (XOA) formation and decarboxylation of carboxylic acids by reactive halogen species - a time-resolved aerosol flow-reactor study

    NASA Astrophysics Data System (ADS)

    Ofner, Johannes; Zetzsch, Cornelius

    2013-04-01

    Reactive halogen species (RHS) are released to the atmosphere from various sources like photo-activated sea-salt aerosol and salt lakes. Recent studies (Cai et al., 2006 and 2008, Ofner et al., 2012) indicate that RHS are able to interact with SOA precursors similarly to common atmospheric oxidizing gases like OH radicals and ozone. The reaction of RHS with SOA precursors like terpenes forms so-called halogen-induced organic aerosol (XOA). On the other hand, RHS are also able to change the composition of functional groups, e.g. to initiate the decarboxylation of carboxylic acids (Ofner et al., 2012). The present study uses a 50 cm aerosol flow-reactor, equipped with a solar simulator to investigate the time-resolved evolution and transformation of vibrational features in the mid-infrared region. The aerosol flow-reactor is coupled to a home-made multi-reflection cell (Ofner et al., 2010), integrated into a Bruker IFS 113v FTIR spectrometer. The reactor is operated with an inlet feed (organic compound) and a surrounding feed (reactive halogen species). The moveable inlet of the flow reactor allows us to vary reaction times between a few seconds and up to about 3 minutes. Saturated vapours of different SOA precursors and carboxylic acids were fed into the flow reactor using the moveable inlet. The surrounding feed inside the flow reactor was a mixture of zero air with molecular chlorine as the precursor for the formation of reactive halogen species. Using this setup, the formation of halogen-induced organic aerosol could be monitored with a high time resolution using FTIR spectroscopy. XOA formation is characterized by hydrogen-atom abstraction, carbon-chlorine bond formation and later, even formation of carboxylic acids. Several changes of the entire structure of the organic precursor, caused by the reaction of RHS, are visible. While XOA formation is a very fast process, the decarboxylation of carboxylic acids, induced by RHS is rather slow. However, XOA formation

  5. Spatial and temporal variability of ammonia and other inorganic aerosol species

    NASA Astrophysics Data System (ADS)

    Day, D. E.; Chen, X.; Gebhart, K. A.; Carrico, C. M.; Schwandner, F. M.; Benedict, K. B.; Schichtel, B. A.; Collett, J. L.

    2012-12-01

    Nitrogen deposition to the sensitive ecosystems in Rocky Mountain National Park (RMNP) has been increasing. Ammonia has been shown to be a large fraction of this nitrogen deposition, and sources in northeastern Colorado were found to be a significant contributor. In this work we report on the results from a small network of Radiello passive samplers to investigate the temporal and spatial variability of ammonia gas concentrations in northeastern Colorado. A URG denuder/filter-pack sampler was collocated with a Radiello passive sampler to provide a check on the accuracy of passive ammonia measurements and to provide information about complementary aerosol and trace gas species. These measurements showed seasonal variations in the concentrations of both particulate- and gas-phase aerosol components. The highest concentrations of ammonia occurred during summer months. These were almost twice the lowest concentrations, which occurred during spring and fall months. Ammonia also exhibited higher than expected concentrations during winter. There was considerable spatial variability in average ammonia concentrations, with May-August averages ranging from 3 μg m-3 in rural grasslands to 4-11 μg m-3 at suburban-urban sites to almost 30 μg m-3 in an area of intensive livestock feeding and farming operations. The large ammonia gradients near sources are expected for this primary pollutant with high deposition rates. The overall concentrations in this region are significantly larger than those measured in RMNP, which were around 0.5 μg m-3, and represent a large reservoir of ammonia that can be transported to RMNP with easterly winds.

  6. Field Study of Filter Sampling Artifacts for Inorganic and Organic Aerosol Species

    NASA Astrophysics Data System (ADS)

    Maenhaut, W.; Wang, W.; Chi, X.

    2009-12-01

    It is well-known that the collection of carbonaceous aerosols on quartz fibre filters is prone to both positive and negative artifacts (e.g., Turpin et al., 2000). In studies on these artifacts, one normally concentrates on organic carbon (OC) as a whole or occasionally on water-soluble OC (WSOC). It is rare that studies are carried on individual organic species. Examples of the latter type of study are those by Limbeck et al. (2001; 2005), who used a low-volume tandem filter set-up at a rural background site in South Africa and at the urban site Vienna in Austria, and measured dicarboxylic acids (DCAs) on the front and back filters. We conducted a similar study as those of Limbeck et al. (2001; 2005). For our study we collected high-volume PM2.5 samples during summer field campaigns at three European forested sites, i.e., in Hungary, Belgium, and Finland. The front and back filters of our samples were analysed for OC with a thermal-optical transmission technique (Birch & Cary, 1996), for WSOC as described by Viana et al. (2006), and for water-soluble inorganic cationic and anionic species and organic anionic species by suppressed ion chromatography with conductometric detection. The organic species measured included methanesulphonic acid (MSA) and the four major DCAs, i.e., oxalic, malonic, succinic, and glutaric. The median back/front percentage ratios for ammonium and sulphate were low, below 5% and 1%, respectively, but for nitrate they were around 25-30%. That undenuded filter samplings for nitrate are prone to artifacts is well-documented (e.g., Schaap et al., 2004). For OC the median back/front percentage ratios were around 15% and for WSOC around 20%. For MSA and the four DCAs, they increased in the following order: oxalic (1.5%), succinic (3%), MSA (4%), malonic (2-9%), glutaric (7-26%). Our back/front ratios for three of the four DCAs are lower to much lower than these found by Limbeck et al. (2001; 2005); for malonic, however, we found higher back

  7. Climate missing links: Aqueous greenhouse species in clouds, fogs and aerosols

    SciTech Connect

    Gaffney, J.S.; Marley, N.A.; Cunningham, M.M.

    1991-11-01

    Recently, there has been considerable interest regarding possible greenhouse effects due to combustion and energy-related pollution. This concern has been due to the release and secondary production of greenhouse gases such as carbon dioxide, freons, methane, nitrous oxide, and ozone. These gases can absorb infrared radiation as it comes back from the heated ground and therefore effectively trap the infrared radiation in the troposphere, leading to climatic change. Beyond these gases, clouds, aerosols, and fogs may also play important roles in affecting, the radiation balance by scattering incoming radiation. This work describes the measurement of water soluble infrared absorbers that are known to be derived from pollution. Polluted precipitation is likely to be an important contributor to radiation balance that is currently being neglected. Pollutants characterized include sulfate, nitrate, formate, acetate, oxalate, phenol, p-nitrophenol, ammonium, carbonate, bicarbonate, formaldehyde (dihydroxy methane), methanol, and ethanol. Band positions and band strengths have been determined. These species show measurable infrared absorption bands in the atmospheric window regions (i.e., 900--1600 cm{sup {minus}1}). These data are discussed with regard to the reported discrepancies in the radiatively important water infrared absorption region commonly referred to as the ``foreign broadened continuum.``

  8. Organic aerosols associated with the generation of reactive oxygen species (ROS) by water-soluble PM2.5.

    PubMed

    Verma, Vishal; Fang, Ting; Xu, Lu; Peltier, Richard E; Russell, Armistead G; Ng, Nga Lee; Weber, Rodney J

    2015-04-01

    We compare the relative toxicity of various organic aerosol (OA) components identified by an aerosol mass spectrometer (AMS) based on their ability to generate reactive oxygen species (ROS). Ambient fine aerosols were collected from urban (three in Atlanta, GA and one in Birmingham, AL) and rural (Yorkville, GA and Centerville, AL) sites in the Southeastern United States. The ROS generating capability of the water-soluble fraction of the particles was measured by the dithiothreitol (DTT) assay. Water-soluble PM extracts were further separated into the hydrophobic and hydrophilic fractions using a C-18 column, and both fractions were analyzed for DTT activity and water-soluble metals. Organic aerosol composition was measured at selected sites using a high-resolution time-of-flight AMS. Positive matrix factorization of the AMS spectra resolved the organic aerosol into isoprene-derived OA (Isop_OA), hydrocarbon-like OA (HOA), less-oxidized oxygenated OA, (LO-OOA), more-oxidized OOA (MO-OOA), cooking OA (COA), and biomass burning OA (BBOA). The association of the DTT activity of water-soluble PM2.5 (WS_DTT) with these factors was investigated by linear regression techniques. BBOA and MO-OOA were most consistently linked with WS_DTT, with intrinsic water-soluble activities of 151 ± 20 and 36 ± 22 pmol/min/μg, respectively. Although less toxic, MO-OOA was most widespread, contributing to WS_DTT activity at all sites and during all seasons. WS_DTT activity was least associated with biogenic secondary organic aerosol. The OA components contributing to WS_DTT were humic-like substances (HULIS), which are abundantly emitted in biomass burning (BBOA) and include highly oxidized OA from multiple sources (MO-OOA). Overall, OA contributed approximately 60% to the WS_DTT activity, with the remaining probably from water-soluble metals, which were mostly associated with the hydrophilic WS_DTT fraction. PMID:25748105

  9. Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect

    NASA Astrophysics Data System (ADS)

    Wang, Z. L.; Zhang, H.; Zhang, X. Y.

    2015-04-01

    Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in the short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate atmosphere-only model BCC_AGCM2.0.1_CUACE/Aero with prescribed sea surface temperature and sea ice cover, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with recent past year 2000 levels if the emissions of only BC are reduced to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial~for the mitigation of global warming. However, both aerosol negative direct and indirect radiative effects are weakened when BC and its co-emitted species (sulfur dioxide and organic carbon) are simultaneously reduced. Relative to year 2000 levels, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 if the emissions of all these aerosols are decreased to the levels projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

  10. Ion mobility spectrometry-mass spectrometry (IMS-MS) for on- and offline analysis of atmospheric gas and aerosol species

    NASA Astrophysics Data System (ADS)

    Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; Budisulistiorini, Sri H.; Zhang, Haofei; Surratt, Jason D.; Knochenmuss, Richard; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis; Canagaratna, Manjula R.

    2016-07-01

    Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS-MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS-MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI-IMS-MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS-MS signals are consistent with laboratory IMS-MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS-MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS-MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the

  11. Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

    DOE PAGES

    Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; et al

    2016-07-25

    Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambientmore » field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of

  12. An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies

    NASA Astrophysics Data System (ADS)

    Wragg, Francis P. H.; Fuller, Stephen J.; Freshwater, Ray; Green, David C.; Kelly, Frank J.; Kalberer, Markus

    2016-10-01

    The adverse health effects associated with ambient aerosol particles have been well documented, but it is still unclear which aerosol properties are most important for their negative health impact. Some studies suggest the oxidative effects of particle-bound reactive oxygen species (ROS) are potential major contributors to the toxicity of particles. Traditional ROS measurement techniques are labour-intensive, give poor temporal resolution and generally have significant delays between aerosol sampling and ROS analysis. However, many oxidising particle components are reactive and thus potentially short-lived. Thus, a technique to quantify particle-bound ROS online would be beneficial to quantify also the short-lived ROS components. We introduce a new portable instrument to allow online, continuous measurement of particle-bound ROS using a chemical assay of 2'7'-dichlorofluorescein (DCFH) with horseradish peroxidase (HRP), via fluorescence spectroscopy. All components of the new instrument are attached to a containing shell, resulting in a compact system capable of automated continuous field deployment over many hours or days. From laboratory measurements, the instrument was found to have a detection limit of ˜ 4 nmol [H2O2] equivalents per cubic metre (m3) air, a dynamic range up to at least ˜ 2000 nmol [H2O2] equivalents per m3 air and a time resolution of ≤ 12 min. The instrument allows for ˜ 16 h automated measurement if unattended and shows a fast response to changes in concentrations of laboratory-generated oxidised organic aerosol. The instrument was deployed at an urban site in London, and particulate ROS levels of up to 24 nmol [H2O2] equivalents per m3 air were detected with PM2.5 concentrations up to 28 µg m-3. The new and portable Online Particle-bound ROS Instrument (OPROSI) allows fast-response quantification; this is important due to the potentially short-lived nature of particle-bound ROS as well as fast-changing atmospheric conditions

  13. Properties and sources of individual particles and some chemical species in the aerosol of a metropolitan underground railway station

    NASA Astrophysics Data System (ADS)

    Salma, Imre; Pósfai, Mihály; Kovács, Kristóf; Kuzmann, Ernő; Homonnay, Zoltán; Posta, József

    Aerosol samples in PM 10-2.0 and PM 2.0 size fractions were collected on the platform of a metropolitan underground railway station in central Budapest. Individual aerosol particles were studied using atomic force microscopy, scanning electron microscopy and transmission electron microscopy with energy-dispersive X-ray spectrometry and electron diffraction. The bulk aerosol samples were investigated by 57Fe Mössbauer spectroscopy, and they were subjected to chemical speciation analysis for Cr. The particles were classified into groups of iron oxides and iron, carbonates, silicates, quartz and carbonaceous debris. Electron micrographs showed that the Fe-rich particles in the PM 2.0 size fraction typically consisted of aggregates of nano-sized hematite crystals that were randomly oriented, had round shapes and diameters of 5-15 nm. In addition to hematite, a minor fraction of the iron oxide particles also contained magnetite. In addition, the PM 2.0-fraction particles typically had a rugged surface with layered or granular morphologies. Mössbauer spectroscopy suggested that hematite was a major Fe-bearing species in the PM 10-2.0 size fraction; its mass contribution to the Fe was 36%. Further constituents (ferrite, carbides and FeOOH) were also identified. The water soluble amounts of Cr for the underground railway station and city center were similar. In the PM 10-2.0 size fraction, practically all dissolved Cr had an oxidation state of three, which corresponds to ambient conditions. In the PM 2.0 size fraction, however, approximately 7% of the dissolved Cr was present as Cr(VI), which was different from that for the urban aerosol. It is suggested that the increased adverse health effects of aerosol particles in metros with respect to ambient outdoor particles is linked to the differences in the oxidation states, surface properties or morphologies.

  14. "Virtual injector" flow tube method for measuring relative rates kinetics of gas-phase and aerosol species.

    PubMed

    Renbaum-Wolff, Lindsay; Smith, Geoffrey D

    2012-06-28

    A new method for measuring gas-phase and aerosol reaction kinetics is described in which the gas flow, itself, acts as a "virtual injector" continuously increasing the contact time in analogy to conventional movable-injector kinetics techniques. In this method a laser is directed down the length of a flow tube, instantly initiating reaction by photodissociation of a precursor species at every point throughout the flow tube. Key tropospheric reactants such as OH, Cl, NO(3), and O(3) can be generated with nearly uniform concentrations along the length of the flow tube in this manner using 355 nm radiation from the third harmonic of a Nd:YAG laser. As the flow travels down the flow tube, both the gas-phase and particle-phase species react with the photogenerated radicals or O(3) for increasingly longer time before exiting and being detected. The advantages of this method are that (1) any wall loss of gas-phase and particle species is automatically accounted for, (2) the reactions are conducted under nearly pseudo-first-order conditions, (3) the progress of the reaction is followed as a continuous function of reaction time instead of reactant concentration, (4) data collection is quick with an entire decay trace being collected in as little as 1 min, (5) relative rates of several species can be measured simultaneously, and (6) bimolecular rate constants at least as small as k = 10(-17) (cm(3)/molecule)/s, or aerosol uptake coefficients at least as small as γ = 10(-4), can be measured. Using the virtual injector technique with an aerosol chemical ionization mass spectrometer (CIMS) as a detector, examples of gas-phase relative rates and uptake by oleic acid particles are given for OH, Cl, NO(3), and O(3) reactions with most agreeing to within 20% of published values, where available.

  15. Remote sensing of soot carbon - Part 1: Distinguishing different absorbing aerosol species

    NASA Astrophysics Data System (ADS)

    Schuster, G. L.; Dubovik, O.; Arola, A.

    2016-02-01

    We describe a method of using the Aerosol Robotic Network (AERONET) size distributions and complex refractive indices to retrieve the relative proportion of carbonaceous aerosols and free iron minerals (hematite and goethite). We assume that soot carbon has a spectrally flat refractive index and enhanced imaginary indices at the 440 nm wavelength are caused by brown carbon or hematite. Carbonaceous aerosols can be separated from dust in imaginary refractive index space because 95 % of biomass burning aerosols have imaginary indices greater than 0.0042 at the 675-1020 nm wavelengths, and 95 % of dust has imaginary refractive indices of less than 0.0042 at those wavelengths. However, mixtures of these two types of particles can not be unambiguously partitioned on the basis of optical properties alone, so we also separate these particles by size. Regional and seasonal results are consistent with expectations. Monthly climatologies of fine mode soot carbon are less than 1.0 % by volume for West Africa and the Middle East, but the southern African and South American biomass burning sites have peak values of 3.0 and 1.7 %. Monthly averaged fine mode brown carbon volume fractions have a peak value of 5.8 % for West Africa, 2.1 % for the Middle East, 3.7 % for southern Africa, and 5.7 % for South America. Monthly climatologies of free iron volume fractions show little seasonal variability, and range from about 1.1 to 1.7 % for coarse mode aerosols in all four study regions. Finally, our sensitivity study indicates that the soot carbon retrieval is not sensitive to the component refractive indices or densities assumed for carbonaceous and free iron aerosols, and the retrieval differs by only 15.4 % when these parameters are altered from our chosen baseline values. The total uncertainty of retrieving soot carbon mass is ˜ 50 % (when uncertainty in the AERONET product and mixing state is included in the analysis).

  16. Heterogeneous Reduction Pathways for Hg(II) Species on Dry Aerosols: A First-Principles Computational Study.

    PubMed

    Tacey, Sean A; Xu, Lang; Mavrikakis, Manos; Schauer, James J

    2016-04-01

    The atmospheric lifetime of mercury is greatly impacted by redox chemistry resulting from the high deposition rate of reactive mercury (Hg(II)) compared to elemental mercury (Hg(0)). Recent laboratory and field studies have observed the reduction of Hg(II), but the chemical mechanism for this reaction has not been identified. Recent experimental work has shown that the reduction reaction is heterogeneous and can occur on iron and sodium chloride aerosol surfaces. This study explores the use of density functional theory calculations to discern the reduction pathways of HgCl2, HgBr2, Hg(NO3)2, and HgSO4 on clean Fe(110), NaCl(100), and NaCl(111)(Na) surfaces. Potential energy surfaces were prepared for the various reduction pathways, indicating that the reduction pathway leading to the production of gas-phase elemental mercury is highly favorable on Fe(110) and NaCl(111)(Na). Moreover, the Fe(110) surface requires an external energy source of ∼0.5 eV to desorb the reduced mercury, whereas the NaCl(111)(Na) surface requires no energy input. The results indicate that a number of mercury species can be reduced on metallic iron and sodium chloride surfaces, which are known aerosol components, and that a photochemical reaction involving the aerosol surface is likely needed for the reaction to be catalytic. PMID:27014805

  17. Solid-phase supported profluorescent nitroxide probe for the determination of aerosol-borne reactive oxygen species.

    PubMed

    Sleiman, Mohamad; Destaillats, Hugo; Gundel, Lara A

    2013-11-15

    Reactive oxygen species (ROS) and free radicals play important roles in the chemical transformation and adverse health effects of environmental aerosols. This work presents a simple and sensitive method for sampling and analysis of ROS using a packed column coated with a profluorescent nitroxide scavenger, proxyl fluorescamine (PF). Quantification was performed by extraction and analysis using HPLC with fluorescence detection. For comparison, the conventional method of collecting aerosols into dichlorofluorescin (DCFH) aqueous solution was used as a reference. The method was successfully applied to the determination of ROS in a model secondary organic aerosol (SOA) system generated by ozonolysis of nicotine, as well as in secondhand tobacco smoke (SHS). ROS concentrations between 50-565 nmol m(-3) were detected in fresh SOA and SHS samples. After SHS aging for 22 h, 13-18% of the initial ROS mass remained, suggesting the presence of persistent ROS. The new method offers better stability and reproducibility along with sensitivity comparable to that of DCFH (method detection limit of 3.2 and 1.4 nmol m(-3) of equivalent H2O2 for PF and DCFH respectively). The PF probe was stable during storage at room temperature and not reactive with ozone or NOx, whereas DCFH in the particle-collecting liquid system was strongly influenced by ozone and NOx interferences. This case study provides a good basis for employing solid-phase supported PF for field measurement of specific ROS in other combustion systems (i.e. biomass burning, candles, and diesel exhaust) and environmental aerosols. PMID:24148512

  18. Incoherent scatter radar observations of D-region charged aerosol species

    NASA Astrophysics Data System (ADS)

    Strelnikova, Irina; Rapp, Markus; Li, Qiang

    There is today substantial interest in aerosols in the mesosphere and their interaction with their neutral and charged environment. These aerosols comprise both ice particles in the polar summer mesopause region and smoke particles of meteoric origin that are expected to occur in the entire middle atmosphere and during all seasons. The presence of ice particles in the mesosphere has been known for many decades and is most prominently revealed in the form of noctilucent clouds, also known as polar mesospheric clouds. Smoke particles, on the other hand, have sizes of few nanometers only such that their detection by remote sensing techniques has long been deemed impossible. In consequence, sporadic rocket borne in-situ measurements have long been the only source of experimental evidence regarding the existence and properties of these particles. However, it has recently been realized that charged mesospheric aerosol particles modify the plasma properties of the D-region and thereby influence the characteristics of radar backscatter from these altitudes (i.e., radar reflectivity and/or spectral properties). Hence, it is possible to infer properties of these charged aerosol particles in the D-Region using radar observations. In this paper we present two independent methods yielding particles properties based on such measurements and give an overview of recent results.

  19. Solar Occultation Constellation for Retrieving Aerosols and Trace Element Species (SOCRATES): Proposed Mission Concept

    NASA Astrophysics Data System (ADS)

    Gordley, L. L.; Bailey, S. M.

    2015-12-01

    The goal of SOCRATES is to resolve the critical but underexplored role of the upper troposphere/lower stratosphere (UTLS) in climate change. The mission would provide the suite of measurements required to quantify UTLS transport pathways and their contribution to UTLS composition, and to evaluate the radiative forcing implications of changes in UTLS composition forced by expected changes in these pathways as the climate evolves. The discrimination and quantification of UTLS transport pathways requires simultaneous measurement of several key trace gases and aerosols with high precision, accuracy, and vertical resolution. Furthermore, aerosols and clouds, often present in the UTLS, complicate the measurement of trace gases. The SOCRATES sensor is a 23-channel Gas Filter Correlation Radiometer (GFCR), referred to as GLO (GFCR Limb solar Occultation), with heritage from HALOE on UARS, and SOFIE on AIM. GLO measures aerosol extinction from 0.45 to 3.88 μm, important radiatively active gases in the UTLS (H2O, O3, CH4, N2O), key tracers of UTLS transport (HCN, CO, HDO), gases important in stratospheric O3 chemistry (HCl and HF), and temperature from cloud top to 50 km at a vertical resolution of < 1 km. Improved pointing knowledge will provide dramatically better retrieval precision in the UTLS, even in the presence of aerosols, than possible with HALOE. In addition, the GLO form factor is only of order 10% of that of HALOE, and costs for a constellation of GLO sensors is within the cost cap of a NASA Earth Venture mission. The SOCRATES mission concept is a 6-element constellation of autonomous small satellites, each mated with a GLO sensor, and deployed from a single launch vehicle. The SOCRATES/GLO approach reaps the advantages of solar occultation: high precision and accuracy; robust calibration; and high vertical resolution, while mitigating the sparse coverage of a single solar occultation sensor. We present the SOCRATES science case, and key elements of the

  20. Solar Occultation Constellation for Retrieving Aerosols and Trace Element Species (SOCRATES) Mission Concept

    NASA Astrophysics Data System (ADS)

    Bailey, S. M.; Bevilacqua, R. M.; Fish, C. S.; Gordley, L. L.; Fromm, M. D.

    2014-12-01

    The goal of SOCRATES is to quantify the critical role of the upper troposphere/lower stratosphere (UTLS) in the climate system. The mission would provide, for the first time, the suite of measurements required to quantify stratosphere/troposphere exchange (STE) pathways and their contribution to UTLS composition, and to evaluate the radiative forcing implications of potential changes in STE pathways with climate change. The discrimination and quantification of STE pathways requires simultaneous measurement of several key trace gases and aerosols with high precision, accuracy, and vertical resolution. Furthermore, aerosol and clouds, often present in the UTLS, complicate the measurement of trace gases. The SOCRATES sensor is a 23-channel Gas Filter Correlation Radiometer (GFCR), referred to as GLO (GFCR Limb solar Occultation), with heritage from HALOE on UARS, and SOFIE on AIM. GLO measures aerosol extinction from 0.45 to 3.88 μm, important radiatively active gases in the UTLS (H2O, O3, CH4, N2O), key tracers of STE (HCN, CO, HDO), gases important in stratospheric O3 chemistry (HCl and HF), and temperature from cloud top to 50 km at a vertical resolution of 1 km. Improved pointing knowledge will provide dramatically better retrieval precision in the UTLS, even in the presence of aerosols, than possible with HALOE. In addition, the GLO form factor is only a few percent of that of HALOE, and costs for a constellation of GLO sensors is within the cost cap of a NASA Venture mission. The SOCRATES mission concept is an 8-element constellation of autonomous CubeSats, each mated with a GLO sensor, deployed from a single launch vehicle. The SOCRATES/GLO approach reaps the advantages of solar occultation: high precision and accuracy; robust calibration; and high vertical resolution, while mitigating the sparse coverage of a single solar occultation sensor. We present the SOCRATES science case, and key elements of the SOCRATES mission and GLO instrument concepts.

  1. Single-Species Aerosol Coagulation and Deposition with Arbitrary Size Resolution.

    SciTech Connect

    SAJO, ERNO

    2012-07-31

    Version 00 SAEROSA solves the dynamic aerosol coagulation and deposition problem with arbitrary computational precision under a variety of conditions. The code includes numerous user-selectable coagulation kernels, alone or in combinations, and permits an arbitrary initial size distribution. Many parameter combinations and what-if scenarios under user control are possible. The output gives the particle size distribution suspended in the carrier fluid initially and after the desired aerosol aging time in terms of both differential and integral aerosol volume concentrations. An auxiliary routine designed for the Mac OSX environment provides plotting capability. The output can be further processed by e.g., spreadsheets. The code has been benchmarked against three computer models, including MAEROS, and analytical models with excellent agreement. The test cases also included scenarios where previously published computational coagulation models lack capabilities or exhibit numerical instabilities. These included narrow, delta function, and non-lognormal initial size distributions, and further conditions, such as the presence of simultaneous coagulation mechanisms, including electrostatic effects, spanning multiple flow-regimes.

  2. Single-Species Aerosol Coagulation and Deposition with Arbitrary Size Resolution.

    2012-07-31

    Version 00 SAEROSA solves the dynamic aerosol coagulation and deposition problem with arbitrary computational precision under a variety of conditions. The code includes numerous user-selectable coagulation kernels, alone or in combinations, and permits an arbitrary initial size distribution. Many parameter combinations and what-if scenarios under user control are possible. The output gives the particle size distribution suspended in the carrier fluid initially and after the desired aerosol aging time in terms of both differential andmore » integral aerosol volume concentrations. An auxiliary routine designed for the Mac OSX environment provides plotting capability. The output can be further processed by e.g., spreadsheets. The code has been benchmarked against three computer models, including MAEROS, and analytical models with excellent agreement. The test cases also included scenarios where previously published computational coagulation models lack capabilities or exhibit numerical instabilities. These included narrow, delta function, and non-lognormal initial size distributions, and further conditions, such as the presence of simultaneous coagulation mechanisms, including electrostatic effects, spanning multiple flow-regimes.« less

  3. Measurements of HNO3, SO2 High Resolution Aerosol SO4 (sup 2-), and Selected Aerosol Species Aboard the NASA DC-8 Aircraft: During the Transport and Chemical Evolution Over the Pacific Airborne Mission (TRACE-P)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    2004-01-01

    The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.

  4. 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.

  5. 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.

  6. Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

    NASA Astrophysics Data System (ADS)

    Xu, Lingling; Chen, Jinsheng

    2016-04-01

    Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

  7. Examining the role of NOx and acidity on organic aerosol formation through predictions of key isoprene aerosol species in the United States

    EPA Science Inventory

    Isoprene is a significant contributor to organic aerosol in the Southeastern United States. Later generation isoprene products, specifically isoprene epoxydiols (IEPOX) and methacryloylperoxynitrate (MPAN), have been identified as SOA precursors. The contribution of each pathway ...

  8. Measuring Uptake Coefficients and Henry's Law Constants of Gas-Phase Species with Models for Secondary Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Fairhurst, M. C.; Waring-Kidd, C.; Ezell, M. J.; Finlayson-Pitts, B. J.

    2014-12-01

    Volatile organic compounds (VOC) are oxidized in the atmosphere and their products contribute to secondary organic aerosol (SOA) formation. These particles have been shown to have effects on visibility, climate, and human health. Current models typically under-predict SOA concentrations from field measurements. Underestimation of these concentrations could be a result of how models treat particle growth. It is often assumed that particles grow via instantaneous thermal equilibrium partitioning between liquid particles and gas-phase species. Recent work has shown that growth may be better represented by irreversible, kinetically limited uptake of gas-phase species onto more viscous, tar-like SOA. However, uptake coefficients for these processes are not known. The goal of this project is to measure uptake coefficients and solubilities for different gases onto models serving as proxies for SOA and determine how they vary based on the chemical composition of the gas and the condensed phase. Experiments were conducted using two approaches: attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy and a flow system coupled to a mass spectrometer. The ATR crystal was coated with the SOA proxy and the gas-phase species introduced via a custom flow system. Uptake of the gas-phase species was characterized by measuring the intensity of characteristic IR bands as a function of time, from which a Henry's law constant and initial estimate of uptake coefficients could be obtained. Uptake coefficients were also measured in a flow system where the walls of the flow tube were coated with the SOA proxy and gas-phase species introduced via a moveable inlet. Uptake coefficients were derived from the decay in gas-phase species measured by mass spectrometry. The results of this work will establish a structure-interaction relationship for uptake of gases into SOA that can be implemented into regional and global models.

  9. The optical constants of several atmospheric aerosol species - Ammonium sulfate, aluminum oxide, and sodium chloride

    NASA Technical Reports Server (NTRS)

    Toon, O. B.; Pollack, J. B.; Khare, B. N.

    1976-01-01

    An investigation is conducted of problems which are related to a use of measured optical constants in the simulation of the optical constants of real atmospheric aerosols. The techniques of measuring optical constants are discussed, taking into account transmission measurements through homogeneous and inhomogeneous materials, the immersion of a material in a liquid of a known refractive index, the consideration of the minimum deviation angle of prism measurement, the interference of multiply reflected light, reflectivity measurements, and aspects of mathematical analysis. Graphs show the real and the imaginary part of the refractive index as a function of wavelength for aluminum oxide, NaCl, and ammonium sulfate. Tables are provided for the dispersion parameters and the optical constants.

  10. Statistical analysis of aerosol species, trace gasses, and meteorology in Chicago.

    PubMed

    Binaku, Katrina; O'Brien, Timothy; Schmeling, Martina; Fosco, Tinamarie

    2013-09-01

    Both canonical correlation analysis (CCA) and principal component analysis (PCA) were applied to atmospheric aerosol and trace gas concentrations and meteorological data collected in Chicago during the summer months of 2002, 2003, and 2004. Concentrations of ammonium, calcium, nitrate, sulfate, and oxalate particulate matter, as well as, meteorological parameters temperature, wind speed, wind direction, and humidity were subjected to CCA and PCA. Ozone and nitrogen oxide mixing ratios were also included in the data set. The purpose of statistical analysis was to determine the extent of existing linear relationship(s), or lack thereof, between meteorological parameters and pollutant concentrations in addition to reducing dimensionality of the original data to determine sources of pollutants. In CCA, the first three canonical variate pairs derived were statistically significant at the 0.05 level. Canonical correlation between the first canonical variate pair was 0.821, while correlations of the second and third canonical variate pairs were 0.562 and 0.461, respectively. The first canonical variate pair indicated that increasing temperatures resulted in high ozone mixing ratios, while the second canonical variate pair showed wind speed and humidity's influence on local ammonium concentrations. No new information was uncovered in the third variate pair. Canonical loadings were also interpreted for information regarding relationships between data sets. Four principal components (PCs), expressing 77.0 % of original data variance, were derived in PCA. Interpretation of PCs suggested significant production and/or transport of secondary aerosols in the region (PC1). Furthermore, photochemical production of ozone and wind speed's influence on pollutants were expressed (PC2) along with overall measure of local meteorology (PC3). In summary, CCA and PCA results combined were successful in uncovering linear relationships between meteorology and air pollutants in Chicago and

  11. Characterization of radicals and high-molecular weight species from alpha-pinene/ozone reaction and ambient aerosol samples

    NASA Astrophysics Data System (ADS)

    Pavlovic, Jelica

    Secondary organic aerosol formed during oxidation of different volatile organic compounds is composed from a number of final and intermediate reaction products. The final products include compounds in both low and high molecular weight range called also oligomer species. These compounds can be highly volatile, as well as being semi- or low-volatility compounds. This study characterized intermediate reactive radical products formed from previously often studied alpha-pinene/ozone reaction. In order to passivate those radical species nitrone spin traps were used. 5,5-dimethyl-4,5-dihydro-3H-pyrrole-N-oxide (DMPO), and 5-dietoxyphosphoryl-5-methyl-1-pyrroline-N-oxide (DEPMPO) traps were able to successfully trap oxygen- and carbon-centered radicals produced from alpha-pinene/ozone reaction. Electrospray ionization (ESI) in negative ion mode with mass spectrometry (MS) detection was used to scan spectra of formed spin trap adducts and the tandem mass spectrometry (MSn) to elucidate its structures as well as structures of captured radicals. The same method was applied to analyze radical species present in ambient PM2.5 samples. Few carbon- (alkyl) and oxygen- (alkoxyl) centered radicals were captured with DMPO and DEPMPO traps. The second part of this study was focused on high molecular weight (high-MW) species formed from the same reaction (alpha-pinene/ozone), but found also in fine particulate matter fractions of ambient samples. LC/MS/MS analysis of dimer species from chamber study revealed fragments that can originate from peroxide structures. Proposed reaction for these peroxide dimer formation is self reaction of two peroxyl radicals, followed by the loss of oxygen molecule. These findings emphasize the role of peroxyl (ROO) radicals in formation of high-MW products and are in line with the high O:C ratio results reported in other studies. Water soluble organic carbon (WSOC) extracts of three size fractions of the ambient aerosol, PM1--2.5, PM0.1--1, and PM<0

  12. Speciation of 127I and 129I in atmospheric aerosols at Risø, Denmark: insight into sources of iodine isotopes and their species transformations

    NASA Astrophysics Data System (ADS)

    Zhang, Luyuan; Hou, Xiaolin; Xu, Sheng

    2016-02-01

    Speciation analysis of iodine in aerosols is a very useful approach for understanding geochemical cycling of iodine in the atmosphere. In this study, overall iodine species, including water-soluble iodine species (iodide, iodate and water-soluble organic iodine), NaOH-soluble iodine, and insoluble iodine have been determined for 129I and 127I in the aerosols collected at Risø, Denmark, during March and May 2011 (shortly after the Fukushima nuclear accident) and in December 2014. The measured concentrations of total iodine are in the range of 1.04-2.48 ng m-3 for 127I and (11.3-97.0) × 105 atoms m-3 for 129I, corresponding to 129I / 127I atomic ratios of (17.8-86.8) × 10-8. The contribution of Fukushima-derived 129I (peak value of 6.3 × 104 atoms m-3) is estimated to be negligible (less than 6 %) compared to the total 129I concentration in northern Europe. The concentrations and species of 129I and 127I in the aerosols are found to be strongly related to their sources and atmospheric pathways. Aerosols that were transported over the contaminated seas contained higher concentrations of 129I than aerosols transported over the European continent. The high 129I concentrations of the marine aerosols are attributed to secondary emission of marine discharged 129I in the contaminated seawater in the North Sea, North Atlantic Ocean, English Channel, Kattegat, etc., rather than direct gaseous release from the European nuclear reprocessing plants (NRPs). Water-soluble iodine was found to be a minor fraction to the total iodine for both 127I (7.8-13.7 %) and 129I (6.5-14.1 %) in ocean-derived aerosols, but accounted for 20.2-30.3 % for 127I and 25.6-29.5 % for 129I in land-derived aerosols. Iodide was the predominant form of water-soluble iodine, accounting for more than 97 % of the water-soluble iodine. NaOH-soluble iodine seems to be independent of the sources of aerosols. The significant proportion of 129I and 127I found in NaOH-soluble fractions is likely bound with

  13. Speciation of 127I and 129I in atmospheric aerosols at Risø, Denmark: insight into sources of iodine isotopes and their species transformations

    NASA Astrophysics Data System (ADS)

    Zhang, L. Y.; Hou, X. L.; Xu, S.

    2015-09-01

    Speciation analysis of iodine in aerosols is a very useful approach for understanding geochemical cycling of iodine in the atmosphere. In this study, overall iodine species, including water-soluble iodine species (iodide, iodate and water-soluble organic iodine), NaOH-soluble iodine and insoluble iodine have been determined for 129I and 127I in the aerosols collected at Risø, Denmark, between March and May 2011 (shortly after the Fukushima nuclear accident) and in December 2014. The measured concentrations of total iodine are in the range of 1.04-2.48 ng m-3 for 127I and (11.3-97.0) × 105 atoms m-3 for 129I, and 129I / 127I atomic ratios of (17.8-86.8) × 10-8. The contribution of Fukushima-derived 129I (peak value of 6.3 × 104 atoms m-3) is estimated to be negligible (less than 6 %) compared to the total 129I concentration in northern Europe. The concentrations and species of 129I and 127I in the aerosols are found to be strongly related to their sources and atmospheric pathways. Aerosols that were transported over the contaminated ocean, contained higher amounts of 129I than aerosols transported over the European continent. The high 129I concentrations of the marine aerosols are attributed to secondary emission from heavily 129I-contaminated seawater rather than primary gaseous release from nuclear reprocessing plants. Water-soluble iodine was found to be a minor fraction to total iodine for both 127I (7.8-13.7 %) and 129I (6.5-14.1 %) in ocean-derived aerosols, but accounted for 20.2-30.3 % for 127I and 25.6-29.5 % for 129I in land-derived aerosols. Iodide was the predominant form of water-soluble iodine, accounting for more than 97 % of the water-soluble iodine. NaOH-soluble iodine seems to be independent of the sources of aerosols. The significant proportion of 129I and 127I found in NaOH-soluble fractions is likely bound with organic substances. In contrast to water-soluble iodine however, the sources of air masses exerted distinct influences on insoluble

  14. Backscattering measurements of atmospheric aerosols at CO2 laser wavelengths: implications of aerosol spectral structure on differential-absorption lidar retrievals of molecular species.

    PubMed

    Ben-David, A

    1999-04-20

    The volume backscattering coefficients of atmospheric aerosol were measured with a tunable CO2 lidar system at various wavelengths in Utah (a desert environment) along a horizontal path a few meters above the ground. In deducing the aerosol backscattering, a deconvolution (to remove the smearing effect of the long CO2 lidar pulse and the lidar limited bandwidth) and a constrained-slope method were employed. The spectral shape beta(lambda) was similar for all the 13 measurements during a 3-day period. A mean aerosol backscattering-wavelength dependence beta(lambda) was computed from the measurements and used to estimate the error Delta(CL) (concentration-path-length product) in differential-absorption lidar measurements for various gases caused by the systematic aerosol differential backscattering and the error that is due to fluctuations in the aerosol backscattering. The water-vapor concentration-path-length product CL and the average concentration C = /L for a path length L computed from the range-resolved lidar measurements is consistently in good agreement with the water-vapor concentration measured by a meteorological station. However, I was unable to deduce, reliably, the range-resolved water-vapor concentration C(r), which is the derivative of the range-dependent product CL, because of the effect of residual noise caused mainly by errors in the deconvolved lidar measurements.

  15. Reactions of SIV species with organic compounds: formation mechanisms of organo-sulfur derivatives in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Passananti, Monica; Shang, Jing; Dupart, Yoan; Perrier, Sébastien; George, Christian

    2015-04-01

    Secondary organic aerosol (SOA) have an important impact on climate, air quality and human health. However the chemical reactions involved in their formation and growth are not fully understood or well-constrained in climate models. It is well known that inorganic sulfur (mainly in oxidation states (+IV) and (+VI)) plays a key role in aerosol formation, for instance sulfuric acid is known to be a good nucleating gas. In addition, acid-catalyzed heterogeneous reactions of organic compounds has shown to produce new particles, with a clear enhancement in the presence of ozone (Iinuma 2013). Organosulfates have been detected in tropospheric particles and aqueous phases, which suggests they are products of secondary organic aerosol formation process (Tolocka 2012). Originally, the production of organosulfates was explained by the esterification reaction of alcohols, but this reaction in atmosphere is kinetically negligible. Other formation pathways have been suggested such as hydrolysis of peroxides and reaction of organic matter with sulfite and sulfate radical anions (SO3-, SO4-) (Nozière 2010), but it remains unclear if these can completely explain atmospheric organo-sulfur aerosol loading. To better understand the formation of organo-sulfur compounds, we started to investigate the reactivity of SIV species (SO2 and SO32-) with respect to specific functional groups (organic acids and double bonds) on atmospherically relevant carboxylic acids and alkenes. The experiments were carried out in the homogeneous aqueous phase and at the solid-gas interface. A custom built coated-wall flow tube reactor was developed to control relativity humidity, SO2 concentration, temperature and gas flow rate. Homogeneous and heterogeneous reaction kinetics were measured and resulting products were identified using liquid chromatography coupled with an orbitrap mass spectrometer (LC-HR-MS). The experiments were performed with and without the presence of ozone in order to evaluate any

  16. 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.

  17. 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

  18. Airborne Fungi in Sahara Dust Aerosols Reaching the Eastern Caribbean: II. Species Identification Using Molecular Techniques

    NASA Astrophysics Data System (ADS)

    de La Mota, A.; Betancourt, C.; Detres, Y.; Armstrong, R.

    2003-12-01

    Fungi samples from filters collected in Castle Bruce, Dominica from March through July 2002, were previously purified and identified to genus level using classic macroscopic and microscopic techniques. A total of 105 isolated colonies were cultured in liquid media and the mycelial mats used for DNA extraction. PCR was used to amplify the ITS region of the rDNA using the ITS1 and ITS4 primers. Both strands of the amplified products were sequenced and the final identification to species level was completed by a GenBank search. Fourteen different species and one fungal endophyte were identified from genders Aspergillus,Penicillium, Fusarium, Cladosporium, Curvularia and Phanerochaete. Some of these species such as A. fumigatus, A. japonicus, P. citrinum and C. cladosporoides are known to cause respiratory disorders in humans. A. fumigatus causes an aggressive pulmonary allergic response that might result in allergic bronchopulmonary aspergillosis. Other species such as F. equiseti and C. brachyspora are plant pathogens affecting economically important crops. Sahara dust is an important source of fungal spores of species that are not common in the Caribbean region.

  19. Vertical distribution of non-volatile species of upper tropospheric and lower stratospheric aerosol observed by balloon-borne optical particle counter above Ny-Aalesund, Norway in the winter of 2015

    NASA Astrophysics Data System (ADS)

    Shiraishi, K.; Hayashi, M.; Shibata, T.; Neuber, R.; Ruhe, W.

    2015-12-01

    The polar lower stratosphere is the sink area of stratospheric global circulation. The composition, concentration and size distribution of aerosol in the polar stratosphere are considered to be strongly influenced by the transportations from mid-latitude to polar region and exchange of stratosphere to troposphere. In order to study the aerosol composition and size distribution in the Arctic stratosphere and the relationship between their aerosol microphysical properties and transport process, we carried out balloon-borne measurement of aerosol volatility above Ny-Aalesund, Norway in the winter of 2015. In our observation, two optical particle counters and a thermo denuder were suspended by one rubber balloon. A particle counter measured the heated aerosol size distribution (after heating at the temperature of 300 degree by the thermo denuder) and the other measured the ambient aerosol size distribution during the observation. The observation was carried out on 15 January, 2015. Balloon arrived at the height of 30km and detailed information of aerosol size distributions in upper troposphere and lower stratosphere for both heated aerosol and ambient aerosol were obtained. As a Result, the number ratio of non-volatile particles to ambient aerosol particles in lower stratosphere (11-15km) showed different feature in particle size range of fine mode (0.3aerosol particles were 1-3% in fine mode range and 7-20% in coarse mode range. They suggested that fine particles are composed dominantly of volatile species (probably sulfuric acid), and coarse particles are composed of non-volatile species such as minerals, sea-salts. In our presentation, we show the obtained aerosol size distribution and discuss the aerosol compositions and their transport process.

  20. An Investigation of Aerosol Measurements from the Halogen Occultation Experiment: Validation, Size Distributions, Composition, and Relation to Other Chemical Species

    NASA Technical Reports Server (NTRS)

    Deshler, Terry; Hervig, Mark E.

    1998-01-01

    The efforts envisioned within the original proposal (accepted February 1994) and the extension of this proposal (accepted February 1997) included measurement validations, the retrieval of aerosol size distributions and distribution moments, aerosol correction studies, and investigations of polar stratospheric clouds. A majority of the results from this grant have been published. The principal results from this grant are discussed.

  1. Intercomparison of methods for the measurement of carbonaceous aerosol species. Final report

    SciTech Connect

    Appel, B.R.; Cheng, W.; Tokiwa, Y.; Salaymeh, F.; Povard, V.

    1987-01-01

    The principal goal of the study, as part of the Carbonaceous Species Methods Comparison Study, was to perform field trials at Citrus College, Glendora, CA, in August 1986 with a sampler intended to minimize positive and negative artifacts for sampling particulate carbon. In addition, organic and elemental carbon in atmospheric and laboratory-generated samples were analyzed to permit intermethod comparisons. The particulate carbon sampler consisted of a cyclone, parallel-plate diffusion denuder packed with coarse, activated alumina, and a quartz-fiber filter followed by a fluidized bed of activated alumina. The sampler failed to perform effectively in atmospheric trials; alumina showed little activity in decreasing the positive error in filter carbon sampling due to sorption of gas-phase carbonaceous material. The measurement of organic (Co) and elemental carbon (Ce) employed an optical absorption technique for Ce and a coulometer for total C (Ct). Organic carbon was then obtained by difference between Ct and Ce. In addition, organic and elemental carbon in atmospheric and laboratory-generated samples were analyzed to permit intermethod comparisons.

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

    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

  3. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

    anthropogenic aerosols are thought to be of comparable magnitude to the positive forcings resulting from incremental concentrations of greenhouse gases.The magnitudes and estimated uncertainties of the several forcings over the industrial period are summarized in Figure 2, which was prepared as part of the recent assessment of climate change by the Intergovernmental Panel on Climate Change (IPCC, 2001). This figure shows for each forcing a best estimate of its magnitude and of the associated uncertainty. The uncertainty associated with forcing by the long-lived greenhouse gases is relatively small, reflective of the rather high level of understanding of both the magnitude of the incremental concentrations of these species and of the radiative perturbation per incremental concentration. In marked contrast, the uncertainties associated with the several aerosol forcings are much greater, indicative of a much lesser understanding of the controlling quantities. For direct forcing by dust aerosols, which may be positive or negative, and for indirect radiative forcing by anthropogenic aerosols the IPCC working groups ( Penner et al., 2001; Ramaswamy et al., 2001) declined to present best estimates but indicated only possible ranges. This situation is unsatisfying but unavoidable, given the current state of knowledge. Other reviews of aerosol forcings are provided by Ramanathan et al. (2001a), Haywood and Boucher (2000), Shine and Forster (1999), Schwartz (1996), and Schwartz and Slingo (1996). Hobbs (1993) provides an introduction to aerosol-cloud interactions. (9K)Figure 2. The effects of various anthropogenic constituents of the atmosphere on the global climate system for the year 2000 relative to 1750 as estimated by the Intergovernmental Panel on Climate Change (IPCC, 2001). The effects are expressed as forcings, which in this case are changes in global mean radiative flux components arising from the indicated perturbing influence. Best estimates are indicated by the bars and

  4. Aqueous aerosol SOA formation: impact on aerosol physical properties.

    PubMed

    Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

    2013-01-01

    Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions. PMID:24601011

  5. Characterization and quantification of aerosol chemical species present below and within cloud over an eastern Himalayan high altitude hill station in India

    NASA Astrophysics Data System (ADS)

    Roy, Arindam; Chatterjee, Abhijit; Sarkar, Chirantan; Ghosh, Sanjay; Raha, Sibaji

    2016-07-01

    There are two main processes through which aerosols and gases get scavenged by rain called below-cloud scavenging or "washout" and in-cloud scavenging or "rainout". The first process refers to the washout of the aerosols and gases present below the cloud during precipitation events by raindrops along their fall. The second process corresponds to the condensation of water vapor on aerosol particles during the formation of cloud droplets and incorporation of gases surrounding the droplets by aqueous-phase reactions. However, the most efficient pathway to remove the atmospheric pollutants is below cloud scavenging which is a major pointer of ecosystem, biogeochemical cycle as well as the climate change. A study has been conducted in 2014 and 2015 monsoon (June-September) in Darjeeling (27.01 ° N, 88.15 ° E), a high altitude (2200 m asl) hill station over eastern Himalaya in India. The study was focused on the below-cloud and in-cloud scavenging of various aerosol ionic species. Attempt was also made to estimate the contribution of in-cloud scavenging and below-cloud scavenging by collecting rain samples sequentially for different rain events. Sea-salt (Na+, sea-Mg2+, Cl- and sea-SO4 2-) and soil dust (non-sea Ca2+, non-sea-Mg2+) species show sharp decrease in concentration for each of the rain sample. This indicates that these species were mostly accumulated below the cloud and washed out during rain. Their concentrations were thus decreased sharply as rains progressed. On the other hand, non-SO4-2 and NH4+ showed different behavior. Their concentrations decreased sharply at the initial stage of the rain and then remained almost constant with rainfall. This explains wash out of these two species at the initial stage of the rain and their contribution from "within the cloud". NH4 + and non-sea-SO4 2- could thus act as cloud condensation nuclei over this part of Himalaya. A strong correlation between these two species indicates their association as (NH4)2SO4. Acidity

  6. Real-time measurement of aerosol black carbon during the Carbonaceous Species Methods Comparison Study, Citrus College, Glendora, California, August 12-21, 1986: Final report

    SciTech Connect

    Hansen, A.D.A.; Novakov, T.

    1987-11-01

    During the period August 12-21, 1986, the Atmospheric Aerosol Research Group of Lawrence Berkeley Laboratory participated in the Carbonaceous Species Method Comparison Study (CSMCS) conducted at Citrus College, Glendora, California. The equipment that we used was the aethalometer, an instrument developed at LBL that measures the concentration of aerosol black carbon in real time. In this report we present our results from that study in the form of 1-minute, 1-hour, and multi-hour average concentrations. We found concentrations generally ranging from 2 to 5 ..mu..g (BC)m/sup 3/, usually with increases in the morning traffic hours. We also observed short-duration (2-15 min) peaks in the black carbon concentration that could be directly attributed to the activity of vehicles in a delivery area less than 50 m from the study site. We conclude that mobile sources were the major contributor to the short- and medium-term variability of aerosol black carbon measured at this site. 5 refs., 5 figs., 1 tab

  7. 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

  8. Biomass burning as an important source of reactive oxygen species associated with the atmospheric aerosols in Southeastern United States - Implications for health effects of ambient particulate matter

    NASA Astrophysics Data System (ADS)

    Verma, V.; Weber, R. J. J.; Fang, T.; Xu, L.; Ng, N. L.; Russell, A. G.

    2014-12-01

    We assessed the potential of water-soluble fraction of atmospheric fine aerosols in the southeastern US to generate reactive oxygen species (ROS). ROS-generation potential of particles was quantified by the dithiothreitol (DTT) assay and involved analysis of fine particulate matter (PM) extracted from high-volume quartz filters (23 h integrated daily samples) collected for one year at various sites in different environmental settings in the southeast, including three urban Atlanta sites, and one rural site in Yorkville. Water-soluble PM extracts were further separated into the hydrophobic and hydrophilic fractions using a C-18 column, and both fractions were analyzed for the DTT activity. Organic aerosol (OA) composition was measured at selected sites using a High-Resolution Time-of-Flight Aerosol Mass Spectrophotometer (HR-ToF-AMS). The various factors of the organic aerosols, i.e. Isoprene OA (Isop-OA), hydrocarbon-like OA (HOA), less-oxidized oxygenated OA, (LO-OOA), more-oxidized OOA (MO-OOA), cooking OA (COA), and biomass burning OA (BBOA) were also resolved, and their ability to generate ROS investigated by linear regression techniques. Among all OA factors, BBOA was most consistently associated with ROS, with the highest intrinsic DTT activity of 151±20 pmol/min/μg. The water-soluble bioavailable fraction of BBOA-DTT activity is 2-3 times higher than the reported total-DTT activity of diesel exhaust particles. The total contribution of various aerosol sources to the ROS generating potential was also determined by the positive matrix factorization approach. Interestingly, biomass burning appears as the strongest source of ROS generation, with its annual contribution of 35 % to DTT activity; the contribution was higher in winter (47 %), than summer (24 %) and fall (17 %) seasons. The good agreement between the hydrophobic DTT activity with that estimated from the summed OA components, indicates that humic-like substances (HULIS), which are abundantly emitted

  9. Distributions of Beryllium 7 and Lead 210, and Soluble Aerosol-Associated Ionic Species Over the Western Pacific: PEM West B, February - March 1994

    NASA Technical Reports Server (NTRS)

    Dibb, J. E.; Talbot, R. W.; Lefer, B. L.; Scheuer, E.; Gregory, G. L.; Browell, E. V.; Bradshaw, J. D.; Sandholm, S. T.; Singh, H. B.

    1997-01-01

    Aerosol sampling for the determination of the concentrations of soluble ionic species and the natural radionuclides Be-7 and Pb-210 was conducted from the NASA DC-8 over the western Pacific as part of GTE/PEM-West B during February - March 1994. Concentrations of most soluble ionic species in the free troposphere were higher in samples collected on flights originating from Hong Kong and Japan than those collected further east over the open ocean. In both regions the measured concentrations were higher than those found during PEM-West A (fall 1991). Activities of Pb-210, a tracer of air masses influenced by sources on the Asian continent, showed the same patterns. These data indicate the effect of stronger continental outflow from Asia over the western Pacific during the spring compared to fall season. For readily scavenged aerosol-associated species and soluble acidic gases the strongest indications of Asian outflow were restricted to altitudes below 6 km. The distribution of the continental tracer Pb-210 was also compared to those of a large number of gas phase species measured on the DC-8. Relatively strong correlations were found with O3, and peroxyacetylnitrate (PAN), but only during the flights over the remote Pacific. During PEM-West A, similar correlations were seen, but they were stronger near Asia. We believe that correlations are a signature of continental air that has been processed by deep wet convection over land before being advected over the ocean. One flight over the Sea of Japan provided the opportunity to sample upper troposphere/lower stratosphere air in and around a tropopause fold. Concentrations of Be-7 reached 7 pCi/cu m STP, and peak O3, mixing ratios of 480 ppb were encountered at 10.7 km. The Be-7 data are used to estimate the fraction of stratospheric air mixed down into the troposphere by circulation in the fold.

  10. Distributions of Beryllium 7 and Lead 210, and Soluble Aerosol-Associated Ionic Species Over the Western Pacific: PEM West B

    NASA Technical Reports Server (NTRS)

    Didd, J. E.; Talbot, R. W.; Lefer, B. L.; Scheuer, E.; Gregory, G. L.; Browell, E. V.; Sandholm, S. T.; Singh, H. B.

    1997-01-01

    Aerosol sampling for the determination of the concentrations of soluble ionic species and the natural radionuclides Be-7 and Pb-210 was conducted from the NASA DC-8 over the western Pacific as part of GTE/PEM-West B during February - March 1994. Concentrations of most soluble ionic species in the free troposphere were higher in samples collected on flights originating from Hong Kong and Japan than those collected further east over the open ocean. In both regions the measured concentrations were higher than those found during PEM-West A (fall 1991). Activities of Pb-210 tracer of air masses influenced by sources on the Asian continent, showed the same patterns. These data indicate the effect of stronger continental outflow from Asia over the western Pacific during the spring compared to fall season. For readily scavenged aerosol-associated species and soluble acidic gases the strongest indications of Asian outflow were restricted to altitudes below 6 km. The distribution of the continental tracer Pb-210 was also compared to those of a large number of gas phase species measured on the DC-8. Relatively strong correlations were found with O3 and peroxyacetylnitrate (PAN), but only during the flights over the remote Pacific. During PEM-West A, similar correlations were seen, but they were stronger near Asia. We believe that these correlations are a signature of continental air that has been processed by deep wet convection over land before being advected over the ocean. One flight over the Sea of Japan provided the opportunity to sample upper troposphere/lower stratosphere air in and around a tropopause fold. Concentrations of Be-7 reached 7 pCi/cu m STP, and peak O3, mixing ratios of 480 ppb were encountered at 10.7 km. The Be-7 data are used to estimate the fraction of stratospheric air mixed down into the troposphere by circulation in the fold.

  11. Coupled Aerosol-Chemistry-Climate Twentieth-Century Transient Model Investigation: Trends in Short-Lived Species and Climate Responses

    NASA Technical Reports Server (NTRS)

    Koch, Dorothy; Bauer, Susanne E.; Del Genio, Anthony; Faluvegi, Greg; McConnell, Joseph R.; Menon, Surabi; Miller, Ronald L.; Rind, David; Ruedy, Reto; Schmidt, Gavin A.; Shindell, Drew

    2011-01-01

    The authors simulate transient twentieth-century climate in the Goddard Institute for Space Studies (GISS) GCM, with aerosol and ozone chemistry fully coupled to one another and to climate including a full dynamic ocean. Aerosols include sulfate, black carbon (BC), organic carbon, nitrate, sea salt, and dust. Direct and BC snow-albedo radiative effects are included. Model BC and sulfur trends agree fairly well with records from Greenland and European ice cores and with sulfur deposition in North America; however, the model underestimates the sulfur decline at the end of the century in Greenland. Global BC effects peak early in the century (1940s); afterward the BC effects decrease at high latitudes of the Northern Hemisphere but continue to increase at lower latitudes. The largest increase in aerosol optical depth occurs in the middle of the century (1940s-80s) when sulfate forcing peaks and causes global dimming. After this, aerosols decrease in eastern North America and northern Eurasia leading to regional positive forcing changes and brightening. These surface forcing changes have the correct trend but are too weak. Over the century, the net aerosol direct effect is -0.41 Watts per square meter, the BC-albedo effect is -0.02 Watts per square meter, and the net ozone forcing is +0.24 Watts per square meter. The model polar stratospheric ozone depletion develops, beginning in the 1970s. Concurrently, the sea salt load and negative radiative flux increase over the oceans around Antarctica. Net warming over the century is modeled fairly well; however, the model fails to capture the dynamics of the observedmidcentury cooling followed by the late century warming.Over the century, 20% of Arctic warming and snow ice cover loss is attributed to the BC albedo effect. However, the decrease in this effect at the end of the century contributes to Arctic cooling. To test the climate responses to sulfate and BC pollution, two experiments were branched from 1970 that removed

  12. Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

    NASA Astrophysics Data System (ADS)

    Faiola, C. L.; Wen, M.; VanReken, T. M.

    2015-04-01

    The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- and post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.

  13. Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

    DOE PAGES

    Faiola, C. L.; Wen, M.; VanReken, T. M.

    2015-04-01

    The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- andmore » post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.« less

  14. Water-soluble ions species of size-resolved aerosols: Implications for the atmospheric acidity in São Paulo megacity, Brazil

    NASA Astrophysics Data System (ADS)

    Vieira-Filho, Marcelo; Pedrotti, Jairo J.; Fornaro, Adalgiza

    2016-11-01

    Over the last decade, an increase of ammonium salts in atmospheric deposition has been reported worldwide, especially in megacities. The present study aims to give a better comprehension analysis about particulate matter acidity in São Paulo megacity (MASP), Brazil. Size-resolved aerosols were sampled in MASP, during 2012 winter, showing a bimodal mass concentration distribution, with sulfate concentration exceeding 3.40 μg m- 3, which accounted for over 25% of PM0.56 mass. Regarding the relative distribution of ionic species, 90% of NH4+ levels, were restricted to smaller than 1 μm diameter range. The average neutralization index for PM < 1 μm was 0.62, which indicated an ammonia-limiting atmosphere due to partial neutralization of atmospheric acids. Particles of the accumulation mode presented more acid behavior than other aerosol fractions, with pH value as low as 4.15 in PM0.56. The total neutralization index registered the lowest value for PM0.56, but it did not respond promptly to aerosol variations as the E-AIM model predictions. The highest discrepancies between the acidity proxies occurred in the smaller fractions of particulate matter, especially in the after-filter (AF) stage (diameter < 0.020 μm). In addition, AF stage had the highest contribution to PM total mass, about 14% for all the stages analyzed. Such contribution indicates that acidity in ultrafine particles are still mixed for the MASP and need further investigation.

  15. Identification of nitrogenous organic species in Titan aerosols analogs: Implication for prebiotic chemistry on Titan and early Earth

    NASA Astrophysics Data System (ADS)

    He, Chao; Smith, Mark A.

    2014-08-01

    Titan has a significant atmosphere composed primarily of nitrogen and methane with a significant organic haze component. Its nitrogen-rich atmosphere, abundant organics, and liquid surface make this moon of interest as a prebiotic laboratory at the planetary scale and one of the best targets for studying prebiotic planetary organic chemistry. In our previous work, we have investigated the chemical composition of Titan aerosol analogs (tholins) and identified a variety of nitrogenous organic molecules. Here we continue our structural investigation and identify four important prebiotic molecules in Titan tholins using NMR, GC-MS and standard sample comparison, including aminoacetonitrile, succinonitrile, acetoguanamine and adenine. On the basis of their structural characteristics, we suggest their formation pathways via simple precursors including methanimine (CH2NH), HCN, NH3, CH3CN and C2H2 in laboratory N2sbnd CH4 plasma or potentially in Titan’s atmosphere. Among these molecules, aminoacetonitrile is a potential precursor of amino acids and peptides, while adenine is a necessary ingredient for DNA and RNA. The identification of these molecules in Titan’s organic aerosol analogs increases our knowledge of Titan’s organic chemistry and its prebiotic implications.

  16. Organic aerosols and inorganic species from post-harvest agricultural-waste burning emissions over northern India: impact on mass absorption efficiency of elemental carbon.

    PubMed

    Rajput, Prashant; Sarin, M M; Sharma, Deepti; Singh, Darshan

    2014-01-01

    Atmospheric PM2.5 (particulate matter with aerodynamic diameter of ≤ 2.5 μm), collected from a source region [Patiala: 30.2 °N; 76.3 °E; 250 m above mean sea level] of emissions from post-harvest agricultural-waste (paddy-residue) burning in the Indo-Gangetic Plain (IGP), North India, has been studied for its chemical composition and impact on regional atmospheric radiative forcing. On average, organic aerosol mass accounts for 63% of PM2.5, whereas the contribution of elemental carbon (EC) is ∼3.5%. Sulphate, nitrate and ammonium contribute up to ∼85% of the total water-soluble inorganic species (WSIS), which constitutes ∼23% of PM2.5. The potassium-to-organic carbon ratio from paddy-residue burning emissions (KBB(+)/OC: 0.05 ± 0.01) is quite similar to that reported from Amazonian and Savanna forest-fires; whereas non-sea-salt-sulphate-to-OC ratio (nss-SO4(2-)/OC: 0.21) and nss-SO4(2-)/EC ratio of 2.6 are significantly higher (by factor of 5 to 8). The mass absorption efficiency of EC (3.8 ± 1.3 m(2) g(-1)) shows significant decrease with a parallel increase in the concentrations of organic aerosols and scattering species (sulphate and nitrate). A cross plot of OC/EC and nss-SO4(2-)/EC ratios show distinct differences for post-harvest burning emissions from paddy-residue as compared to those from fossil-fuel combustion sources in south-east Asia.

  17. 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.

  18. Cantera Aerosol Dynamics Simulator

    SciTech Connect

    Moffat, Harry

    2004-09-01

    The Cantera Aerosol Dynamics Simulator (CADS) package is a general library for aerosol modeling to address aerosol general dynamics, including formation from gas phase reactions, surface chemistry (growth and oxidation), bulk particle chemistry, transport by Brownian diffusion, thermophoresis, and diffusiophoresis with linkage to DSMC studies, and thermal radiative transport. The library is based upon Cantera, a C++ Cal Tech code that handles gas phase species transport, reaction, and thermodynamics. The method uses a discontinuous galerkin formulation for the condensation and coagulation operator that conserves particles, elements, and enthalpy up to round-off error. Both O-D and 1-D time dependent applications have been developed with the library. Multiple species in the solid phase are handled as well. The O-D application, called Tdcads (Time Dependent CADS) is distributed with the library. Tdcads can address both constant volume and constant pressure adiabatic homogeneous problems. An extensive set of sample problems for Tdcads is also provided.

  19. Stress-induced biogenic VOC emissions from typical European tree species, their impact on secondary organic aerosol formation and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Kleist, E.; Mentel, T. F.; Andres, S.; Dal Maso, M.; Hohaus, T.; Kindler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2011-12-01

    Biogenic volatile organic compounds (BVOC) are precursors of secondary organic aerosols (SOA), which can scatter and absorb radiation. BVOC therefore indirectly impact the Earth's climate. Earth's climate is projected to change, possibly putting and vegetation under stress due to intensive heat and drought periods. Such stress situations will alter BVOC emissions that may induce feedbacks between vegetation and climate change. The main aim of our study is to determine whether such effect exists. A first step was to determine the impacts of drought and heat on BVOC emissions and subsequent SOA formation. Experiments were performed in the Juelich plant atmosphere chamber. Pine and Spruce were taken as representatives for species exhibiting storage organs for monoterpenes (MT). Beech and Birch were used as species with MT emissions closely coupled to CO2 uptake. The plants were stored under well-defined conditions of temperature and light intensity. Heat stress was induced by increasing the chamber temperature; drought stress was induced by not irrigating the plants. A fraction of the air leaving the plant chamber was fed into a reaction chamber where SOA formation was induced by OH-initiated oxidation. During stress situations the plants' BVOC emissions changed significantly. As a general feature we found that combined heat and drought stress increased MT emissions from conifers but decreased MT emissions from the broadleaf species. The former was attributed to a heat-induced breakdown of storage organs. The latter was attributed to a general breakdown of biosynthetic activity. SOA formation potentials were changed together with the MT emissions. The decrease in SOA formation potential due to the decrease of MT emissions from broadleaf species was amplified by additional emissions of green leaf volatiles (GLV). Obviously, GLV can suppress SOA formation by suppressing OH concentrations. GLV were also emitted from the conifers under heat stress. However the

  20. 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.

  1. A thermoluminescent method for aerosol characterization

    NASA Technical Reports Server (NTRS)

    Long, E. R., Jr.; Rogowski, R. S.

    1976-01-01

    A thermoluminescent method has been used to study the interactions of aerosols with ozone. The preliminary results show that ozone reacts with many compounds found in aerosols, and that the thermoluminescence curves obtained from ozonated aerosols are characteristic of the aerosol. The results suggest several important applications of the thermoluminescent method: development of a detector for identification of effluent sources; a sensitive experimental tool for study of heterogeneous chemistry; evaluation of importance of aerosols in atmospheric chemistry; and study of formation of toxic, electronically excited species in airborne particles.

  2. Aerosol in the Pacific troposphere

    NASA Technical Reports Server (NTRS)

    Clarke, Antony D.

    1989-01-01

    The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

  3. Aerosolized Antibiotics.

    PubMed

    Restrepo, Marcos I; Keyt, Holly; Reyes, Luis F

    2015-06-01

    Administration of medications via aerosolization is potentially an ideal strategy to treat airway diseases. This delivery method ensures high concentrations of the medication in the targeted tissues, the airways, with generally lower systemic absorption and systemic adverse effects. Aerosolized antibiotics have been tested as treatment for bacterial infections in patients with cystic fibrosis (CF), non-CF bronchiectasis (NCFB), and ventilator-associated pneumonia (VAP). The most successful application of this to date is treatment of infections in patients with CF. It has been hypothesized that similar success would be seen in NCFB and in difficult-to-treat hospital-acquired infections such as VAP. This review summarizes the available evidence supporting the use of aerosolized antibiotics and addresses the specific considerations that clinicians should recognize when prescribing an aerosolized antibiotic for patients with CF, NCFB, and VAP.

  4. 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 ...

  5. Impact of clouds and precipitation on atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Andronache, Constantin

    2015-04-01

    Aerosols have a significant impact on the dynamics and microphysics of continental mixed-phase convective clouds. High aerosol concentrations provide enhanced cloud condensation nuclei that can lead to the invigoration of convection and increase of surface rainfall. Such effects are dependent on environmental conditions and aerosol properties. Clouds are not only affected by aerosol, they also alter aerosol properties by various processes. Cloud processing of aerosol includes: convective redistribution, modification in the number and size of aerosol particles, chemical processing, new particle formation around clouds, and aerosol removal by rainfall to the surface. Among these processes, the wet removal during intense rain events, in polluted continental regions, can lead to spikes in acidic deposition into environment. In this study, we address the effects of clouds and precipitation on the aerosol distribution in cases of convective precipitation events in eastern US. We examine the effects of clouds and precipitation on various aerosol species, as well as their temporal and spatial variability.

  6. Influence of aerosol vertical distribution on radiative budget and climate

    NASA Astrophysics Data System (ADS)

    Nabat, Pierre; Michou, Martine; Saint-Martin, David; Watson, Laura

    2016-04-01

    Aerosols interact with shortwave and longwave radiation with ensuing consequences on radiative budget and climate. Aerosols are represented in climate models either using an interactive aerosol scheme including prognostic aerosol variables, or using climatologies, such as monthly aerosol optical depth (AOD) fields. In the first case, aerosol vertical distribution can vary rapidly, at a daily or even hourly scale, following the aerosol evolution calculated by the interactive scheme. On the contrary, in the second case, a fixed aerosol vertical distribution is generally imposed by climatological profiles. The objective of this work is to study the impact of aerosol vertical distribution on aerosol radiative forcing, with ensuing effects on climate. Simulations have thus been carried out using CNRM-CM, which is a global climate model including an interactive aerosol scheme representing the five main aerosol species (desert dust, sea-salt, sulfate, black carbon and organic matter). Several multi-annual simulations covering the past recent years are compared, including either the prognostic aerosol variables, or monthly AOD fields with different aerosol vertical distributions. In the second case, AOD fields directly come from the first simulation, so that all simulations have the same integrated aerosol loads. The results show that modifying the aerosol vertical distribution has a significant impact on radiative budget, with consequences on global climate. These differences, highlighting the importance of aerosol vertical distribution in climate models, probably come from the modification of atmospheric circulation induced by changes in the heights of the different aerosols. Besides, nonlinear effects in the superposition of aerosol and clouds reinforce the impact of aerosol vertical distribution, since aerosol radiative forcing depends highly upon the presence of clouds, and upon the relative vertical position of aerosols and clouds.

  7. Reactive Oxygen Species Production Mediated by Humic-like Substances in Atmospheric Aerosols: Enhancement Effects by Pyridine, Imidazole, and Their Derivatives.

    PubMed

    Dou, Jing; Lin, Peng; Kuang, Bin-Yu; Yu, Jian Zhen

    2015-06-01

    Ambient particulate matter (PM) can cause adverse health effects via their ability to produce reactive oxygen species (ROS). Humic-like substances (HULIS), a complex mixture of amphiphilic organic compounds, have been demonstrated to contain the majority of redox activity in the water-extractable organic fraction of PM. Reduced organic nitrogen compounds, such as alkaloids resulting from biomass burning emissions, are among HULIS constituents. In this study, we examined the redox activities of pyridine, imidazole and their alkyl derivatives using a cell-free dithiothreitol (DTT) assay under simulated physiological conditions (37 °C, pH = 7.40). These compounds were found to have little redox activity on their own as measured by the DTT assay, but they enhanced ROS generation catalyzed by 1,4-naphthoquinone (as a model quinone compound) and HULIS isolated from multiple aerosol samples. The enhancement effect by the individual nitrogen-containing bases was determined to be proportional to their amount in the assay solutions. It is postulated that the underlying mechanism involves the unprotonated N atom acting as a H-bonding acceptor to facilitate hydrogen-atom transfer in the ROS generation cycle. The enhancement capability was found to increase with their basicity (i.e., pKa of their conjugated acids, BH(+)), consistent with the proposed mechanism for enhancement. Among the imidazole homologues, a linear relationship was observed between the enhancement factors (in log scale) of the unprotonated form of the imidazole compounds (B) and the pKa of their conjugated acids (BH(+)). This relationship predicts that the range of alkylimidazole homologues (C6-C13) observed in atmospheric HULIS would be 1.5-4.4 times more effective than imidazole in facilitating HULIS-mediated ROS generation. Our work reveals that the ability of atmospheric PM organics to catalyze generation of ROS in cells could be affected by coexisting redox inactive organic constituents and suggests

  8. Inorganic Components of Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Wexler, Anthony Stein

    The inorganic components comprise 15% to 50% of the mass of atmospheric aerosols. For about the past 10 years the mass of these components was predicted assuming thermodynamic equilibrium between the volatile aerosol -phase inorganic species NH_4NO _3 and NH_4Cl and their gas-phase counterparts NH_3, HNO_3, and HCl. In this thesis I examine this assumption and prove that (1) the time scales for equilibration between the gas and aerosol phases are often too long for equilibrium to hold, and (2) even when equilibrium holds, transport considerations often govern the size distribution of these aerosol components. Water can comprise a significant portion of atmospheric aerosols under conditions of high relative humidity, whereas under conditions of sufficiently low relative humidity atmospheric aerosols tend to be dry. The deliquescence point is the relative humidity where the aerosol goes from a solid dry phase to an aqueous or mixed solid-aqueous phase. In this thesis I derive the temperature dependence of the deliquescence point and prove that in multicomponent solutions the deliquescence point is lower than for corresponding single component solutions. These theories of the transport, thermodynamic, and deliquescent properties of atmospheric aerosols are integrated into an aerosol inorganics model, AIM. The predictions of AIM compare well to fundamental thermodynamic measurements. Comparison of the prediction of AIM to those of other aerosol equilibrium models shows substantial disagreement in the predicted water content at lower relative humidities. The disagreement is due the improved treatment in AIM of the deliquescence properties of multicomponent solutions. In the summer and fall of 1987 the California Air Resources Board conducted the Southern California Air Quality Study, SCAQS, during which atmospheric aerosols were measured in Los Angeles. The size and composition of the aerosol and the concentrations of their gas phase counterparts were measured. When the

  9. Characterization of water-soluble species of PM10 and PM2.5 aerosols in urban area in Nanjing, China

    NASA Astrophysics Data System (ADS)

    Wang, Gehui; Huang, Liming; Gao, Shixiang; Gao, Songting; Wang, Liansheng

    The characterization for water-soluble species of PM10 (particle matter with aerodynamical diameter <10 μm) and PM2.5 (particle matter with aerodynamical diameter <2.5 μm) in five sites of Nanjing, China was carried out during February-May 2001.The pH and conductivity K of water-soluble matters of PM10 and PM2.5 were determined, and the water-soluble fraction of the sample was followed to identify the total carbon (TC), total organic carbon (TOC), inorganic carbon (IC), elements, NO 3-, SO 42- and NH 3-N.The experimental results show that water-soluble matters of PM10 and PM2.5 in Nanjing are acidic, and the pH of PM2.5 is lower than PM10. Conductivity of water-soluble species of PM10 and PM2.5 aerosols varied over a wide range from 1087 to 225 μs/cm. Conductivity between PM10 and PM2.5 has a linear correlationship, and the equation is Y=0.8459 X+44.74, r2=0.9376 ( Y: conductivity of PM2.5, X: conductivity of PM10). TOC make up the majority of TC and accounts for 3.17-14.13% of PM10 and/or PM2.5 loadings, while IC only accounts for 0.12-0.47% of PM10 and/or PM2.5 mass. Al, As, Ba, Ca, Cr, Cu, Fe, K, Li, Mg, Mn, Na, Ni, Pb, Ti, V and Zn, 17 elements were detected in water-soluble matters of PM10 and/or PM2.5. Ca, K and Na are the most abundant chemical components, which account for more than 95% of total water-soluble elements (TWSE). Of all the five sites, TWSE accounts for 1.80-6.13% of the particle mass and 61.28-72.73% of TWSE of PM10 is enriched in fine particles (<2.5 μm in diameter). Nitrate (NO 3-), sulfate (SO 42-), ammonia and ammonium (NH 3-N) were determined. The highest level of nitrate was 15.49 μg/m 3 for PM10 and 12.66 μg/m 3 for PM2.5 at site FZ. As was the case for nitrate, the highest level of sulfate was also presented at the same site, which was 28.22 μg/m 3 for PM10 and 21.48 μg/m 3 for PM2.5. However, a higher level of ammonia and ammonium was presented at site ZS, which was 36.05 μg/m 3 for PM10 and 22.06 μg/m 3 for PM2.5.

  10. Mycobacterial Aerosols and Respiratory Disease

    PubMed Central

    2003-01-01

    Environmental opportunistic mycobacteria, including Mycobacterium avium, M. terrae, and the new species M. immunogenum, have been implicated in outbreaks of hypersensitivity pneumonitis or respiratory problems in a wide variety of settings. One common feature of the outbreaks has been exposure to aerosols. Aerosols have been generated from metalworking fluid during machining and grinding operations as well as from indoor swimming pools, hot tubs, and water-damaged buildings. Environmental opportunistic mycobacteria are present in drinking water, resistant to disinfection, able to provoke inflammatory reactions, and readily aerosolized. In all outbreaks, the water sources of the aerosols were disinfected. Disinfection may select for the predominance and growth of mycobacteria. Therefore, mycobacteria may be responsible, in part, for many outbreaks of hypersensitivity pneumonitis and other respiratory problems in the workplace and home. PMID:12890314

  11. Cantera Aerosol Dynamics Simulator

    2004-09-01

    The Cantera Aerosol Dynamics Simulator (CADS) package is a general library for aerosol modeling to address aerosol general dynamics, including formation from gas phase reactions, surface chemistry (growth and oxidation), bulk particle chemistry, transport by Brownian diffusion, thermophoresis, and diffusiophoresis with linkage to DSMC studies, and thermal radiative transport. The library is based upon Cantera, a C++ Cal Tech code that handles gas phase species transport, reaction, and thermodynamics. The method uses a discontinuous galerkinmore » formulation for the condensation and coagulation operator that conserves particles, elements, and enthalpy up to round-off error. Both O-D and 1-D time dependent applications have been developed with the library. Multiple species in the solid phase are handled as well. The O-D application, called Tdcads (Time Dependent CADS) is distributed with the library. Tdcads can address both constant volume and constant pressure adiabatic homogeneous problems. An extensive set of sample problems for Tdcads is also provided.« less

  12. [Aerosol therapy].

    PubMed

    Wildhaber, J H

    1998-08-15

    Aerosol therapy plays a major role in the diagnosis and treatment of various lung diseases. The aim of inhalation therapy is to deposit a reproducible and adequate dose of a specific drug to the airways, in order to achieve a high, local, clinical effect while avoiding serious systemic side effects. To achieve this goal, it is therefore important to have an efficient inhalation device to deliver different medications. However, the currently available therapeutic inhalation devices (nebuliser, pressurised metered-dose inhaler and dry powder inhaler) are not very efficient in aerosol delivery and have several disadvantages. Inhalation devices can be assessed by in vitro studies, filter studies and radiolabelled deposition studies. Several radiolabelled deposition studies have shown that nebulisers and pressurised metered-dose inhalers are not very efficient in aerosol delivery. In children, before 1997, only 0.5% to 15% of the total nebulised or actuated dose from a nebuliser or pressurised metered-dose inhaler actually reached the lungs. These numbers were somewhat improved in adults, 30% of the total nebulised or actuated dose reaching the airways. Aerosol therapy with dry powder inhalers was the most efficient before 1997, 30% of the total dose being deposited in the lungs of adults and children. In 1997, new developments in pressurised metered-dose inhalers much improved their efficiency in aerosol delivery. Lung deposition can be increased by up to 60% with use of a non-electrostatic holding chamber and/or a pressurised metered-dose inhaler with a hydrofluoroalkane propellant possessing superior aerosol characteristics. Several studies comparing the clinical efficiency of different inhalation devices have shown that the choice of an optimal inhalation device is crucial. In addition to the aerosol characteristics, ventilation parameters and airway morphology have an important bearing on deposition patterns. These parameters may be greatly influenced by the

  13. An Investigation of Aerosol and Ozone Measurements from the Cryogenic Limb Array Etalon Spectrometer: Validation and Relation to Other Chemical Species

    NASA Technical Reports Server (NTRS)

    Deshler, Terry

    1997-01-01

    Throughout this study we focused on comparisons of CLAES and in situ measurements of ozone and aerosol extinction. Thus the comparison is between satellite data representative of large spatial regions and in situ data representative of nearly point samples. Both instruments provide vertical profiles, but the region of overlap is limited to between approximately 10 and 100 mb. CLAES Version 7 ozone measurements have been compared to electrochemical cell ozonesonde measurements over McMurdo Station, Antarctica (78 deg S, 167 deg E), Dumont d'Urville, Antarctica (66.7 deg S, 140 deg E), Laramie, Wyoming (41 deg N, 106 deg W), and Bear Island, Norway (74.3 deg N, 19 deg E). Comparisons were made between vertical ozone profiles, and between integrated column ozone over the region of overlap of the measurements. Comparisons using CLAES Version 8 data are underway. CLAES Version 8 aerosol extinction measurements at all wavelengths have also been compared to University of Wyoming aerosol extinctions over McMurdo Station, Antarctica, and over Laramie, Wyoming. Coincidences in all cases were determined by minimizing the distance between the CLAES observations and the surface station, and the time separation between the satellite and in situ measurements.

  14. Water-soluble species in the marine aerosol from the northern South China Sea: High chloride depletion related to air pollution

    NASA Astrophysics Data System (ADS)

    Hsu, Shih-Chieh; Liu, Shaw Chen; Kao, Shuh-Ji; Jeng, Woei-Lih; Huang, Yi-Tang; Tseng, Chun-Mao; Tsai, Fujung; Tu, Jien-Yi; Yang, Yih

    2007-10-01

    Dichotomous (PM2.5-10 and PM2.5 modes) and size-resolved marine aerosols collected during the northeastern monsoon on two wintertime cruises in the subtropical South China Sea (SCS) were analyzed for water-soluble ions. During the sampling periods the study region was under the influence of strong pollution originating primarily from the Asian continent. Elevated levels of non-sea-salt sulfate and ammonium ions of up to 4.5 and 1.2 μg/m3, respectively, were observed, indicating that the SCS is now substantially contaminated by massive amounts of air pollutants most likely from China and South/Southeast Asia. The non-sea-salt sulfate to nitrate mass ratios reaching 3.8 ± 1.9 are much larger than those (approximately 2) in and around East Asia and the western Pacific Ocean, suggesting that the Asian outflow aerosols measured in the SCS experienced different traveling history from those in the vicinity of source regions. High chloride depletion (Cl-depletion) measured in the SCS marine aerosols was, on average, 30% for coarse-mode particles and nearly 90% for fine-mode particles. Cl-depletion is size-dependent, and maximizes in submicrometer particles (i.e., Cl has almost been completely lost). Acid displacement is responsible for the observed high Cl-depletion: nitrate substitution accounts for the coarse-mode depletion, whereas sulfate substitution accounts for the fine-mode depletion. The acid displacement of sea salt aerosols may be related to a variety of factors, especially the substantial air pollution, which is discussed in detail in this paper. On cloudy/rainy days, fine-mode aerosol samples have moderate Cl-depletion (i.e., ˜40-50%), in contrast to nearly complete Cl loss on sunny days, presumably indicating that photochemical reactions would play a key role in the Cl-deficit; however, it merits further investigation as the available samples were limited.

  15. Toxicity of atmospheric aerosols on marine phytoplankton

    USGS Publications Warehouse

    Paytan, A.; Mackey, K.R.M.; Chen, Y.; Lima, I.D.; Doney, S.C.; Mahowald, N.; Labiosa, R.; Post, A.F.

    2009-01-01

    Atmospheric aerosol deposition is an important source of nutrients and trace metals to the open ocean that can enhance ocean productivity and carbon sequestration and thus influence atmospheric carbon dioxide concentrations and climate. Using aerosol samples from different back trajectories in incubation experiments with natural communities, we demonstrate that the response of phytoplankton growth to aerosol additions depends on specific components in aerosols and differs across phytoplankton species. Aerosol additions enhanced growth by releasing nitrogen and phosphorus, but not all aerosols stimulated growth. Toxic effects were observed with some aerosols, where the toxicity affected picoeukaryotes and Synechococcus but not Prochlorococcus.We suggest that the toxicity could be due to high copper concentrations in these aerosols and support this by laboratory copper toxicity tests preformed with Synechococcus cultures. However, it is possible that other elements present in the aerosols or unknown synergistic effects between these elements could have also contributed to the toxic effect. Anthropogenic emissions are increasing atmospheric copper deposition sharply, and based on coupled atmosphere-ocean calculations, we show that this deposition can potentially alter patterns of marine primary production and community structure in high aerosol, low chlorophyll areas, particularly in the Bay of Bengal and downwind of South and East Asia.

  16. Global measurements of gaseous and aerosol trace species in the upper troposphere and lower stratosphere from daily flights of 747 airliners

    NASA Technical Reports Server (NTRS)

    Perkins, P. J.

    1976-01-01

    Extensive measurements include ozone, carbon monoxide, water vapor, and aerosol and condensation nuclei number density. Less extensive measurements include chlorofluoromethanes, sulfates and nitrates. Certain meteorological and flight information are also recorded at the time of these measurements. World routes range in latitude from about 60 deg N near North America to about 40 deg S over Australia and 23 deg S over South America. Typical data show significant changes in ozone, carbon monoxide, and water vapor when crossing the tropopause either during changes in altitude or at cruise altitude. These gases as well as light scattering particles and condensation nuclei exhibit considerable variability along a flight route.

  17. Measurements of Acidic Gases and Aerosol Species Aboard the NASA DC-8 Aircraft During the Pacific Exploratory Mission in the Tropics (PEM-Tropics A)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    1999-01-01

    We received funding to provide measurements of nitric acid (HNO3), formic acid (HCOOH), acetic acid (CH3COOH), and the chemical composition of aerosols aboard the NASA Ames DC-8 research aircraft during the PEM-Tropics A mission. These measurements were successfully completed and the final data resides in the electronic archive (ftp-gte.larc.nasa.gov) at NASA Langley Research Center. For the PEM-Tropics A mission the University of New Hampshire group was first author of four different manuscripts. Three of these have now appeared in the Journal of Geophysical Research-Atmospheres, included in the two section sections on PEM-Tropics A. The fourth manuscript has just recently been submitted to this same journal as a stand alone paper. All four of these papers are included in this report. The first paper (Influence of biomass combustion emissions on the distribution of acidic trace gases over the Southern Pacific basin during austral springtime) describes the large-scale distributions of HNO3, HCOOH, and CH3COOH. Arguments were presented to show, particularly in the middle tropospheric region, that biomass burning emissions from South America and Africa were a major source of acidic gases over the South Pacific basin. The second paper (Aerosol chemical composition and distribution during the Pacific Exploratory Mission (PEM) Tropics) covers the aerosol aspects of our measurement package. Compared to acidic gases, O3, and selected hydrocarbons, the aerosol chemistry showed little influence from biomass burning emissions. The data collected in the marine boundary layer showed a possible marine source of NH3 to the troposphere in equatorial areas. This source had been speculated on previously, but our data was the first collected from an airborne platform to show its large-scale features. The third paper (Constraints on the age and dilution of Pacific Exploratory Mission-Tropics biomass burning plumes from the natural radionuclide tracer Pb-210) utilized the unexpectedly

  18. Identification of oxidized organic atmospheric species during the Southern Oxidant and Aerosol Study (SOAS) using a novel Ion Mobility Time-of-Flight Chemical Ionization Mass Spectrometer (IMS-ToF-CIMS)

    NASA Astrophysics Data System (ADS)

    Krechmer, J.; Canagaratna, M.; Kimmel, J.; Junninen, H.; Knochenmuss, R.; Cubison, M.; Massoli, P.; Stark, H.; Jayne, J. T.; Surratt, J. D.; Jimenez, J. L.; Worsnop, D. R.

    2013-12-01

    We present results from the field deployment of a novel Ion Mobility Time-of-flight Chemical Ionization Mass Spectrometer (CI-IMS-TOF) during the Southern Oxidant and Aerosol Study (SOAS). IMS-TOF is a 2-dimensional analysis method, which separates gas-phase ions by mobility prior to determination of mass-to-charge ratio by mass spectrometry. Ion mobility is a unique physical property that is determined by the collisional cross section of an ion. Because mobility depends on size and shape, the IMS measurement is able to resolve isomers and isobaric compounds. Additionally, trends in IMS-TOF data space can be used to identify relationships between ions, such as common functionality or polymeric series. During SOAS we interfaced the IMS-TOF to a nitrate ion (NO3-) chemical ionization source that enables the selective ionization of highly oxidized gas phase species (those having a high O:C ratio) through clustering with the reagent ion. Highly oxidized products of terpenes and isoprene are important secondary organic aerosol precursors (SOA) that play an uncertain but important role in particle-phase chemistry. We present several case studies of atmospheric events during SOAS that exhibited elevated concentrations of sulfuric acid and/or organics. These events exhibited a rise in particle number and provide an opportunity to examine the role that organic species may have in local atmospheric new particle formation events. We also present the results from the field deployment and subsequent laboratory studies utilizing a Potential Aerosol Mass (PAM) flow reactor as the inlet for the CI-IMS-TOF. The reactor draws in ambient air and exposes it to high concentrations of the OH radical, created by photolysis O3 in the presence of water. The highly oxidized products are then sampled directly by the CI-IMS-TOF. We performed several experiments including placing pine and deciduous plants directly in front of the reactor opening and observed large increases in the number and

  19. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3− aerosol during the 2013 Southern Oxidant and Aerosol Study

    DOE PAGES

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; Ault, A.; Bondy, A.; Takahama, S.; Modini, R. L.; Baumann, K.; Edgerton, E.; Knote, C.; et al

    2015-09-25

    Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3−) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3more » and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3− is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3− and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.« less

  20. Longwave radiative forcing by aqueous aerosols

    SciTech Connect

    Gaffney, J.S.; Marley, N.A.

    1995-01-01

    Recently, a great deal of interest has been focused on the role of aerosols in climatic change because of their potential cooling impacts due to light scattering. Recent advances in infrared spectroscopy using cylindrical internal reflectance have allowed the longwave absorption of dissolved aerosol species and the associated liquid water to be accurately determined and evaluated. Experimental measurements using these techniques have shown that dissolved sulfate, nitrate, and numerous other aerosol species will act to cause greenhouse effects. Preliminary calculations indicate that the longwave climate forcing (i.e., heating) for sulfate aerosol will be comparable in magnitude to the cooling effect produced by light scattering. However, more detailed modeling will clearly be needed to address the impact of the longwave forcing due to aerosols as a function of atmospheric height and composition. Their work has shown that aerosol composition will be important in determining longwave forcing, while shortwave forcing will be more related to the physical size of the aerosol droplets. On the basis of these studies, it is increasingly apparent that aerosols, fogs, and clouds play a key role in determining the radiative balance of the atmosphere and in controlling regional and global climates.

  1. How We Can Constrain Aerosol Type Globally

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph

    2016-01-01

    species-specific aerosol mass and size that are tracked in aerosol transport and climate models used to assess aerosol forcing and its anthropogenic components. This presentation will summarize where we stand on the development of the SAM-CAAM concept.

  2. Sulfur speciation in individual aerosol particles

    NASA Astrophysics Data System (ADS)

    Neubauer, Kenneth R.; Sum, Stephen T.; Johnston, Murray V.; Wexler, Anthony S.

    1996-08-01

    Sulfur aerosols play an important role in acid deposition and the Earth's energy balance. Important species in these aerosols include methanesulfonates, hydroxymethanesulfonates, sulfates, and sulfites. Because the relative amounts of these species indicate different sources and atmospheric processes, it is important to distinguish them in single-aerosol particles. To accomplish this task, we use rapid single-particle mass spectrometry (RSMS), a technique that permits individual particles to be analyzed in an online mode. Each sulfur species produces a characteristic set of ions in the mass spectra. In simulated marine and urban aerosols the relative amounts of methanesulfonic acid (MSA) and sodium hydroxymethanesulfonate (NaHMSA) in a single particle can be determined from peak area ratios in the mass spectra. Improved quantitation is possible by application of the classification and regression tree (CART) algorithm to distinguish the mass spectra of particles having different compositions. Factors that influence speciation include particle size, morphology, and laser fluence.

  3. Acquisition of in-situ and remote sensors for measurements of aerosols and chemical species. Final report, 12 December 1994-30 November 1996

    SciTech Connect

    Clarke, A.D.; Sharma, S.K.; Porter, J.N.

    1997-02-26

    Under this grant, the University of Hawaii has acquired instrumentation to relate remotely sensed lidar backscatter signals to both in situ measurements and to satellite derived radiances. These instruments include a turn key pulsed Nd:YAG and Ti-sapphire tunable laser transmitter and 12` lidar scanner, that are now part of SOEST scanning lidar system. The in situ characterization instrumentation package includes forward scattering spectrometer probe (FSSP), GPS receiver, and a portable satellite receiving station that would be deployed with lidar and in situ measurements to extend the range of observations and put these in broader context. These instruments are currently being used for studying coastal marine aerosols as a function of meteorological conditions on the island of Oahu.

  4. Subarctic atmospheric aerosol composition: 1. Ambient aerosol characterization

    SciTech Connect

    Friedman, Beth; Herich, Hanna; Kammermann, Lukas; Gross, Deborah S.; Ameth, Almut; Holst, Thomas; Lohmann, U.; Cziczo, Daniel J.

    2009-07-10

    Sub-Arctic aerosol was sampled during July 2007 at the Abisko Research Station Stordalen field site operated by the Royal Swedish Academy of Sciences. Located in northern Sweden at 68º latitude and 385 meters above sea level (msl), this site is classified as a semi-continuous permafrost mire. Number density, size distribution, cloud condensation nucleus properties, and chemical composition of the ambient aerosol were determined. Backtrajectories showed that three distinct airmasses were present over Stordalen during the sampling period. Aerosol properties changed and correlated with airmass origin to the south, northeast, or west. We observe that Arctic aerosol is not compositionally unlike that found in the free troposphere at mid-latitudes. Internal mixtures of sulfates and organics, many on insoluble biomass burning and/or elemental carbon cores, dominate the number density of particles from ~200 to 2000 nm aerodynamic diameter. Mineral dust which had taken up gas phase species was observed in all airmasses. Sea salt, and the extent to which it had lost volatile components, was the aerosol type that most varied with airmass.

  5. Aerosol volatility in a boreal forest environment

    NASA Astrophysics Data System (ADS)

    Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

    2012-04-01

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

  6. Characterization of Speciated Aerosol Direct Radiative Forcing Over California

    SciTech Connect

    Zhao, Chun; Leung, Lai-Yung R.; Easter, Richard C.; Hand, Jenny; Avise, J.

    2013-03-16

    A fully coupled meteorology-chemistry model (WRF-Chem) with added capability of diagnosing the spatial and seasonal distribution of radiative forcings for individual aerosol species over California is used to characterize the radiative forcing of speciated aerosols in California. Model simulations for the year of 2005 are evaluated with various observations including meteorological data from California Irrigation Management Information System (CIMIS), aerosol mass concentrations from US EPA Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE), and aerosol optical depth from AErosol RObotic NETwork (AERONET) and satellites. The model well captures the observed seasonal meteorological conditions over California. Overall, the simulation is able to reproduce the observed spatial and seasonal distribution of mass concentration of total PM2.5 and the relative contribution from individual aerosol species, except the model significantly underestimates the surface concentrations of organic matter (OM) and elemental carbon (EC), potentially due to uncertainty in the anthropogenic emissions of OM and EC and the outdated secondary organic aerosol mechanism used in the model. A sensitivity simulation with anthropogenic EC emission doubled significantly reduces the model low bias of EC. The simulation reveals high anthropogenic aerosol loading over the Central Valley and the Los Angeles metropolitan regions and high natural aerosol (dust) loading over southeastern California. The seasonality of aerosol surface concentration is mainly determined by vertical turbulent mixing, ventilation, and photochemical activity, with distinct characteristics for individual aerosol species and between urban and rural areas. The simulations show that anthropogenic aerosols dominate the aerosol optical depth (AOD). The ratio of AOD to AAOD (aerosol absorption optical depth) shows distinct seasonality with a winter maximum and a summer minimum

  7. Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

    2015-12-01

    The German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new

  8. Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

    NASA Astrophysics Data System (ADS)

    McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

    2011-09-01

    Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

  9. Global Atmospheric Aerosol Modeling

    NASA Technical Reports Server (NTRS)

    Hendricks, Johannes; Aquila, Valentina; Righi, Mattia

    2012-01-01

    Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models.

  10. Light Absorbing Aerosols in Mexico City

    NASA Astrophysics Data System (ADS)

    Marley, N. A.; Kelley, K. L.; Kilaparty, P. S.; Gaffney, J. S.

    2008-12-01

    The direct effects of aerosol radiative forcing has been identified by the IPCC as a major uncertainty in climate modeling. The DOE Megacity Aerosol Experiment-Mexico City (MAX-Mex), as part of the MILAGRO study in March of 2006, was undertaken to reduce these uncertainties by characterization of the optical, chemical, and physical properties of atmospheric aerosols emitted from this megacity environment. Aerosol samples collected during this study using quartz filters were characterized in the uv-visible-infrared by using surface spectroscopic techniques. These included the use of an integrating sphere approach combined with the use of Kubelka-Munk theory to obtain aerosol absorption spectra. In past work black carbon has been assumed to be the only major absorbing species in atmospheric aerosols with an broad band spectral profile that follows a simple inverse wavelength dependence. Recent work has also identified a number of other absorbing species that can also add to the overall aerosol absorption. These include primary organics from biomass and trash burning and secondary organic aerosols including nitrated PAHs and humic-like substances, or HULIS. By using surface diffuse reflection spectroscopy we have also obtained spectra in the infrared that indicate significant IR absorption in the atmospheric window-region. These data will be presented and compared to spectra of model compounds that allow for evaluation of the potential importance of these species in adding strength to the direct radiative forcing of atmospheric aerosols. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64327 as part of the Atmospheric Science Program.

  11. Aerosol gels

    NASA Technical Reports Server (NTRS)

    Sorensen, Christopher M. (Inventor); Chakrabarti, Amitabha (Inventor); Dhaubhadel, Rajan (Inventor); Gerving, Corey (Inventor)

    2010-01-01

    An improved process for the production of ultralow density, high specific surface area gel products is provided which comprises providing, in an enclosed chamber, a mixture made up of small particles of material suspended in gas; the particles are then caused to aggregate in the chamber to form ramified fractal aggregate gels. The particles should have a radius (a) of up to about 50 nm and the aerosol should have a volume fraction (f.sub.v) of at least 10.sup.-4. In preferred practice, the mixture is created by a spark-induced explosion of a precursor material (e.g., a hydrocarbon) and oxygen within the chamber. New compositions of matter are disclosed having densities below 3.0 mg/cc.

  12. Global Aerosol Distributions Derived From the CALIPSO Observations

    NASA Astrophysics Data System (ADS)

    Kittaka, C.; Winker, D.; Omar, A.; Liu, Z.; Vaughan, M.; Trepte, C.

    2008-12-01

    Since June 2006, CALIPSO continues to provide routine and systematic measurements of lidar backscatter at two wavelengths, 532 and 1064 nm. As an active sensor, the quality of the measurement is nearly insensitive to surface properties allowing quantitative measurements in regions that are problematic to passive sensors. In particular, aerosol and cloud observations in the polar regions and desert areas are possible with the CALIPSO lidar through the different seasons of a year. The CALIPSO level 2 products, which include aerosol and cloud vertical profiles along tracks, reveal, for the first time, the multi-layer structure of aerosols and clouds on a global scale. This allows not only a depiction of aerosols in relation to clouds, but also the investigation of the interaction between aerosols and clouds. In this study, we present global distributions of aerosol in terms of season, layer height, aerosol species, and in relation to clouds using two years of CALIPSO observations. The CALIPSO aerosol extinction data sets under clear sky are evaluated against the AERONET aerosol optical depth (AOD) and the MODIS AOD collection 5 data sets. The agreement and discrepancies from these comparisons are characterized regionally and investigated using other CALIPSO observable and retrieved parameters. Furthermore, aerosols above clouds and in the vicinity of clouds are examined on a global scale. The implications for aerosol radiative forcing are discussed, highlighting the new and interesting aerosol features obtained from CALIPSO observations.

  13. Aerosol typing - key information from aerosol studies

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  14. Measurements of nitric acid, carboxylic acids, and selected aerosol species for the NASA/GTE Pacific Mission - West (PEM-WEST)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    1993-01-01

    The research investigation funded through this grant to the University of New Hampshire was performed during a major field expedition conducted by the NASA Tropospheric Chemistry Program. The NASA Global Tropospheric Experiment (GTE) executed an airborne science mission (PEM-WEST A) aboard the NASA Ames DC-8 over the Pacific Ocean during Sep./Oct. 1981. The atmosphere over the central Pacific Ocean is the only major region in the Northern Hemisphere that is relatively free from direct anthropogenic influence. Thus, this environment is ideally suited to study the natural biogeochemical cycles of carbon, nitrogen, ozone, sulfur, and aerosols without serious confounding problems related to anthropogenic emissions. Asian sources account for about 17 percent of the global budgets of nitrogen oxides (NO(x)) and sulfur dioxide (SO2). The Pacific Rim region therefore provides the opportunity to study the anthropogenic impact on natural atmospheric chemical cycles. The PEM-WEST A flights were focused on contrasting the chemistry of 'clean' air over the central Pacific with anthropogenically impacted air advected off the Asian continent. The principal objectives of PEM-WEST A were to investigate the atmospheric chemistry of ozone (O3) and its precursors, and to study important aspects of the atmospheric sulfur cycle over the western Pacific Ocean. Measurements conducted by the University of New Hampshire contributed directly to both of these objectives. Subsequent PEM-WEST field missions are planned by GTE in the mid-1990's to contrast atmospheric chemistry documented during PEM-WEST A with other time periods. This report presents preliminary findings from the PEM-WEST A field mission. Data interpretation is currently ongoing with the goal of manuscript submission of scientific results to a special issue of the Journal of Geophysical Research-Atmospheres in Feb. 1994. The reader is strongly encouraged to review this suite of profession articles to appreciate the overall

  15. Aerosol mobility size spectrometer

    DOEpatents

    Wang, Jian; Kulkarni, Pramod

    2007-11-20

    A device for measuring aerosol size distribution within a sample containing aerosol particles. The device generally includes a spectrometer housing defining an interior chamber and a camera for recording aerosol size streams exiting the chamber. The housing includes an inlet for introducing a flow medium into the chamber in a flow direction, an aerosol injection port adjacent the inlet for introducing a charged aerosol sample into the chamber, a separation section for applying an electric field to the aerosol sample across the flow direction and an outlet opposite the inlet. In the separation section, the aerosol sample becomes entrained in the flow medium and the aerosol particles within the aerosol sample are separated by size into a plurality of aerosol flow streams under the influence of the electric field. The camera is disposed adjacent the housing outlet for optically detecting a relative position of at least one aerosol flow stream exiting the outlet and for optically detecting the number of aerosol particles within the at least one aerosol flow stream.

  16. Experimental Technique for Studying Aerosols of Lyophilized Bacteria

    PubMed Central

    Cox, Christopher S.; Derr, John S.; Flurie, Eugene G.; Roderick, Roger C.

    1970-01-01

    An experimental technique is presented for studying aerosols generated from lyophilized bacteria by using Escherichia coli B, Bacillus subtilis var. niger, Enterobacter aerogenes, and Pasteurella tularensis. An aerosol generator capable of creating fine particle aerosols of small quantities (10 mg) of lyophilized powder under controlled conditions of exposure to the atmosphere is described. The physical properties of the aerosols are investigated as to the distribution of number of aerosol particles with particle size as well as to the distribution of number of bacteria with particle size. Biologically unstable vegetative cells were quantitated physically by using 14C and Europium chelate stain as tracers, whereas the stable heat-shocked B. subtilis spores were assayed biologically. The physical persistence of the lyophilized B. subtilis aerosol is investigated as a function of size of spore-containing particles. The experimental result that physical persistence of the aerosol in a closed aerosol chamber increases as particle size is decreased is satisfactorily explained on the bases of electrostatic, gravitational, inertial, and diffusion forces operating to remove particles from the particular aerosol system. The net effect of these various forces is to provide, after a short time interval in the system (about 2 min), an aerosol of fine particles with enhanced physical stability. The dependence of physical stability of the aerosol on the species of organism and the nature of the suspending medium for lyophilization is indicated. Also, limitations and general applicability of both the technique and results are discussed. PMID:4992657

  17. AEROSOL AND GAS MEASUREMENT

    EPA Science Inventory

    Measurements provide fundamental information for evaluating and managing the impact of aerosols on air quality. Specific measurements of aerosol concentration and their physical and chemical properties are required by different users to meet different user-community needs. Befo...

  18. Aerosols and environmental pollution

    NASA Astrophysics Data System (ADS)

    Colbeck, Ian; Lazaridis, Mihalis

    2010-02-01

    The number of publications on atmospheric aerosols has dramatically increased in recent years. This review, predominantly from a European perspective, summarizes the current state of knowledge of the role played by aerosols in environmental pollution and, in addition, highlights gaps in our current knowledge. Aerosol particles are ubiquitous in the Earth’s atmosphere and are central to many environmental issues; ranging from the Earth’s radiative budget to human health. Aerosol size distribution and chemical composition are crucial parameters that determine their dynamics in the atmosphere. Sources of aerosols are both anthropogenic and natural ranging from vehicular emissions to dust resuspension. Ambient concentrations of aerosols are elevated in urban areas with lower values at rural sites. A comprehensive understanding of aerosol ambient characteristics requires a combination of measurements and modeling tools. Legislation for ambient aerosols has been introduced at national and international levels aiming to protect human health and the environment.

  19. Aerosols and environmental pollution.

    PubMed

    Colbeck, Ian; Lazaridis, Mihalis

    2010-02-01

    The number of publications on atmospheric aerosols has dramatically increased in recent years. This review, predominantly from a European perspective, summarizes the current state of knowledge of the role played by aerosols in environmental pollution and, in addition, highlights gaps in our current knowledge. Aerosol particles are ubiquitous in the Earth's atmosphere and are central to many environmental issues; ranging from the Earth's radiative budget to human health. Aerosol size distribution and chemical composition are crucial parameters that determine their dynamics in the atmosphere. Sources of aerosols are both anthropogenic and natural ranging from vehicular emissions to dust resuspension. Ambient concentrations of aerosols are elevated in urban areas with lower values at rural sites. A comprehensive understanding of aerosol ambient characteristics requires a combination of measurements and modeling tools. Legislation for ambient aerosols has been introduced at national and international levels aiming to protect human health and the environment.

  20. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3- aerosol during the 2013 Southern Oxidant and Aerosol Study

    SciTech Connect

    Allen, Hannah M.; Draper, Danielle C.; Ayres, Benjamin R.; Ault, Andrew P.; Bondy, Amy L.; Takahama, S.; Modini, Robert; Baumann, K.; Edgerton, Eric S.; Knote, Christoph; Laskin, Alexander; Wang, Bingbing; Fry, Juliane L.

    2015-09-25

    The inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 1 June to 15 July 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA), an ion chromatograph coupled with a wet rotating denuder and a steam-jet aerosol collector for monitoring of ambient inorganic gas and aerosol species, revealed two periods of high aerosol nitrate (NO3 ) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of coarse mode mineral or sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 um) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of mineral dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3 is produced primarily by this process, and is likely limited by the availability of mineral dust surface area. Modeling of NO3 and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas/aerosol phase partitioning.

  1. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

    Gao, Y.; Tsigaridis, K.; Bauer, S.

    2015-12-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  2. Modeling aerosol processes at the local scale

    SciTech Connect

    Lazaridis, M.; Isukapalli, S.S.; Georgopoulos, P.G.

    1998-12-31

    This work presents an approach for modeling photochemical gaseous and aerosol phase processes in subgrid plumes from major localized (e.g. point) sources (plume-in-grid modeling), thus improving the ability to quantify the relationship between emission source activity and ambient air quality. This approach employs the Reactive Plume Model (RPM-AERO) which extends the regulatory model RPM-IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, sodium, chloride and crustal material of aerosols are treated and attributed to the PM size distribution. A modified version of the Carbon Bond IV chemical mechanism is included to model the formation of organic aerosol, and the inorganic multicomponent atmospheric aerosol equilibrium model, SEQUILIB is used for calculating the amounts of inorganic species in particulate matter. Aerosol dynamics modeled include mechanisms of nucleation, condensation and gas/particle partitioning of organic matter. An integrated trajectory-in-grid modeling system, UAM/RPM-AERO, is under continuing development for extracting boundary and initial conditions from the mesoscale photochemical/aerosol model UAM-AERO. The RPM-AERO is applied here to case studies involving emissions from point sources to study sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions.

  3. Aerosol distribution apparatus

    DOEpatents

    Hanson, W.D.

    An apparatus for uniformly distributing an aerosol to a plurality of filters mounted in a plenum, wherein the aerosol and air are forced through a manifold system by means of a jet pump and released into the plenum through orifices in the manifold. The apparatus allows for the simultaneous aerosol-testing of all the filters in the plenum.

  4. Improved solid aerosol generator

    DOEpatents

    Prescott, D.S.; Schober, R.K.; Beller, J.

    1988-07-19

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates. 2 figs.

  5. Solid aerosol generator

    DOEpatents

    Prescott, Donald S.; Schober, Robert K.; Beller, John

    1992-01-01

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates.

  6. Solid aerosol generator

    DOEpatents

    Prescott, D.S.; Schober, R.K.; Beller, J.

    1992-03-17

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration is disclosed. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates. 2 figs.

  7. A pathway analysis of global aerosol processes

    NASA Astrophysics Data System (ADS)

    Schutgens, Nick; Stier, Philip

    2014-05-01

    Although budgets for aerosol emission and deposition (macrophysical fluxes) have been studied before, much less is known about the budgets of processes e.g. nucleation, coagulation and condensation. A better understanding of their relative importance would improve our understanding of the aerosol system and help model development and evaluation. Aerosols are not only emitted from and deposited to the Earth's surface but are modified during their transport. The processes for these modifications include nucleation of H2SO4 gas into new aerosol, coagulation with other aerosol and condensation of H2SO4 unto existing aerosol. As a result of these processes, aerosol grow in size and change their chemical composition, often becoming hydrophilic where they were hydrophobic before. This affects their characteristics for various deposition processes (sedimentation, dry or wet deposition) as well as their radiative properties and hence climate forcing by aerosol. We present a complete budget of all aerosol processes in the aerosol-climate model ECHAM-HAM including the M7 microphysics. This model treats aerosol as 7 distinct but interacting two-moment modes of mixed species (soot, organic carbons, sulfate, sea salt and dust). We will show both global budgets as well as regional variations in dominant processes. Some of our conclusions are: condensation of H2SO4 gas onto pre-existing particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the ageing of hydrophobic matter. Together with in-cloud production of H2SO4, it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. However, the coarse mode is mostly decoupled from the

  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. Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: an AQMEII-2 perspective

    EPA Science Inventory

    The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model in...

  10. Characterization of gas-aerosol interaction kinetics using morphology dependent stimulated Raman scattering. Final technical report

    SciTech Connect

    Aker, P.M.

    1992-12-31

    A research program on the influence of aerosol surface structure on the kinetics of gas-aerosol interactions is proposed. The experiments involve measuring changes in gas phase chemical reaction rates as a function of exposure to a specific aerosol. Aerosols with differing surface properties will be generated by changing the composition and/or temperature of the material making up the aerosol. Kinetic data generated can be used directly in atmospheric modelling calculations. The surface structure of the aerosol will be measured, both before and after reaction, using morphology-dependent enhancement of simulated Raman scattering (MDSRS). Information about the detailed dynamics of gas-aerosol interactions can be obtained by correlating the change in the reaction rate with change in surface structure and by monitoring the change in aerosol surface structure during the course of the reaction. Studies will focus on the condensation and oxidation of sulfur species (sulfur dioxide and dimethyl sulfide) on water aerosols.

  11. Characterization of gas-aerosol interaction kinetics using morphology dependent stimulated Raman scattering

    SciTech Connect

    Aker, P.M.

    1992-01-01

    A research program on the influence of aerosol surface structure on the kinetics of gas-aerosol interactions is proposed. The experiments involve measuring changes in gas phase chemical reaction rates as a function of exposure to a specific aerosol. Aerosols with differing surface properties will be generated by changing the composition and/or temperature of the material making up the aerosol. Kinetic data generated can be used directly in atmospheric modelling calculations. The surface structure of the aerosol will be measured, both before and after reaction, using morphology-dependent enhancement of simulated Raman scattering (MDSRS). Information about the detailed dynamics of gas-aerosol interactions can be obtained by correlating the change in the reaction rate with change in surface structure and by monitoring the change in aerosol surface structure during the course of the reaction. Studies will focus on the condensation and oxidation of sulfur species (sulfur dioxide and dimethyl sulfide) on water aerosols.

  12. Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS OZone and Nitrogen Oxide Experiment (SONEX)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    1999-01-01

    The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the north Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope greater than 0.9 and r(sup 2) greater than 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(x). (NO + NO2), HNO3, and PAN. Median values of NO(x)/NO(y) were approx. = 0.25, HNO3/NO(y) approx. = 0.35 and PAN/NO(y) approx. = 0.17. Particulate NO3 and alkyl nitrates together composed less than 10% of NO(y), while model estimated HNO4 averaged 12%.

  13. Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS Ozone and Nitrogen Oxide Experiment (SONEX)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    1999-01-01

    The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the North Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(sub y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(sub y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(sub y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(sub y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope > 0.9 and r(exp 2) > 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(sub x). (NO + NO2), HNO3, and PAN. Median values of NO(sub x)/NO(sub y) were approximately equal to 0.25, HNO3/NO(sub y) were approximately equal to 0.35 and Peroxyacetyl Nitrate (PAN)/NO(sub y) were approximately equal to 0. 17. Particulate NO3 and alkyl nitrates together composed <10 % of NO(sub y), while model estimated HNO4 averaged 12%.

  14. The influence of metallurgy on the formation of welding aerosols.

    PubMed

    Zimmer, Anthony T

    2002-10-01

    Recent research has indicated that insoluble ultrafine aerosols (ie., particles whose physical diameters are less than 100 nm) may cause adverse health effects due to their small size, and that toxicological response may be more appropriately represented by particle number or particle surface area. Unfortunately, current exposure criteria and the associated air-sampling techniques are primarily mass-based. Welding processes are high-temperature operations that generate substantial number concentrations of ultrafine aerosols. Welding aerosols are formed primarily through the nucleation of metal vapors followed by competing growth mechanisms such as coagulation and condensation. Experimental results and mathematical tools are presented to illustrate how welding metallurgy influences the chemical aspects and dynamic processes that initiate and evolve the resultant aerosol. This research suggests that a fundamental understanding of metallurgy and aerosol physics can be exploited to suppress the formation of undesirable chemical species as well as the amount of aerosol generated during a welding process.

  15. Evaluation of an assimilated aerosol climatology using AERONET

    NASA Astrophysics Data System (ADS)

    Collins, W. D.; Rasch, P. J.; Conley, A.

    2002-05-01

    The estimates of multi-wavelength aerosol optical depth and optical properties from AERONET represent a valuable data set for evaluating aerosol models. We have analyzed the fidelity of a new aerosol climatology using the AERONET network. An aerosol climatology for 1995-2000 has been created using an aerosol assimilation model. The model produces global three-dimensional distributions of major aerosol species at six-hourly intervals (Collins et al, 2001; Rasch et al, 2001). The atmospheric state and dynamical fields are obtained from the NCEP meteorological reanalysis for 1979 to the present. The model is adjusted to reduce discrepancies relative to retrievals of aerosol optical depth from the AVHRR imagers on board NOAA polar-orbiting satellites. While these adjustments improve the realism of modeled optical depths over ocean regions (e.g., Collins et al, 2001), the satellite observations do not constrain the model over continental surfaces close to major aerosol source regions. We compare the predictions of the assimilation model to selected AERONET observations of aerosol optical depths and single-scattering albedos at multiple wavelengths. The results will be used to improve the treatment of aerosol sources and optical properties in subsequent versions of the climatology.

  16. Generation and Characterization of Indoor Fungal Aerosols for Inhalation Studies

    PubMed Central

    Larsen, Søren T.; Koponen, Ismo K.; Kling, Kirsten I.; Barooni, Afnan; Karottki, Dorina Gabriela; Tendal, Kira; Wolkoff, Peder

    2016-01-01

    In the indoor environment, people are exposed to several fungal species. Evident dampness is associated with increased respiratory symptoms. To examine the immune responses associated with fungal exposure, mice are often exposed to a single species grown on an agar medium. The aim of this study was to develop an inhalation exposure system to be able to examine responses in mice exposed to mixed fungal species aerosolized from fungus-infested building materials. Indoor airborne fungi were sampled and cultivated on gypsum boards. Aerosols were characterized and compared with aerosols in homes. Aerosols containing 107 CFU of fungi/m3 air were generated repeatedly from fungus-infested gypsum boards in a mouse exposure chamber. Aerosols contained Aspergillus nidulans, Aspergillus niger, Aspergillus ustus, Aspergillus versicolor, Chaetomium globosum, Cladosporium herbarum, Penicillium brevicompactum, Penicillium camemberti, Penicillium chrysogenum, Penicillium commune, Penicillium glabrum, Penicillium olsonii, Penicillium rugulosum, Stachybotrys chartarum, and Wallemia sebi. They were all among the most abundant airborne species identified in 28 homes. Nine species from gypsum boards and 11 species in the homes are associated with water damage. Most fungi were present as single spores, but chains and clusters of different species and fragments were also present. The variation in exposure level during the 60 min of aerosol generation was similar to the variation measured in homes. Through aerosolization of fungi from the indoor environment, cultured on gypsum boards, it was possible to generate realistic aerosols in terms of species composition, concentration, and particle sizes. The inhalation-exposure system can be used to study responses to indoor fungi associated with water damage and the importance of fungal species composition. PMID:26921421

  17. Effect of hydrophilic organic seed aerosols on secondary organic aerosol formation from ozonolysis of α-pinene.

    PubMed

    Song, Chen; Zaveri, Rahul A; Shilling, John E; Alexander, M Lizabeth; Newburn, Matt

    2011-09-01

    Gas-particle partitioning theory is widely used in atmospheric models to predict organic aerosol loadings. This theory predicts that secondary organic aerosol (SOA) yield of an oxidized volatile organic compound product will increase as the mass loading of preexisting organic aerosol increases. In a previous work, we showed that the presence of model hydrophobic primary organic aerosol (POA) had no detectable effect on the SOA yields from ozonolysis of α-pinene, suggesting that the condensing SOA compounds form a separate phase from the preexisting POA. However, a substantial faction of atmospheric aerosol is composed of polar, hydrophilic organic compounds. In this work, we investigate the effects of model hydrophilic organic aerosol (OA) species such as fulvic acid, adipic acid, and citric acid on the gas-particle partitioning of SOA from α-pinene ozonolysis. The results show that only citric acid seed significantly enhances the absorption of α-pinene SOA into the particle-phase. The other two seed particles have a negligible effect on the α-pinene SOA yields, suggesting that α-pinene SOA forms a well-mixed organic aerosol phase with citric acid and a separate phase with adipic acid and fulvic acid. This finding highlights the need to improve the thermodynamics treatment of organics in current aerosol models that simply lump all hydrophilic organic species into a single phase, thereby potentially introducing an erroneous sensitivity of SOA mass to emitted OA species. PMID:21790137

  18. Role of Clouds, Aerosols, and Aerosol-Cloud Interaction in 20th Century Simulations with GISS ModelE2

    NASA Technical Reports Server (NTRS)

    Nazarenko, Larissa; Rind, David; Bauer, Susanne; Del Genio, Anthony

    2015-01-01

    The key uncertainties in the climate sensitivity to the increasing greenhouse gases lie in the behavior and impact of short-lived species, such as tropospheric aerosols and ozone, and secondly, in the response and impact of the ocean circulation.

  19. Aerosol MTF revisited

    NASA Astrophysics Data System (ADS)

    Kopeika, Norman S.; Zilberman, Arkadi; Yitzhaky, Yitzhak

    2014-05-01

    Different views of the significance of aerosol MTF have been reported. For example, one recent paper [OE, 52(4)/2013, pp. 046201] claims that the aerosol MTF "contrast reduction is approximately independent of spatial frequency, and image blur is practically negligible". On the other hand, another recent paper [JOSA A, 11/2013, pp. 2244-2252] claims that aerosols "can have a non-negligible effect on the atmospheric point spread function". We present clear experimental evidence of common significant aerosol blur and evidence that aerosol contrast reduction can be extremely significant. In the IR, it is more appropriate to refer to such phenomena as aerosol-absorption MTF. The role of imaging system instrumentation on such MTF is addressed too.

  20. The Regional Environmental Impacts of Atmospheric Aerosols over Egypt

    NASA Astrophysics Data System (ADS)

    Zakey, Ashraf; Ibrahim, Alaa

    2015-04-01

    Identifying the origin (natural versus anthropogenic) and the dynamics of aerosols over Egypt at varying temporal and spatial scales provide valuable knowledge on the regional climate impacts of aerosols and their ultimate connections to the Earth's regional climate system at the MENA region. At regional scale, Egypt is exposed to air pollution with levels exceeding typical air-quality standards. This is particularly true for the Nile Delta region, being at the crossroads of different aerosol species originating from local urban-industrial and biomass-burning activities, regional dust sources, and European pollution from the north. The Environmental Climate Model (EnvClimA) is used to investigate both of the biogenic and anthropogenic aerosols over Egypt. The dominant natural aerosols over Egypt are due to the sand and dust storms, which frequently occur during the transitional seasons (spring and autumn). In winter, the maximum frequency reaches 2 to 3 per day in the north, which decreases gradually southward with a frequency of 0.5-1 per day. Monitoring one of the most basic aerosol parameters, the aerosol optical depth (AOD), is a main experimental and modeling task in aerosol studies. We used the aerosol optical depth to quantify the amount and variability of aerosol loading in the atmospheric column over a certain areas. The aerosols optical depth from the model is higher in spring season due to the impacts of dust activity over Egypt as results of the westerly wind, which carries more dust particles from the Libyan Desert. The model result shows that the mass load of fine aerosols has a longer life-time than the coarse aerosols. In autumn season, the modelled aerosol optical depth tends to increase due to the biomass burning in the delta of Egypt. Natural aerosol from the model tends to scatter the solar radiation while most of the anthropogenic aerosols tend to absorb the longwave solar radiation. The overall results indicate that the AOD is lowest in winter

  1. MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

    2015-01-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  2. Radiative Effects of Aerosols

    NASA Technical Reports Server (NTRS)

    Valero, Francisco P. J.

    1997-01-01

    During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size resolved aerosol microphysics and chemistry. Both profiles included pollution haze layer from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core.

  3. Thermoluminescent aerosol analysis

    NASA Technical Reports Server (NTRS)

    Rogowski, R. S.; Long, E. R., Jr. (Inventor)

    1977-01-01

    A method for detecting and measuring trace amounts of aerosols when reacted with ozone in a gaseous environment was examined. A sample aerosol was exposed to a fixed ozone concentration for a fixed period of time, and a fluorescer was added to the exposed sample. The sample was heated in a 30 C/minute linear temperature profile to 200 C. The trace peak was measured and recorded as a function of the test aerosol and the recorded thermoluminescence trace peak of the fluorescer is specific to the aerosol being tested.

  4. 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.

  5. Influence of Aerosols on Monsoon Circulation and Hydroclimate

    NASA Technical Reports Server (NTRS)

    Lau, William K.M.

    2007-01-01

    Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global water cycles and climate change. In the Asian monsoon regions, the response of the regional water cycle and climate to aerosol forcing is very complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. Up to now, besides the general notion that aerosols may significantly impact monsoon through altering large scale radiative heating gradients, there has been very little information regarding the specific signatures, and mechanisms of aerosol-monsoon water cycle interaction. In this talk, based on preliminary results from observations and climate model experiments, I will offer some insights into how aerosols may impact the Asian monsoon water cycle, in particular the effects of absorbing aerosols (dust and black carbon), and the role of the Tibetan Plateau. The influence of aerosol forcing relative to those due to sea surface temperature and land surface processes, and impact on potential predictability of the monsoon climate system will also be discussed.

  6. Influence of Aerosols on Monsoon Circulation and Hydroclimate

    NASA Technical Reports Server (NTRS)

    Lau, William K.

    2006-01-01

    Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global water cycles and climate change. In the Asian monsoon regions, the response of the regional water cycle and climate to aerosol forcing is very complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. Up to now, besides the general notion that aerosols may significantly impact monsoon through altering large scale radiative heating gradients, there has been very little information regarding the specific signatures, and mechanisms of aerosol-monsoon water cycle interaction. In this talk, based on preliminary results from observations and climate model experiments, I will offer some insights into how aerosols may impact the Asian monsoon water cycle, in particular the effects of absorbing aerosols (dust and black carbon), and the role of the Tibetan Plateau. The influence of aerosol forcing relative to those due to sea surface temperature and land surface processes, and impact on potential predictability of the monsoon climate system will also be discussed.

  7. Direct radiative effect by multicomponent aerosol over China

    SciTech Connect

    Huang, Xin; Song, Yu; Zhao, Chun; Cai, Xuhui; Zhang, Hongsheng; Zhu, Tong

    2015-05-01

    The direct radiative effect (DRE) of multiple aerosol species (sulfate, nitrate, ammonium, black carbon (BC), organic carbon (OC), and mineral aerosol) and their spatiotemporal variations over China were investigated using a fully coupled meteorology–chemistry model (WRF-Chem) for the entire year of 2006. We made modifications to improve model performance, including updating land surface parameters, improving the calculation of transition metal-catalyzed oxidation of SO2, and adding in heterogeneous reactions between mineral aerosol and acid gases. The modified model well reproduced the magnitude, seasonal pattern, and spatial distribution of the measured meteorological conditions, concentrations of PM10 and its components, and aerosol optical depth (AOD). A diagnostic iteration method was used to estimate the overall DRE of aerosols and contributions from different components. At the land surface, all kinds of aerosol species reduced the incident net radiation flux with a total DRE of 10.2 W m-2 over China. Aerosols significantly warm the atmosphere with the national mean DRE of +10.8 W m-2. BC was the leading radiative-heating component (+8.7 W m-2), followed by mineral aerosol (+1.1 W m-2). At the top of the atmosphere (TOA), BC introduced the largest radiative perturbation (+4.5 W m-2), followed by sulfate (-1.4 W m-2). The overall perturbation of aerosols on radiation transfer is quite small over China, demonstrating the counterbalancing effect between scattering and adsorbing aerosols. Aerosol DRE at the TOA had distinct seasonality, generally with a summer maximum and winter minimum, mainly determined by mass loadings, hygroscopic growth, and incident radiation flux.

  8. Improving Aerosol Transport to the Arctic in CAM5

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Rasch, P.; Wang, M.; Liu, X.; Ghan, S.; Qian, Y.; Yoon, J.; Ma, P.; Vinoj, V.

    2011-12-01

    Of the many factors contributing to the rapid arctic climate change, arctic haze has been identified as a potentially important forcing agent. It has been well established that arctic aerosols largely originate from lower latitudes. Hence, the long-range atmospheric transport of aerosols to the Arctic is of great concern for studying arctic climate change. The treatment of aerosol and cloud processes has been substantially improved in the current version of the Community Atmosphere Model (CAM5) which is widely used in the research of aerosol effects on clouds and climate. However, like many other global models, the CAM5 produces a relatively poor simulation of arctic aerosols and clouds. For example, previous studies have shown that the standard version of CAM5 remarkably underpredicts arctic aerosol concentrations, particularly during the arctic haze season, compared to various measurements. In this study, we focus on improving processes associated with aerosol-cloud interactions, cloud microphysics and macrophysics, and aerosol emission, transformation, removal, and deposition that are key to determining the amount of aerosols reaching the Arctic. Sensitivity experiments are conducted to understand the role of each of the processes and to identify sources of uncertainties, and improvements are made to processes that are not well represented in the CAM5. The evaluation and improvement are guided by aerosol and cloud measurements together with process-oriented model results from the multi-scale aerosol-climate model (PNNL-MMF) that embeds a cloud-resolving model in each CAM5 grid column to explicitly represent convection and aerosol-cloud interactions. Results show that including black carbon (BC) aging process through a more complete 7-mode version of the aerosol module in CAM5 can substantially increase the amount of arctic BC, compared to simulations with the standard 3-mode version, but has minimal effect on other species such as dust and sulfate. Excessive mid

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    biomass burning alters atmospheric composition very significantly. AOT can reach values as high as 2-3 at 550 nm, and concentrations of aerosol species and trace gases are strongly enriched.

  10. Influences of external vs. core-shell mixing on aerosol optical properties at various relative humidities.

    PubMed

    Ramachandran, S; Srivastava, Rohit

    2013-05-01

    Aerosol optical properties of external and core-shell mixtures of aerosol species present in the atmosphere are calculated in this study for different relative humidities. Core-shell Mie calculations are performed using the values of radii, refractive indices and densities of aerosol species that act as core and shell, and the core-shell radius ratio. The single scattering albedo (SSA) is higher when the absorbing species (black carbon, BC) is the core, while for a sulfate core SSA does not vary significantly as the BC in the shell dominates the absorption. Absorption gets enhanced in core-shell mixing of absorbing and scattering aerosols when compared to their external mixture. Thus, SSA is significantly lower for a core-shell mixture than their external mixture. SSA is more sensitive to core-shell ratio than mode radius when BC is the core. The extinction coefficient, SSA and asymmetry parameter are higher for external mixing when compared to BC (core)-water soluble aerosol (shell), and water soluble aerosol (core)-BC (shell) mixtures in the relative humidity range of 0 to 90%. Spectral SSA exhibits the behaviour of the species which acts as a shell in core-shell mixing. The asymmetry parameter for an external mixture of water soluble aerosol and BC is higher than BC (core)-water soluble aerosol (shell) mixing and increases as function of relative humidity. The asymmetry parameter for the water soluble aerosol (core)-BC (shell) is independent of relative humidity as BC is hydrophobic. The asymmetry parameter of the core-shell mixture decreases when BC aerosols are involved in mixing, as the asymmetry parameter of BC is lower. Aerosol optical depth (AOD) of core-shell mixtures increases at a higher rate when the relative humidity exceeds 70% in continental clean and urban aerosol models, whereas AOD remains the same when the relative humidity exceeds 50% in maritime aerosol models. The SSA for continental aerosols varies for core-shell mixing of water soluble

  11. Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

    NASA Technical Reports Server (NTRS)

    Thomason, L. W.

    2012-01-01

    Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

  12. Portable Aerosol Contaminant Extractor

    DOEpatents

    Carlson, Duane C.; DeGange, John J.; Cable-Dunlap, Paula

    2005-11-15

    A compact, portable, aerosol contaminant extractor having ionization and collection sections through which ambient air may be drawn at a nominal rate so that aerosol particles ionized in the ionization section may be collected on charged plate in the collection section, the charged plate being readily removed for analyses of the particles collected thereon.

  13. Global Aerosol Observations

    Atmospheric Science Data Center

    2013-04-19

    ... atmosphere, directly influencing global climate and human health. Ground-based networks that accurately measure column aerosol amount and ... being used to improve Air Quality Models and for regional health studies. To assess the human-health impact of chronic aerosol exposure, ...

  14. Direct Aerosol Forcing Uncertainty

    DOE Data Explorer

    Mccomiskey, Allison

    2008-01-15

    Understanding sources of uncertainty in aerosol direct radiative forcing (DRF), the difference in a given radiative flux component with and without aerosol, is essential to quantifying changes in Earth's radiation budget. We examine the uncertainty in DRF due to measurement uncertainty in the quantities on which it depends: aerosol optical depth, single scattering albedo, asymmetry parameter, solar geometry, and surface albedo. Direct radiative forcing at the top of the atmosphere and at the surface as well as sensitivities, the changes in DRF in response to unit changes in individual aerosol or surface properties, are calculated at three locations representing distinct aerosol types and radiative environments. The uncertainty in DRF associated with a given property is computed as the product of the sensitivity and typical measurement uncertainty in the respective aerosol or surface property. Sensitivity and uncertainty values permit estimation of total uncertainty in calculated DRF and identification of properties that most limit accuracy in estimating forcing. Total uncertainties in modeled local diurnally averaged forcing range from 0.2 to 1.3 W m-2 (42 to 20%) depending on location (from tropical to polar sites), solar zenith angle, surface reflectance, aerosol type, and aerosol optical depth. The largest contributor to total uncertainty in DRF is usually single scattering albedo; however decreasing measurement uncertainties for any property would increase accuracy in DRF. Comparison of two radiative transfer models suggests the contribution of modeling error is small compared to the total uncertainty although comparable to uncertainty arising from some individual properties.

  15. Ganges valley aerosol experiment.

    SciTech Connect

    Kotamarthi, V.R.; Satheesh, S.K.

    2011-08-01

    In June 2011, the Ganges Valley Aerosol Experiment (GVAX) began in the Ganges Valley region of India. The objective of this field campaign is to obtain measurements of clouds, precipitation, and complex aerosols to study their impact on cloud formation and monsoon activity in the region.

  16. The Importance of the Vertical Location of Aerosol Layers on Convective Storms

    NASA Astrophysics Data System (ADS)

    van den Heever, Susan; Grant, Leah

    2014-05-01

    Enhanced aerosol concentrations appear to influence a number of the aspects of convective storms including the strength of the convective updraft, the intensity of the cold pool, and the microphysical and radiative characteristics of the convective anvil. However, in order for such influences to occur, aerosols need to be effectively ingested by the storm system of interest. The vertical location of an aerosol layer impacting a convective storm may influence how effectively aerosol are ingested by the storm system, and hence the degree to which the ingested aerosol subsequently influence storm microphysical and radiative processes. Furthermore, if the aerosol species impacting the storm are effective at absorbing solar radiation, heating within the aerosol layer enhances atmospheric stability, the level of which will be dictated by where the aerosol layer is located. Enhanced static stability may have negative impacts on the initial development of the convection of interest. Convective storms developing within environments of the same aerosol optical depth may therefore respond differently to aerosol indirect forcing by virtue of where the aerosol layer is vertically located. In this talk, the results of various high-resolution, cloud-resolving simulations will be presented, in which the sensitivity to the vertical location of the aerosol source on the convective development, aerosol ingestion efficiency, and subsequent microphysical and radiative properties are investigated. Microphysical budgets and storm trajectories will form an integral part of the analysis.

  17. Analysis of Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Prather, Kimberly A.; Hatch, Courtney D.; Grassian, Vicki H.

    2008-07-01

    Aerosols represent an important component of the Earth's atmosphere. Because aerosols are composed of solid and liquid particles of varying chemical complexity, size, and phase, large challenges exist in understanding how they impact climate, health, and the chemistry of the atmosphere. Only through the integration of field, laboratory, and modeling analysis can we begin to unravel the roles atmospheric aerosols play in these global processes. In this article, we provide a brief review of the current state of the science in the analysis of atmospheric aerosols and some important challenges that need to be overcome before they can become fully integrated. It is clear that only when these areas are effectively bridged can we fully understand the impact that atmospheric aerosols have on our environment and the Earth's system at the level of scientific certainty necessary to design and implement sound environmental policies.

  18. Radiative Effects of Aerosols

    NASA Technical Reports Server (NTRS)

    Valero, Francisco P. J.

    1996-01-01

    During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size-resolved aerosol microphysics and chemistry. Both profiles included a pollution haze from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core. The soot core increased the calculated extinction by about 10% in the most polluted drier layer relative to a pure sulfate aerosol but had significantly less effect at higher humidities. A 3 km descent through a boundary layer air mass dominated by pollutant aerosol with relative humidities (RH) 10-77% yielded a close agreement between the measured and calculated aerosol optical depths (550 nm) of 0.160 (+/- 0.07) and 0. 157 (+/- 0.034) respectively. During descent the aerosol mass scattering coefficient per unit sulfate mass varied from about 5 to 16 m(exp 2)/g and primarily dependent upon ambient RH. However, the total scattering coefficient per total fine mass was far less variable at about 4+/- 0.7 m(exp 2)/g. A subsequent descent through a Saharan dust layer located above the pollution aerosol layer revealed that both layers contributed similarly to aerosol optical depth. The scattering per unit mass of the coarse aged dust was estimated at 1.1 +/- 0.2 m(exp 2)/g. The large difference (50%) in measured and calculated optical depth for the dust layer exceeded measurements.

  19. Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

    SciTech Connect

    Dr. Timothy Onasch

    2009-09-09

    This SBIR Phase I project addressed the critical need for improved characterization of carbonaceous aerosol species in the atmosphere. The proposed work focused on the development of a thermodenuder (TD) system capable of systematically measuring volatility profiles of primary and secondary organic aerosol species and providing insight into the effects of absorbing and nonabsorbing organic coatings on particle absorption properties. This work provided the fundamental framework for the generation of essential information needed for improved predictions of ambient aerosol loadings and radiative properties by atmospheric chemistry models. As part of this work, Aerodyne Research, Inc. (ARI) continued to develop and test, with the final objective of commercialization, an improved thermodenuder system that can be used in series with any aerosol instrument or suite of instruments (e.g., aerosol mass spectrometers-AMS, scanning mobility particle sizers-SMPS, photoacoustic absorption spectrometers-PAS, etc.) to obtain aerosol chemical, physical, and optical properties as a function of particle volatility. In particular, we provided the proof of concept for the direct coupling of our improved TD design with a full microphysical model to obtain volatility profiles for different organic aerosol components and to allow for meaningful comparisons between different TD-derived aerosol measurements. In a TD, particles are passed through a heated zone and a denuding (activated charcoal) zone to remove semi-volatile material. Changes in particle size, number concentration, optical absorption, and chemical composition are subsequently detected with aerosol instrumentation. The aerosol volatility profiles provided by the TD will strengthen organic aerosol emission inventories, provide further insight into secondary aerosol formation mechanisms, and provide an important measure of particle absorption (including brown carbon contributions and identification, and absorption enhancements

  20. CADS:Cantera Aerosol Dynamics Simulator.

    SciTech Connect

    Moffat, Harry K.

    2007-07-01

    This manual describes a library for aerosol kinetics and transport, called CADS (Cantera Aerosol Dynamics Simulator), which employs a section-based approach for describing the particle size distributions. CADS is based upon Cantera, a set of C++ libraries and applications that handles gas phase species transport and reactions. The method uses a discontinuous Galerkin formulation to represent the particle distributions within each section and to solve for changes to the aerosol particle distributions due to condensation, coagulation, and nucleation processes. CADS conserves particles, elements, and total enthalpy up to numerical round-off error, in all of its formulations. Both 0-D time dependent and 1-D steady state applications (an opposing-flow flame application) have been developed with CADS, with the initial emphasis on developing fundamental mechanisms for soot formation within fires. This report also describes the 0-D application, TDcads, which models a time-dependent perfectly stirred reactor.

  1. The investigation of advanced remote sensing techniques for the measurement of aerosol characteristics

    NASA Technical Reports Server (NTRS)

    Deepak, A.; Becher, J.

    1979-01-01

    Advanced remote sensing techniques and inversion methods for the measurement of characteristics of aerosol and gaseous species in the atmosphere were investigated. Of particular interest were the physical and chemical properties of aerosols, such as their size distribution, number concentration, and complex refractive index, and the vertical distribution of these properties on a local as well as global scale. Remote sensing techniques for monitoring of tropospheric aerosols were developed as well as satellite monitoring of upper tropospheric and stratospheric aerosols. Computer programs were developed for solving multiple scattering and radiative transfer problems, as well as inversion/retrieval problems. A necessary aspect of these efforts was to develop models of aerosol properties.

  2. LOAC: A light aerosol counter/sizer for atmospheric balloons

    NASA Astrophysics Data System (ADS)

    Renard, Jean-Baptiste; Thaury, Claire; Mineau, Jean-Luc; Verdier, Nicolas; Dulac, François; Mallet, Marc; Berthet, Gwenael; Gaubicher, Bertrand; Coute, Benoit

    The estimation of the total amount of aerosols in the upper troposphere and in lower -middle stratosphere is necessary to constraint the model calculations of the species that are sensi-tive to heterogeneous chemical reactions, to improve calculations on the atmospheric radiative transfer, and to better establish the sources of aerosols that are vertically transported up to the middle stratosphere. It is now known that different natures of aerosols can be found in the troposphere and in the stratosphere. These aerosols are made of liquid particles, and/or solid particles like soot, sands, meteoritic debris... The identification of the main nature of aerosols is not easily feasible using conventional aerosol counters, which perform in situ scat-tering measurements from a light source at a single angle typically in the 70-110 degrees range. Also, such counters are not very sensitive to soot particles that absorb the light but can be the main population of aerosols in the lower and middle stratosphere. In this work we describe a new generation of aerosol counters under development in the framework of the project LOAC (Light Optical Aerosol Counter) supported by the French ANR/Ecotech programme. LOAC will be a light particle counter/sizer, less than metricconverterProductID1 kg1 kg, designed to be mounted on the various kinds of tropospheric and stratospheric balloons. The measurements will be conducted at 2 scattering angles: the first one, at 10 degrees, is used to determine the aerosols concentration of several size classes within diameter range 0.3 and 20 micrometeres. At such low scattering angle close to forward scattering, the signal is much more intense and the measurements are not strongly sensitive to the nature of the aerosols. The second angle is at 60 degrees, where the light scattered is strongly dependent on the particle refractive index and thus on the nature of the aerosols. The ratio of the measurements at the 2 angles is used to determine the main

  3. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

    Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

    2002-02-01

    The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

  4. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

    Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

    2003-02-01

    The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

  5. Analysis of DIAL/HSRL aerosol backscatter and extinction profiles during the SEAC4RS campaign with an aerosol assimilation system

    NASA Astrophysics Data System (ADS)

    Weaver, C. J.; da Silva, A. M., Jr.; Colarco, P. R.; Randles, C. A.

    2015-12-01

    We retrieve aerosol concentrations and optical information from vertical profiles of airborne 532 nm extinction and 532 and 1064 nm backscatter measurements made during the SEAC4RS summer 2013 campaign. The observations are from the High Spectral Resolution Lidar (HSRL) Airborne Differential Absorption Lidar (DIAL) on board the NASA DC-8. Instead of retrieving information about aerosol microphysical properties such as indexes of refraction, we seek information more directly applicable to an aerosol transport model - in our case the Goddard Chemistry Aerosol Radiation and Transport (GOCART) module used in the GEOS-5 Earth modeling system. A joint atmosphere/aerosol mini-reanalysis was performed for the SEAC4RS period using GEOS-5. The meteorological reanalysis followed the MERRA-2 atmospheric reanalysis protocol, and aerosol information from MODIS, MISR, and AERONET provided a constraint on the simulated aerosol optical depth (i.e., total column loading of aerosols). We focus on the simulated concentrations of 10 relevant aerosol species simulated by the GOCART module: dust, sulfate, and organic and black carbon. Our first retrieval algorithm starts with the SEAC4RS mini-reanalysis and adjusts the concentration of each GOCART aerosol species so that differences between the observed and simulated backscatter and extinction measurements are minimized. In this case, too often we are unable to simulate the observations by simple adjustment of the aerosol concentrations. A second retrieval approach adjusts both the aerosol concentrations and the optical parameters (i.e., assigned mass extinction efficiency) associated with each GOCART species. We present results from DC-8 flights over smoke from forest fires over the western US using both retrieval approaches. Finally, we compare our retrieved quantities with in-situ observations of aerosol absorption, scattering, and mass concentrations at flight altitude.

  6. Sugars in Antarctic aerosol

    NASA Astrophysics Data System (ADS)

    Barbaro, Elena; Kirchgeorg, Torben; Zangrando, Roberta; Vecchiato, Marco; Piazza, Rossano; Barbante, Carlo; Gambaro, Andrea

    2015-10-01

    The processes and transformations occurring in the Antarctic aerosol during atmospheric transport were described using selected sugars as source tracers. Monosaccharides (arabinose, fructose, galactose, glucose, mannose, ribose, xylose), disaccharides (sucrose, lactose, maltose, lactulose), alcohol-sugars (erythritol, mannitol, ribitol, sorbitol, xylitol, maltitol, galactitol) and anhydrosugars (levoglucosan, mannosan and galactosan) were measured in the Antarctic aerosol collected during four different sampling campaigns. For quantification, a sensitive high-pressure anion exchange chromatography was coupled with a single quadrupole mass spectrometer. The method was validated, showing good accuracy and low method quantification limits. This study describes the first determination of sugars in the Antarctic aerosol. The total mean concentration of sugars in the aerosol collected at the "Mario Zucchelli" coastal station was 140 pg m-3; as for the aerosol collected over the Antarctic plateau during two consecutive sampling campaigns, the concentration amounted to 440 and 438 pg m-3. The study of particle-size distribution allowed us to identify the natural emission from spores or from sea-spray as the main sources of sugars in the coastal area. The enrichment of sugars in the fine fraction of the aerosol collected on the Antarctic plateau is due to the degradation of particles during long-range atmospheric transport. The composition of sugars in the coarse fraction was also investigated in the aerosol collected during the oceanographic cruise.

  7. Behavioral-physiological effects of red phosphorous smoke inhalation on two wildlife species. Task 1. Inhalation equipment development/ambient CO evaluation/aerosol distribution and air-quality study. Final report, March 1985-December 1986

    SciTech Connect

    Sterner, R.T.; Shumake, S.A.; Johns, B.E.; Thompson, R.D.

    1987-12-01

    Tests to evaluate the spatial and temporal uniformity of red phosphorous - butyl rubber smoke produced in a commercial 1-CuM inhalation chamber are described. Several modifications to the inhalation exposure system aimed at improving air filtration, relative humidity, and temperature control for the conduct of animal studies are also presented. Smoke generation involved the use of a system for the continuous generation of phosphoric acid aerosols. Assessments of spatial and temporal uniformity of smoke were based upon measurements of aerosol mass concentration (gravimetric analysis), phosphoric acid deposition (titration analysis), aerosol opacity (infrared sensor), and particle size (cascade impactor); assessments of air quality and combustion products within the chamber involved checks for oxygen, carbon dioxide, phosphine, hexane, and carbon monoxide using either gas chromatography or industrial-hygiene-analyzer tubes. Results for aerosol mass, phosphoric acid, and particle size showed that the within-chamber smoke was highly uniform among burns. Although a number of statistically significant effects were obtained, further inspection showed these to be limited to specific sampling locations and within a priori criteria established to define acceptable uniformity.

  8. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGES

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-03-02

    We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized bymore » the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10-5 to 10-11. Free molecular heat and mass transfer theory was

  9. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-05-01

    An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

  10. Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

    2013-11-01

    Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding these transformation processes has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a Southeast Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high-resolution aerosol mass spectrometry and Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyl tetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

  11. Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

    2013-07-01

    Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding the process of these transformations has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a South East Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high resolution aerosol mass spectrometry and fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyltetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

  12. A Physically-Based Estimate of Radiative Forcing by Anthropogenic Sulfate Aerosol

    SciTech Connect

    Ghan, Steven J. ); Easter, Richard C. ); Chapman, Elaine G. ); Abdul-Razzak, Hayder; Zhang, Yang ); Leung, Ruby ); Laulainen, Nels S. ); Saylor, Rick D. ); Zaveri, Rahul A. )

    2001-04-01

    Estimates of direct and indirect radiative forcing by anthropogenic sulfate aerosols from an integrated global aerosol and climate modeling system are presented. A detailed global tropospheric chemistry and aerosol model that predicts concentrations of oxidants as well as aerosols and aerosol precursors, is coupled to a general circulation model that predicts both cloud water mass and cloud droplet number. Both number and mass of several externally-mixed aerosol size modes are predicted, with internal mixing assumed for the different aerosol components within each mode. Predicted aerosol species include sulfate, organic and black carbon, soil dust, and sea salt. The models use physically-based treatments of aerosol radiative properties (including dependence on relative humidity) and aerosol activation as cloud condensation nuclei. Parallel simulations with and without anthropogenic sulfate aerosol are performed for a global domain. The global and annual mean direct and indirect radiative forcing due to anthropogenic sulfate are estimated to be -0.3 to -0.5 and -1.5 to -3.0 W m-2, respectively. The radiative forcing is sensitive to the model's horizontal resolution, the use of predicted vs. analyzed relative humidity, the prediction vs. diagnosis of aerosol number and droplet number, and the parameterization of droplet collision/coalescence. About half of the indirect radiative forcing is due to changes in droplet radius and half to increased cloud liquid water.

  13. Comparisons of Airborne HSRL and Modeled Aerosol Profiles

    NASA Astrophysics Data System (ADS)

    Ferrare, R. A.; Burton, S. P.; Hostetler, C. A.; Hair, J. W.; Ismail, S.; Rogers, R. R.; Notari, A.; Berkoff, T.; Butler, C. F.; Collins, J. E., Jr.; Fenn, M. A.; Scarino, A. J.; Clayton, M.; Mueller, D.; Chemyakin, E.; Fast, J. D.; Berg, L. K.; Randles, C. A.; Colarco, P. R.; daSilva, A.

    2014-12-01

    Aerosol profiles derived from a regional and a global model are compared with aerosol profiles acquired by NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidars (HSRLs) during recent field missions. We compare simulated aerosol profiles obtained from the WRF-Chem regional model with those measured by the airborne HSRL-2 instrument over the Atlantic Ocean east of Cape Cod in July 2012 during the Department of Energy Two-Column Aerosol Project (TCAP). While deployed on the LaRC King Air during TCAP, HSRL-2 acquired profiles of aerosol extinction at 355 and 532 nm, as well as aerosol backscatter and depolarization at 355, 532, and 1064 nm. Additional HSRL-2 data products include profiles of aerosol type, mixed layer depth, and aerosol microphysical parameters (e.g. effective radius, concentration). The HSRL-2 and WRF-Chem aerosol profiles are compared along the aircraft flight tracks. HSRL-2 profiles acquired during the NASA Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission over Houston during September 2013 are compared with the NASA Goddard Earth Observing System global model, version 5 (GEOS-5) profiles. In addition to comparing backscatter and extinction profiles, the fraction of aerosol extinction and optical thickness from various aerosol species from GEOS-5 are compared with aerosol extinction and optical thickness contributed by aerosol types derived from HSRL-2 data. We also compare aerosol profiles modeled by GEOS-5 with those measured by the airborne LaRC DIAL/HSRL instrument during August and September 2013 when it was deployed on the NASA DC-8 for the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) mission. DIAL/HSRL measured extinction (532 nm), backscatter (532 and 1064 nm), and depolarization profiles (532 and 1064 nm) in both nadir and zenith directions during long transects over the

  14. Sensitivity of remote aerosol distributions to representation of cloud-aerosol interactions in a global climate model

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Rasch, P. J.; Wang, M.; Liu, X.; Ghan, S. J.; Qian, Y.; Yoon, J.-H.; Ma, P.-L.; Velu, V.

    2013-01-01

    Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model (PNNL-MMF) that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the sub-grid scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a10-fold (5-fold) increase in the winter (summer) months, resulting in a much better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in

  15. Volcanic Aerosol Radiative Properties

    NASA Technical Reports Server (NTRS)

    Lacis, Andrew

    2015-01-01

    Large sporadic volcanic eruptions inject large amounts of sulfur bearing gases into the stratosphere which then get photochemically converted to sulfuric acid aerosol droplets that exert a radiative cooling effect on the global climate system lasting for several years.

  16. Palaeoclimate: Aerosols and rainfall

    NASA Astrophysics Data System (ADS)

    Partin, Jud

    2015-03-01

    Instrumental records have hinted that aerosol emissions may be shifting rainfall over Central America southwards. A 450-year-long precipitation reconstruction indicates that this shift began shortly after the Industrial Revolution.

  17. Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

    NASA Technical Reports Server (NTRS)

    Wang, Jian; Collins, Don; Covert, David; Elleman, Robert; Ferrare, Richard A.; Gasparini, Roberto; Jonsson, Haflidi; Ogren, John; Sheridan, Patrick; Tsay, Si-Chee

    2006-01-01

    Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

  18. Modelling Aerosol Dispersion in Urban Street Canyons

    NASA Astrophysics Data System (ADS)

    Tay, B. K.; Jones, D. P.; Gallagher, M. W.; McFiggans, G. B.; Watkins, A. P.

    2009-04-01

    flux is the loss of aerosols to the urban canopy and the net effect of mean flow flux is to re-entrain aerosols into the canyon, the net effect of both factors is a net loss of aerosols. Consistent with previous measurement campaigns, a strong correlation was found between turbulent flux and inflow conditions (wind speed and turbulent intensities). Also, the poorer ventilation characteristic of deep canyons is demonstrated. However, when the contribution of buoyancy to the vertical velocity component of the flow field is considered, it was found that the contribution of mean flow flux to the net flux could surpass that of turbulent flux when buoyancy is important. This implies that both mean flow flux and turbulent flux have to be considered together when buoyancy effects are important to the flow regime considered. The multiphase model was further extended to investigate condensational growth of aerosols within the street canyon due to the presence of organic vapour. Condensational growth is incorporated as a function of the partial pressure of the condensing species and its saturation vapour pressure. The size distribution evolution pattern within the canyon and the sensitivity of aerosol growth to the characteristics of the organic vapour and flow conditions will be discussed.

  19. Emergency Protection from Aerosols

    SciTech Connect

    Cristy, G.A.

    2001-11-13

    Expedient methods were developed that could be used by an average person, using only materials readily available, to protect himself and his family from injury by toxic (e.g., radioactive) aerosols. The most effective means of protection was the use of a household vacuum cleaner to maintain a small positive pressure on a closed house during passage of the aerosol cloud. Protection factors of 800 and above were achieved.

  20. Emergency protection from aerosols

    SciTech Connect

    Cristy, G.A.; Chester, C.V.

    1981-07-01

    Expedient methods were developed that could be used by an average person, using only materials readily available, to protect himself and his family from injury by toxic (e.g., radioactive) aerosols. The most effective means of protection was the use of a household vacuum cleaner to maintain a small positive pressure on a closed house during passage of the aerosol cloud. Protection factors of 800 and above were achieved.

  1. Monodisperse aerosol generator

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  2. MISR Aerosol Typing

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2014-01-01

    AeroCom is an open international initiative of scientists interested in the advancement of the understanding of global aerosol properties and aerosol impacts on climate. A central goal is to more strongly tie and constrain modeling efforts to observational data. A major element for exchanges between data and modeling groups are annual meetings. The meeting was held September 20 through October 2, 1014 and the organizers would like to post the presentations.

  3. Variability of aerosol and spectral lidar and backscatter and extinction ratios of key aerosol types derived from selected Aerosol Robotic Network locations

    NASA Astrophysics Data System (ADS)

    Cattrall, Christopher; Reagan, John; Thome, Kurt; Dubovik, Oleg

    2005-05-01

    The lidar (extinction-to-backscatter) ratios at 0.55 and 1.02 μm and the spectral lidar, extinction, and backscatter ratios of climatically relevant aerosol species are computed on the basis of selected retrievals of aerosol properties from 26 Aerosol Robotic Network (AERONET) sites across the globe. The values, obtained indirectly from sky radiance and solar transmittance measurements, agree very well with values from direct observations. Low mean values of the lidar ratio, Sa, at 0.55 μm for maritime (27 sr) aerosols and desert dust (42 sr) are clearly distinguishable from biomass burning (60 sr) and urban/industrial pollution (71 sr). The effects of nonsphericity of mineral dust are shown, demonstrating that particle shape must be taken into account in any spaceborne lidar inversion scheme. A new aerosol model representing pollution over Southeast Asia is introduced since lidar (58 sr), color lidar, and extinction ratios in this region are distinct from those over other urban/industrial centers, owing to a greater number of large particles relative to fine particles. This discrimination promises improved estimates of regional climate forcing by aerosols containing black carbon and is expected to be of utility to climate modeling and remote sensing communities. The observed variability of the lidar parameters, combined with current validated aerosol data products from Moderate Resolution Imaging Spectroradiometer (MODIS), will afford improved accuracy in the inversion of spaceborne lidar data over both land and ocean.

  4. RACORO aerosol data processing

    SciTech Connect

    Elisabeth Andrews

    2011-10-31

    The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurements and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.

  5. Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

    NASA Astrophysics Data System (ADS)

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

    2007-12-01

    Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (<0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. Samples were collected on quartz fiber filters with high volume impactor samplers. Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples. These continuous spectra have also been used to obtain the

  6. Aerosol dynamics in ship tracks

    NASA Astrophysics Data System (ADS)

    Russell, Lynn M.; Seinfeld, John H.; Flagan, Richard C.; Ferek, Ronald J.; Hegg, Dean A.; Hobbs, Peter V.; Wobrock, Wolfram; Flossmann, Andrea I.; O'Dowd, Colin D.; Nielsen, Kurt E.; Durkee, Phillip A.

    1999-01-01

    Ship tracks are a natural laboratory to isolate the effect of anthropogenic aerosol emissions on cloud properties. The Monterey Area Ship Tracks (MAST) experiment in the Pacific Ocean west of Monterey, California, in June 1994, provides an unprecedented data set for evaluating our understanding of the formation and persistence of the anomalous cloud features that characterize ship tracks. The data set includes conditions in which the marine boundary layer is both clean and continentally influenced. Two case studies during the MAST experiment are examined with a detailed aerosol microphysical model that considers an external mixture of independent particle populations. The model allows tracking individual particles through condensational and coagulational growth to identify the source of cloud condensation nuclei (CCN). In addition, a cloud microphysics model was employed to study specific effects of precipitation. Predictions and observations reveal important differences between clean (particle concentrations below 150 cm-3) and continentally influenced (particle concentrations above 400 cm-3) background conditions: in the continentally influenced conditions there is a smaller change in the cloud effective radius, drop number and liquid water content in the ship track relative to the background than in the clean marine case. Predictions of changes in cloud droplet number concentrations and effective radii are consistent with observations although there is significant uncertainty in the absolute concentrations due to a lack of measurements of the plume dilution. Gas-to-particle conversion of sulfur species produced by the combustion of ship fuel is predicted to be important in supplying soluble aerosol mass to combustion-generated particles, so as to render them available as CCN. Studies of the impact of these changes on the cloud's potential to precipitate concluded that more complex dynamical processes must be represented to allow sufficiently long drop

  7. Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

    Organic aerosol can exhibit different phase states in response to changes in relative humidity (RH), thereby influencing heterogeneous reaction rates with trace gas species. OH radical uptake by laboratory-generated levoglucosan and methyl-nitrocatechol particles, serving as surrogates for biomass burning aerosol, is determined as a function of RH. Increasing RH lowers the viscosity of amorphous levoglucosan aerosol particles enabling enhanced OH uptake. Conversely, OH uptake by methyl-nitrocatechol aerosol particles is suppressed at higher RH as a result of competitive coadsorption of H2O that occupies reactive sites. This is shown to have substantial impacts on organic aerosol lifetimes with respect to OH oxidation. The results emphasize the importance of organic aerosol phase state to accurately describe the multiphase chemical kinetics and thus chemical aging process in atmospheric models to better represent the evolution of organic aerosol and its role in air quality and climate.

  8. Thermodynamic Characterization of Mexico City Aerosol during MILAGRO 2006

    SciTech Connect

    Fountoukis, C.; Nenes, A.; Sullivan, A.; Weber, R.; VanReken, T.; Fischer, M.; Matias, E.; Moya, M.; Farmer, D.; Cohen, R.C.

    2008-12-05

    Fast measurements of aerosol and gas-phase constituents coupled with the ISORROPIA-II thermodynamic equilibrium model are used to study the partitioning of semivolatile inorganic species and phase state of Mexico City aerosol sampled at the T1 site during the MILAGRO 2006 campaign. Overall, predicted semivolatile partitioning agrees well with measurements. PM{sub 2.5} is insensitive to changes in ammonia but is to acidic semivolatile species. For particle sizes up to 1 {micro}m diameter, semi-volatile partitioning requires 30-60 min to equilibrate; longer time is typically required during the night and early morning hours. When the aerosol sulfate-to-nitrate molar ratio is less than unity, predictions improve substantially if the aerosol is assumed to follow the deliquescent phase diagram. Treating crustal species as 'equivalent sodium' (rather than explicitly) in the thermodynamic equilibrium calculations introduces important biases in predicted aerosol water uptake, nitrate and ammonium; neglecting crustals further increases errors dramatically. This suggests that explicitly considering crustals in the thermodynamic calculations is required to accurately predict the partitioning and phase state of aerosols.

  9. Application of the VH-TDMA technique to coastal ambient aerosols

    NASA Astrophysics Data System (ADS)

    Johnson, G.; Ristovski, Z.; Morawska, L.

    2004-08-01

    A newly developed VH-TDMA has been used for the first time to measure the volatile fractions and post volatilization hygroscopic growth factors of ambient aerosols in the coastal marine and urban environments. The results are compared with comparable data for laboratory generated aerosols of known composition. Measurements conducted on coastal Aitken mode particles showed volatilization behavior similar to laboratory generated aerosols composed of methane sulfonic acid and ammonium sulfate. Measurements conducted on 60 nm particles during nucleation events contained a greater fraction of material with similar volatility to ammonium sulfate than was found at other times. These particles were hygroscopic but less so than pure ammonium sulfate. Measurements conducted in the Brisbane central business district during sea breeze conditions show similar behavior to the coastal aerosol, but with additional low volatility species. This aerosol may originate from urban sources or from marine particles acquiring additional secondary aerosol species during transport.

  10. Chemical distribution in high-solids paint overspray aerosols.

    PubMed

    D'Arcy, J B; Chan, T L

    1990-03-01

    The chemical composition of high-solids basecoat paint overspray aerosols was determined as a function of particle size. Detailed information on the chemical composition of the overspray aerosols is important in health hazard evaluation since the composition and distribution within the airborne particles may differ significantly from the bulk paint material. This study was conducted in a typical down-draft paint booth equipped with air-atomized spray painting equipment. A fixed paint target was used to simulate typical overspray generation conditions and the aerosols were collected isokinetically with a seven-stage cascade impactor for size-fractionated analysis. The overspray aerosol from six paints consisted of organic paint binders with varying amounts of inorganic species as pigments or luster enhancers. These overspray aerosols had mass median aerodynamic diameters (MMAD) ranging from 2.9 to 9.7 microns. The size-fractionated paint samples collected on the impaction stages were analyzed by energy dispersive X-ray spectrometry on a scanning electron microscope (SEM-EDXRS) to identify the metallic elements. Atomic absorption spectrometry was used to determine the mass distribution of aluminum and iron as indicators of nonuniform distribution. Three of the aerosols containing aluminum were found to have bimodal distributions with most aluminum distributions having cumulative MMADs larger than the total aerosol. Iron in the aerosols was bimodal for three of the paints with all samples having an overall iron MMAD less than or equal to the overspray aerosol MMAD. Analysis using ultraviolet spectrometry revealed that the organic compounds present in the size-fractionated particulate samples consisted of a single, polydispersed mode with an MMAD similar to that of the total overspray aerosol.(ABSTRACT TRUNCATED AT 250 WORDS) PMID:2327324

  11. Chemical distribution in high-solids paint overspray aerosols

    SciTech Connect

    D'Arcy, J.B.; Chan, T.L. )

    1990-03-01

    The chemical composition of high-solids basecoat paint overspray aerosols was determined as a function of particle size. Detailed information on the chemical composition of the overspray aerosols is important in health hazard evaluation since the composition and distribution within the airborne particles may differ significantly from the bulk paint material. This study was conducted in a typical down-draft paint booth equipped with air-atomized spray painting equipment. A fixed paint target was used to simulate typical overspray generation conditions and the aerosols were collected isokinetically with a seven-stage cascade impactor for size-fractionated analysis. The overspray aerosol from six paints consisted of organic paint binders with varying amounts of inorganic species as pigments or luster enhancers. These overspray aerosols had mass median aerodynamic diameters (MMAD) ranging from 2.9 to 9.7 microns. The size-fractionated paint samples collected on the impaction stages were analyzed by energy dispersive X-ray spectrometry on a scanning electron microscope (SEM-EDXRS) to identify the metallic elements. Atomic absorption spectrometry was used to determine the mass distribution of aluminum and iron as indicators of nonuniform distribution. Three of the aerosols containing aluminum were found to have bimodal distributions with most aluminum distributions having cumulative MMADs larger than the total aerosol. Iron in the aerosols was bimodal for three of the paints with all samples having an overall iron MMAD less than or equal to the overspray aerosol MMAD. Analysis using ultraviolet spectrometry revealed that the organic compounds present in the size-fractionated particulate samples consisted of a single, polydispersed mode with an MMAD similar to that of the total overspray aerosol.

  12. Sensitivity of Remote Aerosol Distributions to Representation of Cloud-Aerosol Interactions in a Global Climate Model

    SciTech Connect

    Wang, Hailong; Easter, Richard C.; Rasch, Philip J.; Wang, Minghuai; Liu, Xiaohong; Ghan, Steven J.; Qian, Yun; Yoon, Jin-Ho; Ma, Po-Lun; Vinoj, V.

    2013-06-05

    Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model (PNNL-MMF) that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the sub-grid scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a10-fold (5-fold) increase in the winter (summer) months, resulting in a much better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in

  13. Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

    NASA Astrophysics Data System (ADS)

    Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

    2015-12-01

    Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

  14. 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.

  15. Biological aerosol background characterization

    NASA Astrophysics Data System (ADS)

    Blatny, Janet; Fountain, Augustus W., III

    2011-05-01

    To provide useful information during military operations, or as part of other security situations, a biological aerosol detector has to respond within seconds or minutes to an attack by virulent biological agents, and with low false alarms. Within this time frame, measuring virulence of a known microorganism is extremely difficult, especially if the microorganism is of unknown antigenic or nucleic acid properties. Measuring "live" characteristics of an organism directly is not generally an option, yet only viable organisms are potentially infectious. Fluorescence based instruments have been designed to optically determine if aerosol particles have viability characteristics. Still, such commercially available biological aerosol detection equipment needs to be improved for their use in military and civil applications. Air has an endogenous population of microorganisms that may interfere with alarm software technologies. To design robust algorithms, a comprehensive knowledge of the airborne biological background content is essential. For this reason, there is a need to study ambient live bacterial populations in as many locations as possible. Doing so will permit collection of data to define diverse biological characteristics that in turn can be used to fine tune alarm algorithms. To avoid false alarms, improving software technologies for biological detectors is a crucial feature requiring considerations of various parameters that can be applied to suppress alarm triggers. This NATO Task Group will aim for developing reference methods for monitoring biological aerosol characteristics to improve alarm algorithms for biological detection. Additionally, they will focus on developing reference standard methodology for monitoring biological aerosol characteristics to reduce false alarm rates.

  16. MISR UAE2 Aerosol Versioning

    Atmospheric Science Data Center

    2013-03-21

    ... the MISR aerosol microphysical properties are "Beta." Uncertainty envelopes for the aerosol optical depths are given in  Kahn et ... particle microphysical property validation is in progress, uncertainty envelopes on particle size distribution, shape, and ...

  17. Atmospheric Chemistry: Nature's plasticized aerosols

    NASA Astrophysics Data System (ADS)

    Ziemann, Paul J.

    2016-01-01

    The structure of atmospheric aerosol particles affects their reactivity and growth rates. Measurements of aerosol properties over the Amazon rainforest indicate that organic particles above tropical rainforests are simple liquid drops.

  18. Numerical simulation of advection fog formation on multi-disperse aerosols due to combustion-related pollutants

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Liaw, G. S.

    1980-01-01

    The effects of multi-disperse distribution of the aerosol population are presented. Single component and multi-component aerosol species on the condensation/nucleation processes which affect the reduction in visibility are described. The aerosol population with a high particle concentration provided more favorable conditions for the formation of a denser fog than the aerosol population with a greater particle size distribution when the value of the mass concentration of the aerosols was kept constant. The results were used as numerical predictions of fog formation. Two dimensional observations in horizontal and vertical coordinates, together with time-dependent measurements were needed as initial values for the following physical parameters: (1)wind profiles; (2) temperature profiles; (3) humidity profiles; (4) mass concentration of aerosol particles; (5) particle size distribution of aerosols; and (6) chemical composition of aerosols. Formation and dissipation of advection fog, thus, can be forecasted numerically by introducing initial values obtained from the observations.

  19. Secondary Ion Mass Spectrometry of Environmental Aerosols

    SciTech Connect

    Gaspar, Daniel J.; Cliff, John B.

    2010-08-01

    Atmospheric particles influence many aspects of climate, air quality and human health. Understanding the composition, chemistry and behavior of atmospheric aerosols is a key remaining challenge in improving climate models. Furthermore, particles may be traced back to a particular source based on composition, stable isotope ratios, or the presence of particular surface chemistries. Finally, the characterization of atmospheric particles in the workplace plays an important role in understanding the potential for exposure and environmental and human health effects to engineered and natural nanoscale particles. Secondary ion mass spectrometry (SIMS) is a useful tool in determining any of several aspects of the structure, composition and chemistry of these particles. Often used in conjunction with other surface analysis and electron microscopy methods, SIMS has been used to determine or confirm reactions on and in particles, the presence of particular organic species on the surface of atmospheric aerosols and several other interesting and relevant findings. Various versions of SIMS instruments – dynamic SIMS, time of flight secondary ion mass spectrometry or TOF-SIMS, nanoSIMS – have been used to determine specific aspects of aerosol structure and chemistry. This article describes the strengths of each type of SIMS instrument in the characterization of aerosols, along with guidance on sample preparation, specific characterization specific to the particular information sought in the analysis. Examples and guidance are given for each type of SIMS analysis.

  20. Toward Investigating Optically Trapped Organic Aerosols with CARS Microspectroscopy

    NASA Astrophysics Data System (ADS)

    Voss, L. F.

    2009-12-01

    The Intergovernmental Panel on Climate Change notes the huge uncertainty in the effect that atmospheric aerosols play in determining overall global temperature, specifically in their ability to nucleate clouds. To better understand aerosol chemistry, the novel coupling of gradient force optical trapping with broad bandwidth coherent anti-Stokes Raman scattering (CARS) spectroscopy is being developed to study single particles suspended in air. Building on successful designs employed separately for the techniques, this hybrid technology will be used to explain how the oxidation of organic compounds changes the chemical and physical properties of aerosols. By trapping the particles, an individual aerosol can be studied for up to several days. Using a broad bandwidth pulse for one of the incident beams will result in a Raman vibrational spectrum from every laser pulse. Combined with signal enhancement due to resonance and coherence of nonlinear CARS spectroscopy, this technique will allow for acquisition of data on the millisecond time scale, facilitating the study of dynamic processes. This will provide insights on how aerosols react with and absorb species from the gas phase. These experiments will increase understanding of aerosol oxidation and growth mechanisms and the effects that aerosols have on our atmosphere and climate. Progress in efforts developing this novel technique to study model systems is presented.

  1. Global simulation of chemistry and radiative forcing of mineral aerosols

    SciTech Connect

    Zhang, Yang; Easter, R.C.; Ghan, S.J.; Leung, L.R.

    1996-12-31

    Mineral aerosols are increasingly gaining attention because of their roles in atmospheric chemistry and climate system. A global three-dimensional aerosol/chemistry model (GChM) coupled with a general circulation model (GCM) is used to simulate the sources/sinks, chemistry and radiative forcing of mineral aerosols. Regional and seasonal variations in distribution of mineral aerosols are predicted based on vegetation types, threshold wind velocities and soil moisture data. The role of mineral aerosols as a reactive surface available for heterogeneous uptake of gas-phase species in the global atmosphere is investigated along with their impact on the tropospheric sulfur cycle and the photochemical oxidant cycle. In particular, the heterogeneous surface reactions of SO{sub 2}, H{sub 2}SO{sub 4}, NO{sub 3}, N{sub 2}O{sub 5}, HNO{sub 3}, O{sub 3}, OH, HO{sub 2}, H{sub 2}O{sub 2} and CH{sub 3}O{sub 2} on mineral aerosols are simulated. The direct radiative forcing by mineral aerosols and the indirect forcing through influencing droplet number concentration are further estimated. The model simulation results are analyzed and compared against the available observational data.

  2. Aerosol characterization with lidar methods

    NASA Astrophysics Data System (ADS)

    Sugimoto, Nobuo; Nishizawa, Tomoaki; Shimizu, Atsushi; Matsui, Ichiro

    2014-08-01

    Aerosol component analysis methods for characterizing aerosols were developed for various types of lidars including polarization-sensitive Mie scattering lidars, multi-wavelength Raman scattering lidars, and multi-wavelength highspectral- resolution lidars. From the multi-parameter lidar data, the extinction coefficients for four aerosol components can be derived. The microphysical parameters such as single scattering albedo and effective radius can be also estimated from the derived aerosol component distributions.

  3. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3 aerosol during the 2013 Southern Oxidant and Aerosol Study

    SciTech Connect

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; Ault, A.; Bondy, A.; Takahama, S.; Modini, R. L.; Baumann, K.; Edgerton, E.; Knote, C.; Laskin, A.; Wang, B.; Fry, J. L.

    2015-09-25

    Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3 is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3 and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.

  4. Aerosol Quality Monitor (AQUAM)

    NASA Astrophysics Data System (ADS)

    Liang, X.; Ignatov, A.

    2011-12-01

    The Advanced Clear-Sky Processor for Oceans (ACSPO) developed at NESDIS generates three products from AVHRR, operationally: clear sky radiances in all bands, and sea surface temperature (SST) derived from clear-sky brightness temperatures (BT) in Ch3B (centered at 3.7 μm), Ch4 (11 μm) and Ch5 (12 μm), and aerosol optical depths (AOD) derived from clear-sky reflectances in Ch1 (0.63), Ch2 (0.83) and Ch3A (1.61 μm). An integral part of ACSPO is the fast Community Radiative Transfer Model (CRTM), which calculates first-guess clear-sky BTs using global NCEP forecast atmospheric and Reynolds SST fields. Simulated BTs are employed in ACSPO for improved cloud screening, physical (RTM-based) SST inversions, and to monitor and validate satellite BTs. The model minus observation biases are monitored online in near-real time using the Monitoring IR Clear-sky radiances over Oceans for SST (MICROS; http://www.star.nesdis.noaa.gov/sod/sst/micros/). A persistent positive M-O bias is observed in MICROS, partly attributed to missing aerosol in CRTM input, causing "M" to be warmer than "O". It is thus necessary to include aerosols in CRTM and quantify their effects on AVHRR BTs and SSTs. However, sensitivity of thermal bands to aerosol is only minimal, and use of solar reflectance bands is preferable to evaluate the accuracy of CRTM modeling, with global aerosol fields as input (from e.g. Goddard Chemistry Aerosol Radiation and Transport, GOCART, or Navy Aerosol Analysis and Prediction System, NAAPS). Once available, the corresponding M-O biases in solar reflectance bands will be added to MICROS. Also, adding CRTM simulated reflectances in ACSPO would greatly improve cloud detection, help validate CRTM in the solar reflectance bands, and assist aerosol retrievals. Running CRTM with global aerosol as input is very challenging, computationally. While CRTM is being optimized to handle such global scattering computations, a near-real time web-based Aerosol Quality Monitor (AQUAM

  5. Formation of halogen-induced secondary organic aerosol (XOA)

    NASA Astrophysics Data System (ADS)

    Kamilli, Katharina; Ofner, Johannes; Zetzsch, Cornelius; Held, Andreas

    2013-04-01

    Reactive halogen species (RHS) are very important due to their potential of stratospheric ozone depletion and surface ozone destruction. RHS seem to interact with precursors of secondary organic aerosol (SOA) similarly to common atmospheric oxidants like OH radicals and ozone. The potential interaction of RHS with preformed SOA has recently been studied (Ofner et al., 2012). Although aerosol formation from reaction of RHS with typical SOA precursors was previously studied (e.g. Cai et al., 2006), no data are available on bromine-induced aerosol formation from organic precursors yet. An aerosol smog-chamber was used to examine the halogen-induced secondary organic aerosol (XOA) formation under atmospheric conditions using simulated sunlight. With a concentration of 10 ppb for the organic precursor, 2 ppb for molecular chlorine, and 10 ppb for molecular bromine, the experimental setup is close to ambient conditions. By combined measurements of the aerosol size distribution, ozone and NOx mixing ratios, as well as the decay of the organic precursor, aerosol yields and aerosol growth rates were determined. The decay of the organic precursor was analyzed by capillary gas chromatography coupled with flame-ionization detection (GC-FID) and the aerosol size distribution was measured using a Scanning Mobility Particle Sizer (SMPS). Additionally, with the decay rate of the precursor and the calculated photolysis rates of molecular halogen species, based on the well-known spectrum of the solar simulator, mechanistic details on the XOA formation pathways can be determined. We observed XOA formation even at very low precursor and RHS concentrations with a diameter mode at 10-20 nm and a number concentration up to 1000000 particles cm-3. While the XOA formation from chlorine is very rapid, the interaction of bromine with the organic precursors is about five times slower. The aerosol yield reached maximum values of 0.01 for the reaction of chlorine with α-pinene and 0.0004 for

  6. Indian aerosols: present status.

    PubMed

    Mitra, A P; Sharma, C

    2002-12-01

    This article presents the status of aerosols in India based on the research activities undertaken during last few decades in this region. Programs, like International Geophysical Year (IGY), Monsoon Experiment (MONEX), Indian Middle Atmospheric Program (IMAP) and recently conducted Indian Ocean Experiment (INDOEX), have thrown new lights on the role of aerosols in global change. INDOEX has proved that the effects of aerosols are no longer confined to the local levels but extend at regional as well as global scales due to occurrence of long range transportation of aerosols from source regions along with wind trajectories. The loading of aerosols in the atmosphere is on rising due to energy intensive activities for developmental processes and other anthropogenic activities. One of the significant observation of INDOEX is the presence of high concentrations of carbonaceous aerosols in the near persistent winter time haze layer over tropical Indian Ocean which have probably been emitted from the burning of fossil-fuels and biofuels in the source region. These have significant bearing on the radiative forcing in the region and, therefore, have potential to alter monsoon and hydrological cycles. In general, the SPM concentrations have been found to be on higher sides in ambient atmosphere in many Indian cities but the NOx concentrations have been found to be on lower side. Even in the haze layer over Indian Ocean and surrounding areas, the NOx concentrations have been reported to be low which is not conducive of O3 formation in the haze/smog layer. The acid rain problem does not seem to exist at the moment in India because of the presence of neutralizing soil dust in the atmosphere. But the high particulate concentrations in most of the cities' atmosphere in India are of concern as it can cause deteriorated health conditions. PMID:12492171

  7. Indian aerosols: present status.

    PubMed

    Mitra, A P; Sharma, C

    2002-12-01

    This article presents the status of aerosols in India based on the research activities undertaken during last few decades in this region. Programs, like International Geophysical Year (IGY), Monsoon Experiment (MONEX), Indian Middle Atmospheric Program (IMAP) and recently conducted Indian Ocean Experiment (INDOEX), have thrown new lights on the role of aerosols in global change. INDOEX has proved that the effects of aerosols are no longer confined to the local levels but extend at regional as well as global scales due to occurrence of long range transportation of aerosols from source regions along with wind trajectories. The loading of aerosols in the atmosphere is on rising due to energy intensive activities for developmental processes and other anthropogenic activities. One of the significant observation of INDOEX is the presence of high concentrations of carbonaceous aerosols in the near persistent winter time haze layer over tropical Indian Ocean which have probably been emitted from the burning of fossil-fuels and biofuels in the source region. These have significant bearing on the radiative forcing in the region and, therefore, have potential to alter monsoon and hydrological cycles. In general, the SPM concentrations have been found to be on higher sides in ambient atmosphere in many Indian cities but the NOx concentrations have been found to be on lower side. Even in the haze layer over Indian Ocean and surrounding areas, the NOx concentrations have been reported to be low which is not conducive of O3 formation in the haze/smog layer. The acid rain problem does not seem to exist at the moment in India because of the presence of neutralizing soil dust in the atmosphere. But the high particulate concentrations in most of the cities' atmosphere in India are of concern as it can cause deteriorated health conditions.

  8. Easy Volcanic Aerosol

    NASA Astrophysics Data System (ADS)

    Toohey, Matthew; Stevens, Bjorn; Schmidt, Hauke; Timmreck, Claudia

    2016-04-01

    Radiative forcing by stratospheric sulfate aerosol of volcanic origin is one of the strongest drivers of natural climate variability. Transient model simulations attempting to match observed climate variability, such as the CMIP historical simulations, rely on volcanic forcing reconstructions based on observations of a small sample of recent eruptions and coarse proxy data for eruptions before the satellite era. Volcanic forcing data sets used in CMIP5 were provided either in terms of optical properties, or in terms of sulfate aerosol mass, leading to significant inter-model spread in the actual volcanic radiative forcing produced by models and in their resulting climate responses. It remains therefore unclear to what degree inter-model spread in response to volcanic forcing represents model differences or variations in the forcing. In order to isolate model differences, Easy Volcanic Aerosol (EVA) provides an analytic representation of volcanic stratospheric aerosol forcing, based on available observations and aerosol model results, prescribing the aerosol's radiative properties and primary modes of spatial and temporal variability. In contrast to regriddings of observational data, EVA allows for the production of physically consistent forcing for historic and hypothetical eruptions of varying magnitude, source latitude, and season. Within CMIP6, EVA will be used to reconstruct volcanic forcing over the past 2000 years for use in the Paleo-Modeling Intercomparison Project (PMIP), and will provide forcing sets for VolMIP experiments aiming to quantify model uncertainty in the response to volcanic forcing. Here, the functional form of EVA will be introduced, along with illustrative examples including the EVA-based reconstruction of volcanic forcing over the historical period, and that of the 1815 Tambora eruption.

  9. 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.

  10. Dry season aerosol iron solubility in tropical northern Australia

    NASA Astrophysics Data System (ADS)

    Winton, V. Holly L.; Edwards, Ross; Bowie, Andrew R.; Keywood, Melita; Williams, Alistair G.; Chambers, Scott D.; Selleck, Paul W.; Desservettaz, Maximilien; Mallet, Marc D.; Paton-Walsh, Clare

    2016-10-01

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

  11. Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

    NASA Technical Reports Server (NTRS)

    Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin

    2003-01-01

    During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

  12. simplified aerosol representations in global modeling

    NASA Astrophysics Data System (ADS)

    Kinne, Stefan; Peters, Karsten; Stevens, Bjorn; Rast, Sebastian; Schutgens, Nick; Stier, Philip

    2015-04-01

    The detailed treatment of aerosol in global modeling is complex and time-consuming. Thus simplified approaches are investigated, which prescribe 4D (space and time) distributions of aerosol optical properties and of aerosol microphysical properties. Aerosol optical properties are required to assess aerosol direct radiative effects and aerosol microphysical properties (in terms of their ability as aerosol nuclei to modify cloud droplet concentrations) are needed to address the indirect aerosol impact on cloud properties. Following the simplifying concept of the monthly gridded (1x1 lat/lon) aerosol climatology (MAC), new approaches are presented and evaluated against more detailed methods, including comparisons to detailed simulations with complex aerosol component modules.

  13. Effect of Hydrophilic Organic Seed Aerosols on Secondary Organic Aerosol Formation from Ozonolysis of α-Pinene

    SciTech Connect

    Song, Chen; Zaveri, Rahul A.; Shilling, John E.; Alexander, M. L.; Newburn, Matthew K.

    2011-07-26

    Gas-particle partitioning theory is widely used in atmospheric models to predict organic aerosol loadings. This theory predicts that secondary organic aerosol (SOA) yield of an oxidized VOC product will increase as the mass loading of preexisting organic aerosol increases. In a previous study, we showed that the presence of model hydrophobic primary organic aerosol (POA) had no detectable effect on the secondary organic aerosol (SOA) yields from ozonolysis of {alpha}-pinene, suggesting that the condensing SOA compounds form a separate phase from the preexisting POA. However, non-polar, hydrophobic POA may gradually become polar and hydrophilic as it undergoes oxidative aging while POA formed from biomass burning is already somewhat polar and hydrophilic. In this study, we investigate the effects of model hydrophilic POA such as fulvic acid, adipic acid and citric acid on the gas-particle partitioning of SOA from {alpha}-pinene ozonolysis. The results show that only citric acid seed significantly enhances the absorption of {alpha}-pinene SOA into the particle-phase. The other two POA seed particles have negligible effect on the {alpha}-pinene SOA yields, suggesting that {alpha}-pinene SOA forms a well-mixed organic aerosol phase with citric acid while a separate phase with adipic acid and fulvic acid. This finding highlights the need to improve the thermodynamics treatment of organics in current aerosol models that simply lump all hydrophilic organic species into a single phase, thereby potentially introducing an erroneous sensitivity of SOA mass to emitted POA.

  14. Highly stable aerosol generator

    SciTech Connect

    DeFord, Henry S.; Clark, Mark L.

    1981-01-01

    An improved compressed air nebulizer has been developed such that a uniform aerosol particle size and concentration may be produced over long time periods. This result is achieved by applying a vacuum pressure to the makeup assembly and by use of a vent tube between the atmosphere and the makeup solution. By applying appropriate vacuum pressures to the makeup solution container and by proper positioning of the vent tube, a constant level of aspirating solution may be maintained within the aspirating assembly with aspirating solution continuously replaced from the makeup solution supply. This device may also be adapted to have a plurality of aerosol generators and only one central makeup assembly.

  15. Highly stable aerosol generator

    DOEpatents

    DeFord, H.S.; Clark, M.L.

    1981-11-03

    An improved compressed air nebulizer has been developed such that a uniform aerosol particle size and concentration may be produced over long time periods. This result is achieved by applying a vacuum pressure to the makeup assembly and by use of a vent tube between the atmosphere and the makeup solution. By applying appropriate vacuum pressures to the makeup solution container and by proper positioning of the vent tube, a constant level of aspirating solution may be maintained within the aspirating assembly with aspirating solution continuously replaced from the makeup solution supply. This device may also be adapted to have a plurality of aerosol generators and only one central makeup assembly. 2 figs.

  16. Stratospheric Aerosol Measurements

    NASA Technical Reports Server (NTRS)

    Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

    1998-01-01

    Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

  17. An interfacial mechanism for cloud droplet formation on organic aerosols

    NASA Astrophysics Data System (ADS)

    Ruehl, Christopher R.; Davies, James F.; Wilson, Kevin R.

    2016-03-01

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.

  18. Aerosol optical properties over the midcontinental United States

    SciTech Connect

    Halthore, R.N. ); Markham, B.L.; Ferrare, R.A. ); Aro, T.O. )

    1992-11-30

    This work is part of the First International Satellite Land Surface Climatology Project (ISLSCP) Field Experiment (FIFE), an international land-surface-atmosphere experiment aimed at improving the way climate models represent energy, water, heat, and carbon exchanges, and improving the utilization of satellite based remote sensing to monitor such parameters. Here the authors report on measurements of aerosol optical depth over the FIFE site, making use of a calibrated Sun photometer. Aerosols are relevant for the impact they have on remotely sensed measurements of radiation effects on the earth. They also play a major role in cloud formation, and can impact the atmospheric concentration of minor species gases. Here the authors look at the meteorological effects on aerosols in the troposphere. Wavelength dependence gives information on the size distributions within the aerosols. During 1987 they observe mixing of gulf air with continental air over the site. They report on correlation with surface values of pressure, temperature, specific, and relative humidity.

  19. Volcanic Aerosol Evolution: Model vs. In Situ Sampling

    NASA Astrophysics Data System (ADS)

    Pfeffer, M. A.; Rietmeijer, F. J.; Brearley, A. J.; Fischer, T. P.

    2002-12-01

    Volcanoes are the most significant non-anthropogenic source of tropospheric aerosols. Aerosol samples were collected at different distances from 92°C fumarolic source at Poás Volcano. Aerosols were captured on TEM grids coated by a thin C-film using a specially designed collector. In the sampling, grids were exposed to the plume for 30-second intervals then sealed and frozen to prevent reaction before ATEM analysis to determine aerosol size and chemistry. Gas composition was established using gas chromatography, wet chemistry techniques, AAS and Ion Chromatography on samples collected directly from a fumarolic vent. SO2 flux was measured remotely by COSPEC. A Gaussian plume dispersion model was used to model concentrations of the gases at different distances down-wind. Calculated mixing ratios of air and the initial gas species were used as input to the thermo-chemical model GASWORKS (Symonds and Reed, Am. Jour. Sci., 1993). Modeled products were compared with measured aerosol compositions. Aerosols predicted to precipitate out of the plume one meter above the fumarole are [CaSO4, Fe2.3SO4, H2SO4, MgF2. Na2SO4, silica, water]. Where the plume leaves the confines of the crater, 380 meters distant, the predicted aerosols are the same, excepting FeF3 replacing Fe2.3SO4. Collected aerosols show considerable compositional differences between the sampling locations and are more complex than those predicted. Aerosols from the fumarole consist of [Fe +/- Si,S,Cl], [S +/- O] and [Si +/- O]. Aerosols collected on the crater rim consist of the same plus [O,Na,Mg,Ca], [O,Si,Cl +/- Fe], [Fe,O,F] and [S,O +/- Mg,Ca]. The comparison between results obtained by the equilibrium gas model and the actual aerosol compositions shows that an assumption of chemical and thermal equilibrium evolution is invalid. The complex aerosols collected contrast the simple formulae predicted. These findings show that complex, non-equilibrium chemical reactions take place immediately upon volcanic

  20. AEROSOL INORGANICS AND ORGANICS MODEL (AIOM) WITH USER DEFINED PROPERTIES FOR ORGANIC COMPOUNDS

    EPA Science Inventory

    The Aerosol Inorganics Model (AIM) is widely used to calculate gas/liquid/solid phase equilibrium in aerosol systems containing the species H+-NH4+-SO42--NO3--H2O over a range of tropospheric ...

  1. Anomalies in the South American Monsoon Induced by Aerosols

    NASA Technical Reports Server (NTRS)

    Lau, K. M. William; Kyu-Mong, Kim

    2007-01-01

    We have investigated the direct effects of aerosols on the water cycle of the South American monsoon using the NASA finite-volume general circulation model (fvGCM). Global aerosol forcings are computed from radiative transfer functions derived from global distributions of five species of aerosols, i.e., dust, black carbon, organic carbon, sulphate and sea salt from the Goddard Chemistry Aerosol Radiation Transport (GOCART) model. Comparing fvGCM experiments without aerosol forcing, and with different combinations of aerosol forcing, we evaluate the impacts of aerosol direct heating on the onset, maintenance and evolution of the South American summer monsoon. We find that during the pre-monsoon season (September-October-November) Saharan dust contribute to heating of the atmosphere over the central and eastern equatorial Atlantic/Africa region through the elevated heat pump mechanism. The heating generates an anomalous Walker circulation with sinking motion, and low level northeasterlies over the Caribbean and northwestern South America. The low level flow is blocked by the Andes, and turn south and southeastward, increasing the low level jet (LLJ) along the eastern slope of the Andes. The increased LLJ transports more moisture from the Atlantic and the Amazon, enhancing the moisture convergence over subtropical land regions of South America. The moisture convergence was further accelerated by atmospheric heating by biomass burning over the Amazon. The net results of the dust and biomass heating are: a) an advance of the monsoon rainy season, b) an enhanced LLJ and c) a shifting the South America monsoon land precipitation equatorward, with increased rain over southern Brazil and reduced rain over the La Plata basin. ramifications of this elevated heating heat pump mechanism in aerosol monsoon water cycle on climate variability and change will be discussed. The ramifications of this "elevated heating heat pump" mechanism in aerosol monsoom water cycle on climate

  2. Geometrical Optics of Dense Aerosols

    SciTech Connect

    Hay, Michael J.; Valeo, Ernest J.; Fisch, Nathaniel J.

    2013-04-24

    Assembling a free-standing, sharp-edged slab of homogeneous material that is much denser than gas, but much more rare ed than a solid, is an outstanding technological challenge. The solution may lie in focusing a dense aerosol to assume this geometry. However, whereas the geometrical optics of dilute aerosols is a well-developed fi eld, the dense aerosol limit is mostly unexplored. Yet controlling the geometrical optics of dense aerosols is necessary in preparing such a material slab. Focusing dense aerosols is shown here to be possible, but the nite particle density reduces the eff ective Stokes number of the flow, a critical result for controlled focusing. __________________________________________________

  3. Global atmospheric sulfur budget under volcanically quiescent conditions: Aerosol-chemistry-climate model predictions and validation

    NASA Astrophysics Data System (ADS)

    Sheng, Jian-Xiong; Weisenstein, Debra K.; Luo, Bei-Ping; Rozanov, Eugene; Stenke, Andrea; Anet, Julien; Bingemer, Heinz; Peter, Thomas

    2015-01-01

    The global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol-chemistry-climate model SOCOL-AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size-dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II-based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO2, 23% carbonyl sulfide (OCS), 4% H2S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short-lived species SO2, H2S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

  4. Mixing state of aerosols over the Indo-Gangetic Plain: Radiative forcing and heating rate

    NASA Astrophysics Data System (ADS)

    Srivastava, R.; Ramachandran, S.

    2012-12-01

    Aerosols are a major atmospheric variable which perturb the Earth-atmosphere radiation balance by absorbing and scattering the solar and terrestrial radiation. Aerosols are produced by natural and anthropogenic processes. The presence of different types of aerosol over a location and aerosols transported from long-range can give rise to different mixing states because of aging and interaction among the different aerosol species. Knowledge of the mixing state of aerosols is important for an accurate assessment of aerosols in climate forcing, as assumptions regarding the mixing state of aerosol and its effect on optical properties can give rise to uncertainties in modeling their direct and indirect effects [1]. Seasonal variations in mixing states of aerosols over an urban (Kanpur) and a rural location (Gandhi College) in the Indo-Gangetic Plain (IGP) are determined using the measured and modeled aerosol optical properties, and the impact of aerosol mixing state on aerosol radiative forcing are investigated. IGP is one of the most populated and polluted river basins in the world, rich in fertile lands and agricultural production. Kanpur is an urban, industrial and densely populated city, and has several large/small scale industries and vehicles, while Gandhi College in IGP is a rural village, located southeast of Kanpur. Aerosol optical properties obtained from Aerosol Robotic Network sun/sky radiometers [2] over these two environmentally distinct locations in Indo-Gangetic Plain are used in the study, along with aerosol vertical profiles obtained from CALIPSO (Cloud- Aerosol Lidar and Infrared Pathfinder Satellite Observations) lidar observations. Probable mixing state of aerosols is determined utilizing the aerosol optical properties viz., aerosol optical depth, single scattering albedo and asymmetry parameter. The coated-sphere Mie calculation requires the refractive index of core and shell species, and the radius of core and shell particles. Core to shell radius

  5. Sulfur speciation of single aerosol particles

    SciTech Connect

    Neubauer, K.R.; Sum, S.T.; Johnston, M.V.; Wexler, A.S.

    1995-12-31

    Sulfur enters the atmosphere as gaseous species emitted from both natural and anthropogenic sources. These species can undergo a variety of oxidation reactions that ultimately yield hexavalent sulfur aerosols. Since the final products play an important role in acid rain production and the earth`s energy balance, it is important to distinguish tetravalent and hexavalent sulfur aerosols, as well as differentiate those arising from natural and anthropogenic sources. To attain these goals the authors chose to examine five target compounds that are present in the atmosphere: sodium sulfate, ammonium sulfate, ammonium sulfite, methanesulfonic acid (MSA), and the sodium salt of hydroxymethanesulfonic acid (NaHMSA). Sodium sulfate is observed in oceanic aerosols, while both ammonium salts are observed over land. MSA is found only in the marine environment and originates solely from natural emissions, while HMSA is formed in urban hazes and primarily arises from anthropogenic sources. Thus, MSA and HMSA serve as tracers for distinguishing natural and anthropogenic sulfur emissions. To differentiate these compounds, the authors used Rapid Single-Particle Mass Spectrometry (RSMS), a method that allows single particles to be analyzed on-line and in real time. With RSMS, particles are drawn directly into the source region of a reflectron time-of-flight mass spectrometer where they are detected by light scattering of a continuous laser beam and then ablated by an excimer laser pulse. With this sequence of events, each mass spectrum results from a single laser pulse ablating a single particle.

  6. Influence of aerosols on surface reaching spectral irradiance and introduction to a new technique of estimating aerosol radiative forcing from high resolution spectral flux measurements

    NASA Astrophysics Data System (ADS)

    Rao, Roshan

    2016-04-01

    Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. We look into the approach where ground based spectral radiation flux measurement is made and along with an Radtiative transfer (RT) model, radiative forcing is estimated. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and a 3nm resolution during around 54 clear-sky days during which AOD range was around 0.01 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. The primary study involved in understanding the sensitivity of spectral flux due to change in individual aerosol species (Optical properties of Aerosols and Clouds (OPAC) classified aerosol species) using the SBDART RT model. This made us clearly distinguish the influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves matching different combinations of aerosol species in OPAC model and RT model as long as the combination which gives the minimum root mean squared deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model, aerosol radiative forcing is estimated. Also an alternate method to estimate the spectral SSA is discussed. Here, the RT model, the observed spectral flux and spectral AOD is used. Spectral AOD is input to RT model and SSA is varied till the minimum root mean squared difference between observed and simulated spectral flux from RT model is obtained. The methods discussed are limited to clear sky scenes and its accuracy to derive

  7. Influence of aerosols on surface reaching spectral irradiance and introduction to a new technique for estimating aerosol radiative forcing from spectral flux measurements

    NASA Astrophysics Data System (ADS)

    Rao, R. R.

    2015-12-01

    Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. In this study we look into the approach where ground based spectral radiation flux measurements along with an RT model is used to estimate radiative forcing. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and 3nm resolution for around 54 clear-sky days during which AOD range was around 0.1 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. All the measurements were made in the campus of Indian Institute of Science which is in the heart of Bangalore city. The primary study involved in understanding the sensitivity of spectral flux to change in the mass concentration of individual aerosol species (Optical properties of Aerosols and Clouds -OPAC classified aerosol species) using the SBDART RT model. This made us clearly distinguish the region of influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves an iterative process where the mixture of aerosol species are changed in OPAC model and RT model is run as long as the mixture which mimics the measured spectral flux within 2-3% deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model aerosol radiative forcing is estimated. The new method is limited to clear sky scenes and its accuracy to derive an optically equivalent aerosol mixture reduces when diffuse component of flux increases. Our analysis also showed that direct component of spectral flux is

  8. In situ measurements constraining the role of sulphate aerosols in mid-latitude ozone depletion

    NASA Technical Reports Server (NTRS)

    Fahey, D. W.; Kawa, S. R.; Woodbridge, E. L.; Tin, P.; Wilson, J. C.; Jonsson, H. H.; Dye, J. E.; Baumgardner, D.; Borrmann, S.; Toohey, D. W.

    1993-01-01

    In situ measurements of stratospheric sulphate aerosol, reactive nitrogen and chlorine concentrations at middle latitudes confirm the importance of aerosol surface reactions that convert active nitrogen to a less active, reservoir form. This makes mid-latitude stratospheric ozone less vulnerable to active nitrogen and more vulnerable to chlorine species. The effect of aerosol reactions on active nitrogen depends on gas phase reaction rates, so that increases in aerosol concentration following volcanic eruptions will have only a limited effect on ozone depletion at these latitudes.

  9. Mesospheric aerosol sampling spectrometer

    NASA Astrophysics Data System (ADS)

    Knappmiller, Scott; Robertson, Scott; Sternovsky, Zoltan; Horanyi, Mihaly; Kohnert, Rick

    . The Mesospheric Aerosol Sampling Spectrometer (MASS) instrument has been launched on two sounding rockets in August, 2007 from Andoya, Norway to detect charged sub-visible aerosol particles in the polar mesosphere. The MASS instrument is designed to collect charged aerosols, cluster ions, and electrons on four pairs of graphite electrodes, three of which are biased with increasing voltage. The design of the MASS instrument was complicated by the short mean free path in the mesosphere. The opening to MASS was deliberately built to increase the mean free path and to reduce the shock wave within the instrument. The design procedure began with aerodynamics simulations of the flow through the instrument using Direct Simulation Monte Carlo (DSMC) in 3-D. The electric fields within the instrument were calculated using a Laplace solver in 3-D. With the aerodynamic and electric field simulations completed, an algorithm was created to find the trajectories of charged aerosols including collisions within MASS. Using this algorithm the collection efficiencies for each electrode was calculated as a function of the charge to mass ratio of the incoming particle. The simulation results have been confirmed experimentally using an Argon RF ion beam. The data from the August launches have been analyzed and the initial results show the MASS instrument operated as expected. Additional studies are underway to determine if there were effects from payload charging or spurious charge generation within the instrument. This project is supported by NASA.

  10. Aerosol Analysis via Electrostatic Precipitation-Electrospray Ionization Mass Spectrometry.

    PubMed

    He, Siqin; Li, Lin; Duan, Hongxu; Naqwi, Amir; Hogan, Christopher J

    2015-07-01

    Electrospray ionization (ESI) is the preferred mode of ion generation for mass analysis of many organic species, as alternative ionization techniques can lead to appreciable analyte fragmentation. For this reason, ESI is an ideal method for the analysis of species within aerosol particles. However, because of their low concentrations (∼10 μg/m(3)) in most environments, ESI has been applied sparingly in aerosol particle analysis; aerosol mass spectrometers typically employ analyte volatilization followed by electron ionization or chemical ionization, which can lead to a considerable degree of analyte fragmentation. Here, we describe an approach to apply ESI to submicrometer and nanometer scale aerosol particles, which utilizes unipolar ionization to charge particles, electrostatic precipitation to collect particles on the tip of a Tungsten rod, and subsequently, by flowing liquid over the rod, ESI and mass analysis of the species composing collected particles. This technique, which we term electrostatic precipitation-ESI-MS (EP-ESI-MS), is shown to enable analysis of nanogram quantities of collected particles (from aerosol phase concentrations as low as 10(2) ng m(-3)) composed of cesium iodide, levoglucosan, and levoglucosan within a carbon nanoparticle matrix. With EP-ESI-MS, the integrated mass spectrometric signals are found to be a monotonic function of the mass concentration of analyte in the aerosol phase. We additionally show that EP-ESI-MS has a dynamic range of close to 5 orders of magnitude in mass, making it suitable for molecular analysis of aerosol particles in laboratory settings with upstream particle size classification, as well as analysis of PM 2.5 particles in ambient air. PMID:26024017

  11. Jupiter: Aerosol Chemistry in the Polar Atmosphere.

    PubMed

    Wong; Lee; Yung; Ajello

    2000-05-10

    Aromatic compounds have been considered a likely candidate for enhanced aerosol formation in the polar region of Jupiter. We develop a new chemical model for aromatic compounds in the Jovian auroral thermosphere/ionosphere. The model is based on a previous model for hydrocarbon chemistry in the Jovian atmosphere and is constrained by observations from Voyager, Galileo, and the Infrared Space Observatory. Precipitation of energetic electrons provides the major energy source for the production of benzene and other heavier aromatic hydrocarbons. The maximum mixing ratio of benzene in the polar model is 2x10-9, a value that can be compared with the observed value of 2+2-1x10-9 in the north polar auroral region. Sufficient quantities of the higher ring species are produced so that their saturated vapor pressures are exceeded. Condensation of these molecules is expected to lead to aerosol formation. PMID:10813686

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

    NASA Technical Reports Server (NTRS)

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

    2014-01-01

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

  13. Thermodynamics of water condensation on a primary marine aerosol coated by surfactant organic molecules.

    PubMed

    Djikaev, Yuri S; Ruckenstein, Eli

    2014-10-23

    A large subset of primary marine aerosols can be initially (immediately upon formation) treated using an "inverted micelle" model. We study the thermodynamics of heterogeneous water condensation on such a marine aerosol. Its hydrophobic organic coating can be processed by chemical reactions with atmospheric species; this enables the marine aerosol to serve as a nucleating center for water condensation. The most probable pathway of such "aging" involves atmospheric hydroxyl radicals that abstract hydrogen atoms from organic molecules coating the aerosol (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). Taking these two reactions into account, we derive an expression for the free energy of formation of an aqueous droplet on a marine aerosol. The model is illustrated by numerical calculations. The results suggest that the formation of aqueous droplets on marine aerosols is most likely to occur via Köhler activation rather than via nucleation. The model allows one to determine the threshold parameters necessary for the Köhler activation of such aerosols. Numerical results also corroborate previous suggestions that one can omit some chemical species of aerosols (and other details of their chemical composition) in investigating aerosol effects on climate.

  14. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics

    NASA Astrophysics Data System (ADS)

    Cremer, Johannes W.; Thaler, Klemens M.; Haisch, Christoph; Signorell, Ruth

    2016-03-01

    Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions.

  15. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics.

    PubMed

    Cremer, Johannes W; Thaler, Klemens M; Haisch, Christoph; Signorell, Ruth

    2016-01-01

    Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions. PMID:26979973

  16. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics

    PubMed Central

    Cremer, Johannes W.; Thaler, Klemens M.; Haisch, Christoph; Signorell, Ruth

    2016-01-01

    Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions. PMID:26979973

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

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, P.; Platt, U.; Zetzsch, C.

    2012-01-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS released from simulated natural halogen sources like salt pans. Subsequently the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which result in new functional groups, changed UV/VIS absorption, or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  18. Lagrangian Displacement Ensembles for Aerosol Data Assimilation (Invited)

    NASA Astrophysics Data System (ADS)

    da Silva, A.; Colarco, P. R.; Govindaraju, R. C.

    2010-12-01

    A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely-sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentractions for initializing a prognostic model. This problem is exarcebated in the the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols). An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meterorological fields and realistc emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from innacurate emissions, and the Lagrangian misplacement of plumes induced by errors in the driving meterorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of errors is no longer the main order of business. We will describe and aerosol data assimilation scheme in which the anaysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes explicit sequential bias estimation as in Dee and da Silva (1998). Unlikely existing aerosol data assimiltion schemes we do not obtain analysis increments of the 3D concentrations by scalling the background profiles. Instead, we explore the Langrangian characteristics of the problem for generating local displacement ensembles. These high-resolution, state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity comparable to the forecasting step by the aerosol transport model

  19. Measurements of aerosol chemical composition in boreal forest summer conditions

    NASA Astrophysics Data System (ADS)

    ńijälä, M.; Junninen, H.; Ehn, M.; Petäjä, T.; Vogel, A.; Hoffmann, T.; Corrigan, A.; Russell, L.; Makkonen, U.; Virkkula, A.; Mäntykenttä, J.; Kulmala, M.; Worsnop, D.

    2012-04-01

    Boreal forests are an important biome, covering vast areas of the northern hemisphere and affecting the global climate change via various feedbacks [1]. Despite having relatively few anthropogenic primary aerosol sources, they always contain a non-negligible aerosol population [2]. This study describes aerosol chemical composition measurements using Aerodyne Aerosol Mass Spectrometer (C-ToF AMS, [3]), carried out at a boreal forest area in Hyytiälä, Southern Finland. The site, Helsinki University SMEAR II measurement station [4], is situated at a homogeneous Scots pine (Pinus sylvestris) forest stand. In addition to the station's permanent aerosol, gas phase and meteorological instruments, during the HUMPPA (Hyytiälä United Measurements of Photochemistry and Particles in Air) campaign in July 2010, a very comprehensive set of atmospheric chemistry measurement instrumentation was provided by the Max Planck Institute for chemistry, Johannes Gutenberg-University, University of California and the Finnish Meteorological institute. In this study aerosol chemical composition measurements from the campaign are presented. The dominant aerosol chemical species during the campaign were the organics, although periods with elevated amounts of particulate sulfates were also seen. The overall AMS measured particle mass concentrations varied from near zero to 27 μg/m observed during a forest fire smoke episode. The AMS measured aerosol mass loadings were found to agree well with DMPS derived mass concentrations (r2=0.998). The AMS data was also compared with three other aerosol instruments. The Marga instrument [5] was used to provide a quantitative semi-online measurement of inorganic chemical compounds in particle phase. Fourier Transform Infrared Spectroscopy (FTIR) analysis was performed on daily filter samples, enabling the identification and quantification of organic aerosol subspecies. Finally an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI

  20. Anthropogenic Aerosols and Tropical Precipitation

    NASA Astrophysics Data System (ADS)

    Wang, C.; Kim, D.; Ekman, A. M. L.; Barth, M. C.; Rasch, P. J.

    2009-04-01

    Anthropogenic aerosols can affect the radiative balance of the Earth-atmosphere system and precipitation by acting as cloud condensation nuclei (CCN) or ice nuclei (IN) and thus modifying the optical and microphysical properties as well as lifetimes of clouds. Recent studies have also suggested that the direct radiative effect of anthropogenic aerosols, particularly absorbing aerosols, can perturb the large-scale circulation and cause a significant change in both quantity and distribution of critical tropical precipitation systems ranging from Pacific and Indian to Atlantic Oceans. This effect of aerosols on precipitation often appears in places away from aerosol-concentrated regions and current results suggest that the precipitation changes caused by it could be much more substantial than that by the microphysics-based aerosol effect. To understand the detailed mechanisms and strengths of such a "remote impact" and the climate response/feedback to anthropogenic aerosols in general, an interactive aerosol-climate model has been developed based on the Community Climate System Model (CCSM) of NCAR. Its aerosol module describes size, chemical composition, and mixing states of various sulfate and carbonaceous aerosols. Several model processes are derived based on 3D cloud-resolving model simulations. We have conducted a set of long integrations using the model driven by radiative effects of different combinations of various carbonaceous and sulfate aerosols and their mixtures. The responses of tropical precipitation systems to the forcing of these aerosols are analyzed using both model and observational data. Detailed analyses on the aerosol-precipitation causal relations of two systems: i.e., the Indian summer monsoon and Pacific ITCZ will be specifically presented.

  1. Propagation of global model uncertainties in aerosol forecasting: A field practitioner's opinion

    NASA Astrophysics Data System (ADS)

    Reid, J. S.; Benedetti, A.; Bozzo, A.; Brooks, I. M.; Brooks, M.; Colarco, P. R.; daSilva, A.; Flatau, M. K.; Kuehn, R.; Hansen, J.; Holz, R.; Kaku, K.; Lynch, P.; Remy, S.; Rubin, J. I.; Sekiyama, T. T.; Tanaka, T. Y.; Zhang, J.

    2015-12-01

    While aerosol forecasting has its own host of aerosol source, sink and microphysical challenges to overcome, ultimately any numerical weather prediction based aerosol model can be no better than its underlying meteorology. However, the scorecard elements that drive NWP model development have varying relationships to the key uncertainties and biases that are of greatest concern to aerosol forecasting. Here we provide opinions from member developers of the International Cooperative for Aerosol Prediction (ICAP) on NWP deficiencies related to multi-specie aerosol forecasting, as well as relevance of current NWP scorecard elements to aerosol forecasting. Comparisons to field mission data to simulations are used to demonstrate these opinions and show how shortcomings in individual processes in the global models cascade into aerosol prediction. While a number of sensitivities will be outlined, as one would expect, the most important processes relate to aerosol sources, sinks and, in the context of data assimilation, aerosol hygroscopicity. Thus, the pressing needs in the global models relate to boundary layer and convective processes in the context of large scale waves. Examples will be derived from tropical to polar field measurements, from simpler to more complex including a) network data on dust emissions and transport from Saharan Africa, b) boundary layer development, instability, and deep convection in the United States during Studies of Emissions and Atmospheric, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS); and c) 7 Southeast Asian Studies (7SEAS) data on aerosol influences by maritime convection up-scaled through tropical waves. While the focus of this talk is how improved meteorological model processes are important to aerosol modeling, we conclude with recent findings of the Arctic Summer Cloud Ocean Study (ASCOS) which demonstrate how aerosol processes may be important to global model simulations of polar cloud, surface energy and subsequently

  2. The Dynamics of Aerosols: Recent Developments In Regional and Global Modelling

    NASA Astrophysics Data System (ADS)

    Vignati, E.

    An efficient and accurate representation of aerosol size distributions and microphysi- cal processes is required to make physically consistent calculations of the direct and indirect radiative effects of aerosols and their impact on climate. Various modelling approaches have been developed to simulate the dynamical evolu- tion of natural and anthropogenic aerosol populations. Among the components of the particulate phase, sulphate, sea salt, black carbon, organic carbon and dust all play an important role. However their contributions vary from region to region. Modal models, in which the aerosol size distribution is represented by a number of modes, present a computational attractive approach for aerosol dynamic modelling in regional and global models. They can describe external as well as internal mixtures of aerosol particles and the full aerosol dynamics. The accuracy of modal models is however dependent on both the suitability of the lognormal approximation to the size distribution and the extent to which processes can be expressed in terms of distribution parameters. Simultaneously, recent developments have been made to treat many aerosol species in global models using discrete size bins. The detailed description allows a more ac- curate calculation of the aerosol water content, an important parameter required for calculations of aerosol optical properties. However, such a fine size resolution is usu- ally time consuming when used in large scale models, therefore sometimes not all the processes modifying aerosol properties are included. Modest requirements for storage and computations is one of the advantages of moment methods. These techniques have the capability of simultaneously represent the aerosol dynamic processes and transport in large scale models. An overview of recent developments of aerosol modelling in global and regional mod- els will be presented outlining the advantages and disadvantages of the various tech- niques for such large scales.

  3. Organic Aerosol Component (OACOMP) Value-Added Product

    SciTech Connect

    Fast, J; Zhang, Q; tilp, A; Shippert, T; Parworth, C; Mei, F

    2013-08-23

    Organic aerosol (OA, i.e., the organic fraction of particles) accounts for 10–90% of the fine aerosol mass globally and is a key determinant of aerosol radiative forcing. But atmospheric OA is poorly characterized and its life cycle insufficiently represented in models. As a result, current models are unable to simulate OA concentrations and properties accurately. This deficiency represents a large source of uncertainty in quantification of aerosol effects and prediction of future climate change. Evaluation and development of aerosol models require data products generated from field observations. Real-time, quantitative data acquired with aerosol mass spectrometers (AMS) (Canagaratna et al. 2007) are critical to this need. The AMS determines size-resolved concentrations of non-refractory (NR) species in submicrometer particles (PM1) with fast time resolution suitable for both ground-based and aircraft deployments. The high-resolution AMS (HR-AMS), which is equipped with a high mass resolution time-of-flight mass spectrometer, can be used to determine the elemental composition and oxidation degrees of OA (DeCarlo et al. 2006).

  4. Weekly patterns of aerosol in the United States

    NASA Astrophysics Data System (ADS)

    Murphy, D. M.; Capps, S. L.; Daniel, J. S.; Frost, G. J.; White, W. H.

    2008-05-01

    Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network of aerosol samplers and NOAA monitoring sites are examined for weekly cycles. At remote and rural sites, fine particle elemental carbon, crustal elements, and coarse particle mass had pronounced (up to 20%) weekly cycles with minima on Sunday or Monday. Fine particle organic carbon and mass had smaller amplitude cycles, also with Sunday or Monday minima. There was no statistically significant weekly cycle in fine particle sulfate despite a 5 to 15% weekly cycle in power plant SO2 emissions. Although results for nitrate may be more susceptible to sampling artifacts, nitrate also showed a pronounced weekly cycle with an amplitude similar to elemental carbon. The only species found with a weekend maximum was Pb, probably from general aviation on weekends. Aerosol optical properties at NOAA monitoring sites were consistent with the IMPROVE chemical data, with significant weekly cycles in aerosol light absorption but not light scattering. These results support a large role of diesel emissions in elemental carbon aerosol over the entire United States and suggest that a large fraction of the airborne soil dust is anthropogenic. They also suggest that studies of weekly cycles in temperature, cloudiness, precipitation, or other meteorological variables should look for causes more in light-absorbing particles and possible ice nucleation by dust rather than sulfate or total aerosol. There are also implications for personal exposure and epidemiological studies of aerosol health effects.

  5. Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

    NASA Astrophysics Data System (ADS)

    Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

    2008-12-01

    The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

  6. Three Dimensional Aerosol Climatology over India and the North Indian Ocean

    NASA Astrophysics Data System (ADS)

    Adams, A.; Zhang, C.

    2013-12-01

    Numerical models are indispensable tools to study aerosol effects on climate, including both aerosol direct and indirect radiative effects and their role in precipitation. But, agreement among the models has not been achieved, and thus it is not possible to accurately and confidently attain estimates of aerosol effects on climate. The lack of reliable knowledge on global three-dimensional (3D) aerosol climatology has prevented us from assessing the degree to which the disagreement in their aerosol climatic effects may come from differences of aerosol vertical structures in their simulations. To that end, we created a six year, global 3D extinction coefficient dataset for each aerosol species identifiable by the Level 2, Version 3, 5 km Aerosol Profile product from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) as a tool to improve 3D model representations. Here we describe the 3D structure of aerosol in the Middle East, India, and the Northern Indian Ocean and some of the interesting dynamical features responsible for the vertical structure and external mixing of aerosol species. One interesting feature in the 3D structure during boreal summer is a well-defined EC core located 0 - 10°N, 40°E - 90°E (Somalia across the Indian subcontinent), centered at 3 km. This is controlled by a shallow meridional circulation about the core. Additionally, the Somali Low-Level Jet exists at this location, but is usually located below the core (~850 mb). Another interesting feature is a strong EC core located 0 - 15°N, 60°E - 90°E below 0.5 km. Polluted dust (external mixture of dust and smoke) and marine aerosol are collocated in this area with maximum AODs of ~0.5 and ~0.2 respectively. Due to the wind stress over ocean, collocation of aerosol species, altitude, and lack of transport pathway for polluted dust, it is possible that this is an example of aerosol misclassification by

  7. Graphical aerosol classification method using aerosol relative optical depth

    NASA Astrophysics Data System (ADS)

    Chen, Qi-Xiang; Yuan, Yuan; Shuai, Yong; Tan, He-Ping

    2016-06-01

    A simple graphical method is presented to classify aerosol types based on a combination of aerosol optical thickness (AOT) and aerosol relative optical thickness (AROT). Six aerosol types, including maritime (MA), desert dust (DD), continental (CO), sub-continental (SC), urban industry (UI) and biomass burning (BB), are discriminated in a two dimensional space of AOT440 and AROT1020/440. Numerical calculations are performed using MIE theory based on a multi log-normal particle size distribution, and the AROT ranges for each aerosol type are determined. More than 5 years of daily observations from 8 representative aerosol sites are applied to the method to confirm spatial applicability. Finally, 3 individual cases are analyzed according to their specific aerosol status. The outcomes indicate that the new graphical method coordinates well with regional characteristics and is also able to distinguish aerosol variations in individual situations. This technique demonstrates a novel way to estimate different aerosol types and provide information on radiative forcing calculations and satellite data corrections.

  8. 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

  9. Exposures to acidic aerosols.

    PubMed

    Spengler, J D; Keeler, G J; Koutrakis, P; Ryan, P B; Raizenne, M; Franklin, C A

    1989-02-01

    Ambient monitoring of acid aerosols in four U.S. cities and in a rural region of southern Ontario clearly show distinct periods of strong acidity. Measurements made in Kingston, TN, and Steubenville, OH, resulted in 24-hr H+ ion concentrations exceeding 100 nmole/m3 more than 10 times during summer months. Periods of elevated acidic aerosols occur less frequently in winter months. The H+ determined during episodic conditions in southern Ontario indicates that respiratory tract deposition can exceed the effects level reported in clinical studies. Observed 12-hr H+ concentrations exceeded 550 nmole/m3 (approximately 27 micrograms/m3 H2SO4). The maximum estimated 1-hr concentration exceeded 1500 nmole/m3 for H+ ions. At these concentrations, an active child might receive more than 2000 nmole of H+ ion in 12 hr and in excess of 900 nmole during the hour when H2SO4 exceeded 50 micrograms/m3.

  10. Aerosol Observing System (AOS) Handbook

    SciTech Connect

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  11. Optical Properties of Polymers Relevant to Secondary Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Marrero-Ortiz, W.; Gomez-Hernandez, M. E.; Xu, W.; Guo, S.; Zhang, R.

    2014-12-01

    Atmospheric aerosols play a critical role in climate directly by scattering and absorbing solar radiation and indirectly by modifying the cloud formation. Currently, the direct and indirect effects of aerosols represent the largest uncertainty in climate predictions models. Some aerosols are directly emitted, but the majority are formed in the atmosphere by the oxidation of gaseous precursors. However, the formation of aerosols at the molecular level is not fully characterized. Certain category of secondary organic aerosols (SOA), which represent a significant fraction of the total aerosol burden, can be light-absorbing, also known as brown carbon. However, the overall contribution of SOA to the brown carbon and the related climate forcing is poorly understood. Such incomplete understanding is due in part to the chemical complexity of SOA and the lack of knowledge regarding SOA formation, transformation, and optical properties. Based on previous laboratory experiments, field measurements, and modeling studies, it has been suggested that the polymers and oligomers play an important role in the SOA formation. Atmospheric polymers could be produced by the hydration or heterogeneous reactions of epoxides and small α-dicarbonyls. Their aqueous chemistry products have been shown to give light-absorbing and high molecular weight oligomeric species, which increase the SOA mass production and alter the direct and indirect effect of aerosols. In this paper, the aerosol chemistry of small α-dicarbonyl compounds with amines is investigated and the associated optical properties are measured using spectroscopic techniques. The differences between primary, secondary and tertiary amines with glyoxal and methylglyoxal are evaluated in terms of SOA browning efficiency. Atmospheric implications of our present work for understanding the formation of light-absorbing SOA will be presented, particularly in terms of the product distribution of light-absorbing SOA formed by aqueous phase

  12. Field and Laboratory Studies of Atmospheric Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Coggon, Matthew Mitchell

    This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of

  13. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    ) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in

  14. Biological aerosol trigger

    NASA Astrophysics Data System (ADS)

    DeSha, Michael S.

    1999-01-01

    In recent history, manmade and natural events have shown us the every-present need for systems to monitor the troposphere for contaminates. These contaminants may take either a chemical or biological form, which determines the methods we use to monitor them. Monitoring the troposphere for biological contaminants is of particular interest to my organization. Whether manmade or natural, contaminants of a biological origin share similar constituents; typically the aromatic amino acids tryptophan, phenylalanine, and tyrosine. All of these proteinaceous compounds autofluorescence when exposed to UV radiation and this established the basis of the laser-induced fluorescence technique we use to detect biological contaminants. This technique can be employed in either point or remote detection schemes and is a valuable tool for discriminating proteinaceous form non-proteinaceous aerosols. For this particular presentation I am going to describe a breadboard point sensor we designed and fabricated to detect proteinaceous aerosols. Previous point sensor designs relied on convoluted flow paths to concentrate the aerosols into a solution. Other systems required precise beam alignment to evenly distribute the energy irradiating the detector elements. Our objective was to build a simple system where beam alignment is not critical, and the flow is straight and laminar. The breadboard system was developed over a nine- month period and its performance assessed at a recent test at Dugway Proving Grounds in Utah. In addition, we have performed chamber experiments in an attempt to establish a baseline for the systems. The results of these efforts are presented here.

  15. Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

    NASA Astrophysics Data System (ADS)

    Metcalf, A. R.; Dutcher, C. S.

    2014-12-01

    Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

  16. Atmospheric aerosols: Their Optical Properties and Effects

    NASA Technical Reports Server (NTRS)

    1976-01-01

    Measured properties of atmospheric aerosol particles are presented. These include aerosol size frequency distribution and complex retractive index. The optical properties of aerosols are computed based on the presuppositions of thermodynamic equilibrium and of Mie-theory.

  17. 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

  18. Volcanic aerosols and lunar eclipses.

    PubMed

    Keen, R A

    1983-12-01

    The moon is visible during total lunar eclipses due to sunlight refracted into the earth's shadow by the atmosphere. Stratospheric aerosols can profoundly affect the brightness of the eclipsed moon. Observed brightnesses of 21 lunar eclipses during 1960-1982 are compared with theoretical calculations based on refraction by an aerosol-free atmosphere to yield globally averaged aerosol optical depths. Results indicate the global aerosol loading from the 1982 eruption of El Chichón is similar in magnitude to that from the 1963 Agung eruption.

  19. Volcanic aerosols and lunar eclipses.

    PubMed

    Keen, R A

    1983-12-01

    The moon is visible during total lunar eclipses due to sunlight refracted into the earth's shadow by the atmosphere. Stratospheric aerosols can profoundly affect the brightness of the eclipsed moon. Observed brightnesses of 21 lunar eclipses during 1960-1982 are compared with theoretical calculations based on refraction by an aerosol-free atmosphere to yield globally averaged aerosol optical depths. Results indicate the global aerosol loading from the 1982 eruption of El Chichón is similar in magnitude to that from the 1963 Agung eruption. PMID:17776243

  20. Stratospheric aerosols and climatic change

    NASA Technical Reports Server (NTRS)

    Toon, O. B.; Pollack, J. B.

    1978-01-01

    Stratospht1ic sulfuric acid particles scatter and absorb sunlight and they scatter, absorb and emit terrestrial thermal radiation. These interactions play a role in the earth's radiation balance and therefore affect climate. The stratospheric aerosols are perturbed by volcanic injection of SO2 and ash, by aircraft injection of SO2, by rocket exhaust of Al2O3 and by tropospheric mixing of particles and pollutant SO2 and COS. In order to assess the effects of these perturbations on climate, the effects of the aerosols on the radiation balance must be understood and in order to understand the radiation effects the properties of the aerosols must be known. The discussion covers the aerosols' effect on the radiation balance. It is shown that the aerosol size distribution controls whether the aerosols will tend to warm or cool the earth's surface. Calculations of aerosol properties, including size distribution, for various perturbation sources are carried out on the basis of an aerosol model. Calculations are also presented of the climatic impact of perturbed aerosols due to volcanic eruptions and Space Shuttle flights.

  1. Fine mode aerosol chemistry over a rural atmosphere near the north-east coast of Bay of Bengal in India

    NASA Astrophysics Data System (ADS)

    Adak, Anandamay; Chatterjee, Abhijit; Ghosh, Sanjay; Raha, Sibaji; Roy, Arindam

    2016-07-01

    A study was conducted on the chemical characterization of fine mode aerosol or PM2.5 over a rural atmosphere near the coast of Bay of Bengal in eastern India. Samples were collected and analyzed during March 2013 - February 2014. The concentration of PM2.5 was found span over a wide range from as low as 3 µg m-3 to as high as 180 µg m-3. The average concentration of PM2.5 was 62 µg m-3. Maximum accumulation of fine mode aerosol was observed during winter whereas minimum was observed during monsoon. Water soluble ionic species of fine mode aerosol were characterized over this rural atmosphere. In spite of being situated near the coast of Bay of Bengal, we observed significantly higher concentrations for anthropogenic species like ammonium and sulphate. The concentrations of these two species were much higher than the sea-salt aerosols. Ammonium and sulphate contributed around 30 % to the total fine mode aerosols. Even dust aerosol species like calcium also showed higher concentrations. Chloride to sodium ratio was found to be much less than that in standard sea-water indicating strong interaction between sea-salt and anthropogenic aerosols. Use of fertilizers in various crop fields and human and animal wastes significantly increased ammonium in fine mode aerosols. Dust aerosol species were accumulated in the atmosphere which could be due to transport of finer dust species from nearby metropolis or locally generated. Non-sea-sulphate and nitrate showed significant contributions in fine mode aerosols having both local and transported sources. Source apportionment shows prominent emission sources of anthropogenic aerosols from local anthropogenic activities and transported from nearby Kolkata metropolis as well.

  2. Heterogeneous OH oxidation of organic aerosols

    NASA Astrophysics Data System (ADS)

    Smith, J.; Kroll, J.; Cappa, C.; Che, D.; Ahmed, M.; Leone, S.; Worsnop, D.; Wilson, K.

    2008-12-01

    The hydroxyl radical (OH) is the most important reactive species in both clean and polluted atmospheres, and therefore gas-phase OH chemistry has been extensively studied for decades. Due to this enormous effort the rates and mechanism of OH reactions with gas phase organics are relatively well understood. However, it unclear whether these well established gas-phase chemical mechanisms apply to the more complex heterogeneous reactions of OH radicals with organic aerosols (OA). Although recent studies have begun to examine OH oxidation of OA, numerous outstanding questions still remain regarding both the rate and chemical mechanism of these reactions. Here we present an in depth investigation of the heterogeneous oxidation of organic squalane particles by OH radicals. By combining a photochemical aerosol flow reactor with a high-resolution aerosol mass spectrometer (AMS), with both electron impact and vacuum ultraviolet photoionization, we investigate OH heterogeneous chemistry in unprecedented detail. Employing elemental composition measurements with detailed kinetics we have arrived at a simple oxidation model which accurately accounts for the evolution of squalane and its" oxidation products. In addition, by exploring a large range of OH concentrations we are able to directly measure the role of secondary particle-phase chain chemistry which can significantly accelerate the oxidation of OA in the atmosphere. Based on these measurements we have arrived at an explicit chemical mechanism for heterogeneous OH oxidation of OA which accurately accounts for our observations over a wide range of reaction conditions.

  3. Heterogeneous Uptake of HO2 Radicals onto Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    George, I. J.; Matthews, P. S.; Brooks, B.; Goddard, A.; Whalley, L. K.; Baeza-Romero, M. T.; Heard, D. E.

    2011-12-01

    The hydroxyl (OH) and hydroperoxyl (HO2) radicals, together known as HOx, play a vital role in atmospheric chemistry by controlling the oxidative capacity of the troposphere. The atmospheric lifetime and concentrations of many trace reactive species, such as volatile organic compounds (VOCs), are determined by HOx radical levels. Therefore, the ability to accurately predict atmospheric HOx concentrations from a detailed knowledge of their sources and sinks is a very useful diagnostic tool to assess our current understanding of atmospheric chemistry. Several recent field studies have observed significantly lower concentrations of HO2 radicals than predicted using box models, where HO2 loss onto aerosols was suggested as a possible missing sink [1, 2]. However, the mechanism on HO2 uptake onto aerosols and its impact on ambient HOx levels are currently not well understood. To improve our understanding of this process, we have conducted laboratory experiments to measure HO2 uptake coefficients onto submicron aerosol particles. The FAGE (Fluorescence Assay by Gas Expansion) technique, a highly sensitive laser induced fluorescence based detection method, was used to monitor HO2 uptake kinetics onto aerosol particles in an aerosol flow tube. The application of the FAGE technique allowed for kinetic experiments to be performed under low HO2 concentrations, i.e. [HO2] < 109 molecules cm-3. HO2 radicals were produced by the photolysis of water vapour in the presence of O2 and aerosol particles were produced either by atomizing dilute salt solutions or by homogeneous nucleation. HO2 uptake coefficients (γ) have been measured for single-component solid and aqueous inorganic salt and organic aerosol particles with a wide range of hygroscopicities. HO2 uptake coefficients on solid particles were below the detection limit (γ < 0.001), whereas on aqueous aerosols uptake coefficients were somewhat larger (γ = 0.001 - 0.008). HO2 uptake coefficients were highest on aerosols

  4. The uptake of HO2 radicals to organic aerosols

    NASA Astrophysics Data System (ADS)

    Matthews, Pascale; Krapf, Manuel; Dommen, Josef; George, Ingrid; Whalley, Lisa; Ingham, Trevor; Baeza-Romero, Maria Teresa; Ammann, Markus; Heard, Dwayne

    2014-05-01

    HOx (OH + HO2) radicals are responsible for the majority of the oxidation in the troposphere and control the concentrations of many trace species in the atmosphere. There have been many field studies where the measured HO2 concentrations have been smaller than the concentration predicted by model calculations [1,2]. The difference has often been attributed to HO2 uptake by aerosols. Organics are a major component of aerosols accounting for 10 - 70 % of their mass [3]. However, there have been very few laboratory studies measuring HO2 uptake onto organic aerosols [4]. Uptake coefficients (γ) were measured for a range of aerosols using a Fluorescence Assay By Gas Expansion (FAGE) detector combined with an aerosol flow tube. HO2 was injected into the flow tube using a moveable injector which allowed first order HO2 decays to be measured along the flow tube both with and without aerosols. Laboratory generated aerosols were made using an atomiser or by homogeneous nucleation. Secondary organic aerosols (SOA) were made using the Paul Scherrer Institute smog chamber and also by means of a Potential Aerosol Mass (PAM) chamber. The total aerosol surface area was then measured using a Scanning Mobility Particle Sizer (SMPS). Experiments were carried out on aerosols containing glutaric acid, glyoxal, malonic acid, stearic acid, oleic acid and squalene. The HO2 uptake coefficients for these species were measured in the range of γ < 0.004 to γ = 0.008 ± 0.004. Humic acid was also studied, however, much larger uptake coefficients (γ = 0.007 - 0.09) were measured, probably due to the fact that these aerosols contained elevated levels of transition metal ions. For humic acid the uptake coefficient was highly dependent on humidity and this may be explained by the liquid water content of the aerosols. Measurements were also performed on copper doped aerosols containing different organics. An uptake coefficient of 0.23 ± 0.07 was measured for copper doped ammonium sulphate

  5. Bacterial Communities in Aerosols and Manure Samples from Two Different Dairies in Central and Sonoma Valleys of California

    PubMed Central

    Ravva, Subbarao V.; Sarreal, Chester Z.; Mandrell, Robert E.

    2011-01-01

    Aerosols have been suspected to transport food pathogens and contaminate fruits and vegetables grown in close proximity to concentrated animal feeding operations, but studies are lacking that substantiate such transport. To monitor the potential transport of bacteria originated from fresh or dry manure through aerosols on a dairy, we identified by 16S rRNA sequencing, bacteria in aerosols collected within 2 to 3 meters from dairy cows at two dairies. Gram-positive Firmicutes were predominant in aerosols from a dairy in Sonoma, California, and surrounded by vineyards, in contrast to sequences of Gram-negative Proteobacteria predominant in aerosols from a dairy in Modesto, California, also surrounded by other dairies. Although Firmicutes represented approximately 50% of the 10 most abundant sequences, aerosols from the Sonoma dairy also contained sequences of Bacteriodetes and Actinobacteria, identified previously with animal feces. While none of the top 10 sequences from fresh or dry manure from Modesto dairy were detected in aerosols, two of the sequences from the phylum Bacteriodetes and one from class Clostridia from fresh manure were detected in aerosols from Sonoma. Interestingly, none of the sequences from dry manure were in the top 10 sequences in aerosols from both dairies. The 10 most abundant sequences in aerosols from the Modesto dairy were all from Proteobacteria and nearly half of them were from genus Massilia, which have been isolated previously from immune-compromised people and aerosols. We conclude that the predominant bacteria in aerosols are diverse among locations and that they do not reflect the predominant species of bacteria present in cow feces and/or in close proximity to cows. These results suggest that the aerosol sequences did not originate from manure. Large volumes of aerosols would be required to determine if bacterial sequences from aerosols could be used to track bacteria in manure to crops grown in proximity. PMID:21364996

  6. Evaluation of Present-day Aerosols over China Simulated from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Liao, H.; Chang, W.

    2014-12-01

    High concentrations of aerosols over China lead to strong radiative forcing that is important for both regional and global climate. To understand the representation of aerosols in China in current global climate models, we evaluate extensively the simulated present-day aerosol concentrations and aerosol optical depth (AOD) over China from the 12 models that participated in Atmospheric Chemistry & Climate Model Intercomparison Project (ACCMIP), by using ground-based measurements and satellite remote sensing. Ground-based measurements of aerosol concentrations used in this work include those from the China Meteorological Administration (CMA) Atmosphere Watch Network (CAWNET) and the observed fine-mode aerosol concentrations collected from the literature. The ground-based measurements of AOD in China are taken from the AErosol RObotic NETwork (AERONET), the sites with CIMEL sun photometer operated by Institute of Atmospheric Physics, Chinese Academy of Sciences, and from Chinese Sun Hazemeter Network (CSHNET). We find that the ACCMIP models generally underestimate concentrations of all major aerosol species in China. On an annual mean basis, the multi-model mean concentrations of sulfate, nitrate, ammonium, black carbon, and organic carbon are underestimated by 63%, 73%, 54%, 53%, and 59%, respectively. The multi-model mean AOD values show low biases of 20-40% at studied sites in China. The ACCMIP models can reproduce seasonal variation of nitrate but cannot capture well the seasonal variations of other aerosol species. Our analyses indicate that current global models generally underestimate the role of aerosols in China in climate simulations.

  7. Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

    NASA Technical Reports Server (NTRS)

    da Silva, Arlindo

    2010-01-01

    A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

  8. 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

  9. Fast Airborne Size Distribution Measurements of an Aerosol Processes and Aging

    NASA Astrophysics Data System (ADS)

    Kapustin, V.; Clarke, A. D.; Zhou, J.; Brekhovskikh, V.; McNaughton, C. S.; Howell, S.

    2009-12-01

    During MILAGRO/INTEX experiment the Hawaii Group for Environmental Aerosol Research (HIGEAR) deployed a wide range of aerosol instrumentation aboard NSF C-130 and NASA DC-8. These were designed to provide rapid information on aerosol composition, state of mixing (internal or external), spectral optical properties (scattering and absorption), the humidity dependence of light scattering - f(RH), and the role of condensed species in changing the absorption properties of black carbon (BC) and inferred properties of organic carbon (OC). We also flew the Fast Mobility Particle Spectrometer (FMPS, TSI Inc.) to measure aerosol size distributions in a range 5.6 - 560 nm. For all our flights around Mexico City, an aerosol number concentration usually was well above the nominal FMPS sensitivity (from ~100 particles/cc @ Dp = 5.6 nm to 1 part/cc @ 560nm), providing us with reliable size distributions even at 1 sec resolution. FMPS measurements revealed small scale structure of an aerosol and allowed us to examine size distributions varying over space and time associated with mixing processes previously unresolved. These 1-Hz measurements during aircraft profiles captured variations in size distributions within shallow layers. Other dynamic processes observed included orography induced aerosol layers and evolution of the nanoparticles formed by nucleation. We put FMPS high resolution size distribution data in a context of aerosol evolution and aging, using a range of established (for MIRAGE/INTEX) chemical, aerosol and transport aging parameters.

  10. Evaluation of synergized pyrethrin aerosol for control of Tribolium castaneum and Tribolium confusum (Coleoptera: Tenebrionidae).

    PubMed

    Kharel, Kabita; Arthur, Frank H; Zhu, Kun Yan; Campbell, James F; Subramanyam, Bhadriraju

    2014-02-01

    Aerosol insecticides are being used in flour mill pest management programs, but there is limited information on their efficacy on different insect life stages. In this study, we evaluated the efficacy of synergized pyrethrin applied as an aerosol against eggs, larvae, pupae, and adults of the red flour beetle, Tribolium castaneum (Herbst), and the confused flour beetle, Tribolium confusum Jacquelin du Val. Effects of direct and indirect exposure were evaluated by exposing each life stage to the aerosol and then transferring to untreated flour, transferring untreated insects to treated flour, or exposing both the insects and the flour to the aerosol. The aerosol produced >88% mortality of both species and all life stages when insects were directly treated and transferred to either treated or untreated flour. Mortality was significantly reduced when insects were either treated together with flour or untreated insects were transferred to treated flour (indirect exposure to the aerosol). Larvae and adults of both species were more tolerant compared with eggs and pupae. Recovery of moribund adults in the indirect exposure treatments was greater compared with recovery of moribund insects in the direct exposure treatments. Good sanitation before aerosol application could facilitate direct exposure of insects and thus increase aerosol efficacy inside flour mills.

  11. Release of Free DNA by Membrane-Impaired Bacterial Aerosols Due to Aerosolization and Air Sampling

    PubMed Central

    Zhen, Huajun; Han, Taewon; Fennell, Donna E.

    2013-01-01

    We report here that stress experienced by bacteria due to aerosolization and air sampling can result in severe membrane impairment, leading to the release of DNA as free molecules. Escherichia coli and Bacillus atrophaeus bacteria were aerosolized and then either collected directly into liquid or collected using other collection media and then transferred into liquid. The amount of DNA released was quantified as the cell membrane damage index (ID), i.e., the number of 16S rRNA gene copies in the supernatant liquid relative to the total number in the bioaerosol sample. During aerosolization by a Collison nebulizer, the ID of E. coli and B. atrophaeus in the nebulizer suspension gradually increased during 60 min of continuous aerosolization. We found that the ID of bacteria during aerosolization was statistically significantly affected by the material of the Collison jar (glass > polycarbonate; P < 0.001) and by the bacterial species (E. coli > B. atrophaeus; P < 0.001). When E. coli was collected for 5 min by filtration, impaction, and impingement, its ID values were within the following ranges: 0.051 to 0.085, 0.16 to 0.37, and 0.068 to 0.23, respectively; when it was collected by electrostatic precipitation, the ID values (0.011 to 0.034) were significantly lower (P < 0.05) than those with other sampling methods. Air samples collected inside an equine facility for 2 h by filtration and impingement exhibited ID values in the range of 0.30 to 0.54. The data indicate that the amount of cell damage during bioaerosol sampling and the resulting release of DNA can be substantial and that this should be taken into account when analyzing bioaerosol samples. PMID:24096426

  12. Clouds, aerosols, and photochemistry in the Jovian atmosphere

    NASA Technical Reports Server (NTRS)

    West, R. A.; Strobel, D. F.; Tomasko, M. G.

    1986-01-01

    An assessment is made of the development status of concepts for cloud and aerosol compositions, vertical and horizontal distributions, and microphysical properties, in the Jovian upper troposphere and stratosphere. Attention is given to several key photochemical species' relationships to aerosol formation as well as their transport process implications, treating photochemistry in the context of comparative planetology and noting differences and similarities among the outer planet atmospheres; since this approach emphasizes observational data, a variegated assortment of ground-based and spacecraft observations is assembled. Current views on the tropospheric distribution of clouds are challenged, and a rationale is presented for alternative accounts.

  13. Cassini/CIRS capabilities for aerosol, cloud, and surface measurements

    NASA Technical Reports Server (NTRS)

    Samuelson, Robert E.

    1992-01-01

    Information that should be revealed by the Cassini Composite Infrared Spectrometer (CIRS) about the aerosol, cloud, and surface properties of Titan are addressed. Limb sounding data will be used to determine aerosol abundances, scale heights, and gradients between 80 and 400 km for various latitudes. Stratospheric condensate cloud top altitudes and column abundances will be inferred as functions of latitude. A search for new species will be conducted. Thermal maps between 500 and 550/cm will be used to investigate tropospheric methane clouds and surface topography; time resolution provided by different orbits will be used to distinguish the two.

  14. Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes During Boreal Spring and Summer

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.; Kim, M. K.; Kim, K. M.; Chin, Mian

    2005-01-01

    Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

  15. Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.; Kim, M. K.; Chin, Mian; Kim, K. M.

    2005-01-01

    Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

  16. Processes influencing secondary aerosol formation in the San Joaquin Valley during winter

    SciTech Connect

    Frederick W. Lurmann; Steven G. Brown; Michael C. McCarthy; Paul T. Roberts

    2006-12-15

    Air quality data collected in the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM2.5) mass concentrations in California ({le} 188 {mu}g/m{sup 3} 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NOx)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NOx and volatile organic compound (VOC) emissions plus background O{sub 3} levels are expected to determine NOx oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter. 59 refs., 11 figs., 1 tab.

  17. CCN Study at Urban Supersite (T0) During MILAGRO: the Essential Information for Prediction of Aerosol CCN Concentrations

    NASA Astrophysics Data System (ADS)

    Wang, J.; Cubison, M.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2009-12-01

    The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols often consist of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban supersite in Mexico City during MILAGRO are analyzed and the degree of closure is evaluated. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The uncertainties associated with these simplifications are compared for different supersaturations and the variation of the uncertainties is examined as a function of aerosol age. The results show that the simplification of internally mixed

  18. Assessing the Performance of Computationally Simple and Complex Representations of Aerosol Processes using a Testbed Methodology

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Ma, P.; Easter, R. C.; Liu, X.; Zaveri, R. A.; Rasch, P.

    2012-12-01

    Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento California during June 2010, and the California Nexus (CalNex) campaign conducted in southern California during May and June of 2010. For the aerosol size distribution, we compare the predictions from the GOCART bulk aerosol model, the MADE/SORGAM modal aerosol model, the Modal Aerosol Model (MAM) employed by CAM5, and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) which uses a sectional representation. For secondary organic aerosols, we compare simple fixed mass yield approaches with the numerically complex volatility basis set approach. All simulations employ the same emissions, meteorology, trace gas chemistry (except for that involving condensable organic species), and initial and boundary conditions. Performance metrics from the AMT are used to assess performance in terms of simulated mass, composition, size distribution (except for GOCART), and aerosol optical properties in relation to computational expense. In addition to statistical measures, qualitative differences among the different aerosol models over the computational domain are presented to examine variations in how aerosols age among the aerosol models.

  19. INDOOR AEROSOLS AND EXPOSURE ASSESSMENT

    EPA Science Inventory

    This chapter provides an overview of both indoor aerosol concentration measurements, and the considerations for assessment of exposure to aerosols in non-occupational settings. The fixed-location measurements of concentration at an outdoor location, while commuting inside an a...

  20. Mount Saint Helens aerosol evolution

    NASA Technical Reports Server (NTRS)

    Oberbeck, V. R.; Farlow, N. H.; Snetsinger, K. G.; Ferry, G. V.; Fong, W.; Hayes, D. M.

    1982-01-01

    Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mt. St. Helens. Analysis of samples shows that aerosol volume increased for 6 months due to gas-to-particle conversion and then decreased to background levels in the following 6 months.

  1. Aerosol Remote Sensing

    NASA Technical Reports Server (NTRS)

    Lenoble, Jacqueline (Editor); Remer, Lorraine (Editor); Tanre, Didier (Editor)

    2012-01-01

    This book gives a much needed explanation of the basic physical principles of radia5tive transfer and remote sensing, and presents all the instruments and retrieval algorithms in a homogenous manner. For the first time, an easy path from theory to practical algorithms is available in one easily accessible volume, making the connection between theoretical radiative transfer and individual practical solutions to retrieve aerosol information from remote sensing. In addition, the specifics and intercomparison of all current and historical methods are explained and clarified.

  2. Thermophoretically Dominated Aerosol Coagulation

    NASA Astrophysics Data System (ADS)

    Rosner, Daniel E.; Arias-Zugasti, Manuel

    2011-01-01

    A theory of aerosol coagulation due to size-dependent thermophoresis is presented. This previously overlooked effect is important when local temperature gradients are large, the sol population is composed of particles of much greater thermal conductivity than the carrier gas, with mean diameters much greater than the prevailing gas mean free path, and an adequate “spread” in sizes (as in metallurgical mists or fumes). We illustrate this via a population-balance analysis of the evolution of an initially log-normal distribution when this mechanism dominates ordinary Brownian diffusion.

  3. Assessment of the aerosol distribution over Indian subcontinent in CMIP5 models

    NASA Astrophysics Data System (ADS)

    Sanap, S. D.; Ayantika, D. C.; Pandithurai, G.; Niranjan, K.

    2014-04-01

    This paper examines the aerosol distribution over Indian subcontinent as represented in 21 models from Coupled Model Inter-comparison Project Phase 5 (CMIP5) simulations, wherein model simulated aerosol optical depth (AOD) is compared with Moderate Resolution Imaging Spectro-radiometer (MODIS) satellite observations. The objective of the study is to provide an assessment of the capability of various global models, participating in CMIP5 project, in capturing the realistic spatial and temporal distribution of aerosol species over the Indian subcontinent. Results from our analysis show that majority of the CMIP5 models (excepting HADGEM2-ES, HADGEM2-CC) seriously underestimates the spatio-temporal variability of aerosol species over the Indian subcontinent, in particular over Indo-Gangetic Plains (IGP). Since IGP region is dominated by anthropogenic activities, high population density, and wind driven transport of dust and other aerosol species, MODIS observations reveal high AOD values over this region. Though the representation of black carbon (BC) loading in many models is fairly good, the dust loading is observed to be significantly low in majority of the models. The presence of pronounced dust activity over northern India and dust being one of the major constituent of aerosol species, the biases in dust loading has a great impact on the AOD of that region. We found that considerable biases in simulating the 850 hPa wind field (which plays important role in transport of dust from adjacent deserts) would be the possible reason for poor representation of dust AOD and in turn total AOD over Indian region in CMIP5 models. In addition, aerosol radiative forcing (ARF) underestimated/overestimated in most of the models. However, spatial distribution of ARF in multi-model ensemble mean is comparable reasonably well with observations with bias in magnitudes. This analysis emphasizes the fundamental need to improve the representation of aerosol species in current state of

  4. 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

  5. The Indian ocean experiment: aerosol forcing obtained from satellite data

    NASA Astrophysics Data System (ADS)

    Rajeev, K.; Ramanathan, V.

    The tropical Indian Ocean provides an ideal and unique natural laboratory to observe and understand the role of anthropogenic aerosols in climate forcing. Since 1996, an international team of American, European and Indian scientists have been collecting aerosol, chemical and radiation data from ships and surface stations, which culminated in a multi-platform field experiment conducted during January to March of 1999. A persistent haze layer that spread over most of the northern Indian Ocean during wintertime was discovered. The layer, a complex mix of organics, black carbon, sulfates, nitrates and other species, subjects the lower atmosphere to a strong radiative heating and a larger reduction in the solar heating of the ocean. We present here the regional distribution of aerosols and the resulting clear sky aerosol radiative forcing at top-of-atmosphere (TOA) observed over the Indian Ocean during the winter months of 1997, 1998 and 1999 based on the aerosol optical depth (AOD) estimated using NOAA14-AVHRR and the TOA radiation budget data from CERES on board TRMM. Using the ratio of surface to TOA clear sky aerosol radiative forcing observed during the same period over the Indian Ocean island of Kaashidhoo (Satheesh and Ramanathan, 2000), the clear sky aerosol radiative forcing at the surface and the atmosphere are discussed. The regional maps of AVHRR derived AOD show abnormally large aerosol concentration during the winter of 1999 which is about 1.5 to 2 times larger than the AOD during the corresponding period of 1997 and 1998. A large latitudinal gradient in AOD is observed during all the three years of observation, with maximum AOD in the northern hemisphere. The diurnal mean clear sky aerosol forcing at TOA in the northern hemisphere Indian Ocean is in the range of -4 to -16 Wm -2 and had large spatio-temporal variations while in the southern hemisphere Indian Ocean it is in the range of 0 to -6Wm -2. The importance of integrating in-situ data with satellite

  6. Aerosol Phage Therapy Efficacy in Burkholderia cepacia Complex Respiratory Infections

    PubMed Central

    Semler, Diana D.; Goudie, Amanda D.; Finlay, Warren H.

    2014-01-01

    Phage therapy has been suggested as a potential treatment for highly antibiotic-resistant bacteria, such as the species of the Burkholderia cepacia complex (BCC). To address this hypothesis, experimental B. cenocepacia respiratory infections were established in mice using a nebulizer and a nose-only inhalation device. Following infection, the mice were treated with one of five B. cenocepacia-specific phages delivered as either an aerosol or intraperitoneal injection. The bacterial and phage titers within the lungs were assayed 2 days after treatment, and mice that received the aerosolized phage therapy demonstrated significant decreases in bacterial loads. Differences in phage activity were observed in vivo. Mice that received phage treatment by intraperitoneal injection did not demonstrate significantly reduced bacterial loads, although phage particles were isolated from their lung tissue. Based on these data, aerosol phage therapy appears to be an effective method for treating highly antibiotic-resistant bacterial respiratory infections, including those caused by BCC bacteria. PMID:24798268

  7. Speciation of Fe in ambient aerosol and cloudwater

    SciTech Connect

    Siefert, L.

    1996-08-15

    Atmospheric iron (Fe) is thought to play an important role in cloudwater chemistry (e.g., S(IV) oxidation, oxidant production, etc.), and is also an important source of Fe to certain regions of the worlds oceans where Fe is believed to be a rate-limiting nutrient for primary productivity. This thesis focuses on understanding the chemistry, speciation and abundance of Fe in cloudwater and aerosol in the troposphere, through observations of Fe speciation in the cloudwater and aerosol samples collected over the continental United States and the Arabian Sea. Different chemical species of atmospheric Fe were measured in aerosol and cloudwater samples to help assess the role of Fe in cloudwater chemistry.

  8. Connecting Water Quality With Air Quality Through Microbial Aerosols

    NASA Astrophysics Data System (ADS)

    Dueker, M. Elias

    Aerosol production from surface waters results in the transfer of aquatic materials (including nutrients and bacteria) to air. These materials can then be transported by onshore winds to land, representing a biogeochemical connection between aquatic and terrestrial systems not normally considered. In urban waterfront environments, this transfer could result in emissions of pathogenic bacteria from contaminated waters. Despite the potential importance of this link, sources, near-shore deposition, identity and viability of microbial aerosols are largely uncharacterized. This dissertation focuses on the environmental and biological mechanisms that define this water-air connection, as a means to build our understanding of the biogeochemical, biogeographical, and public health implications of the transfer of surface water materials to the near-shore environment in both urban and non-urban environments. The effects of tidal height, wind speed and fog on coastal aerosols and microbial content were first quantified on a non-urban coast of Maine, USA. Culture-based, culture-independent, and molecular methods were used to simultaneously sample microbial aerosols while monitoring meteorological parameters. Aerosols at this site displayed clear marine influence and high concentrations of ecologically-relevant nutrients. Coarse aerosol concentrations significantly increased with tidal height, onshore wind speed, and fog presence. Tidal height and fog presence did not significantly influence total microbial aerosol concentrations, but did have a significant effect on culturable microbial aerosol fallout. Molecular analyses of the microbes settling out of near-shore aerosols provided further evidence of local ocean to terrestrial transport of microbes. Aerosol and surface ocean bacterial communities shared species and in general were dominated by organisms previously sampled in marine environments. Fog presence strengthened the microbial connection between water and land through

  9. A TEST OF THERMODYNAMIC EQUILIBRIUM MODELS AND 3-D AIR QUALITY MODELS FOR PREDICTIONS OF AEROSOL NO3-

    EPA Science Inventory

    The inorganic species of sulfate, nitrate and ammonium constitute a major fraction of atmospheric aerosols. The behavior of nitrate is one of the most intriguing aspects of inorganic atmospheric aerosols because particulate nitrate concentrations depend not only on the amount of ...

  10. Mexico City aerosol study

    SciTech Connect

    Falcon, Y.I. ); Ramirez, C.R. )

    1988-01-01

    Mexico City is located in a valley at high elevation (2,268 m) and is subject to atmospheric inversion related problems similar to those found in Denver, Colorado. In addition, Mexico City has a tropical climate (latitude 19{degrees} 25 minutes N), and therefore has more sunlight available for production of photochemical smog. There are approximately 9.5 million people spread in a 1,500 km{sup 2} (25 sq. mi) urban area, and more than two million automobiles (D.G.P.T. 1979) which use leaded gasoline. Furthermore, Mexico City is the principal industrial center in the country with more than 131,000 industries. The growth of the city has led to a serious air pollution problem, and there is concern over the possible pollutant effects on human health. The authors discuss work done to characterize the chemical composition of the aerosol. It is shown that many of the organic compounds which have been detected in urban aerosols are carcinogens.

  11. How Important Is Organic Aerosol Hygroscopicity to Aerosol Indirect Forcing?

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation and yield of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR Community Atmospheric Model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (“κ” value) of POA and SOA. Our model simulation indicates that in the present-day condition changing “κ” value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S=0.1% by 40-60% over the POA source regions, while changing “κ” value of SOA by ±50% (from 0.14 to 0.07 and 0.21) changes the CCN within 30%. Changes in the in-cloud droplet number concentrations (CDNC) are within 20% in most locations on the globe with the above changes in “κ” value of POA and SOA. Global annual mean anthropogenic aerosol indirect forcing (AIF) between present-day (PD) and pre-industrial (PI) conditions change by 0.4 W m-2 with the control run of -1.3 W m-2. AIF reduces with the increase hygroscopicity of organic aerosol, indicating the important role of natural organic aerosol in buffering the relative change of CDNC from PI to PD.

  12. PMSE dependence on aerosol charge number density and aerosol size

    NASA Astrophysics Data System (ADS)

    Rapp, Markus; Lübken, Franz-Josef; Hoffmann, Peter; Latteck, Ralph; Baumgarten, Gerd; Blix, Tom A.

    2003-04-01

    It is commonly accepted that the existence of polar mesosphere summer echoes (PMSEs) depends on the presence of charged aerosols since these are comparatively heavy and reduce the diffusion of free electrons due to ambipolar forces. Simple microphysical modeling suggests that this diffusivity reduction is proportional to rA2 (rA = aerosol radius) but only if a significant amount of charges is bound on the aerosols such that NA∣ZA∣/ne > 1.2 (NA = number of aerosols, ZA = aerosol charge, ne = number of free electrons). The fact that the background electron profile frequently shows large depletions ("biteouts") at PMSE altitudes is taken as a support for this idea since within biteouts a major fraction of free electrons is missing, i.e., bound on aerosols. In this paper, we show from in situ measurements of electron densities and from radar and lidar observations that PMSEs can also exist in regions where only a minor fraction of free electrons is bound on aerosols, i.e., with no biteout and with NA∣ZA∣/ne ≪ 1. We show strong experimental evidence that it is instead the product NA∣ZA∣rA2 that is crucial for the existence of PMSEs. For example, small aerosol charge can be compensated by large aerosol radius. We show that this product replicates the main features of PMSEs, in particular the mean altitude distribution and the altitude of PMSEs in the presence of noctilucent clouds (NLCs). We therefore take this product as a "proxy" for PMSE. The agreement between this proxy and the main characteristics of PMSEs implies that simple microphysical models do not satisfactorily describe PMSE physics and need to be improved. The proxy can easily be used in models of the upper atmosphere to better understand seasonal and geographical variations of PMSEs, for example, the long debated difference between Northern and Southern hemisphere PMSEs.

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

    NASA Astrophysics Data System (ADS)

    Hock, N.; Schneider, J.; Borrmann, S.; Römpp, A.; Moortgat, G.; Franze, T.; Schauer, C.; Pöschl, U.; Plass-Dülmer, C.; Berresheim, H.

    2007-06-01

    particles. The average ratio of OM1 to OC2.5 was 2, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA) over hydrocarbon-like organic aerosol (HOA) inferred from the AMS results (4:1), and also with the high abundance of proteins (~3%) indicating a high proportion of primary biological material (~30%) in PM2.5. Moreover, the low abundance of PAHs (<1 ng m-3) and EC (<1 μg m-3) in PM2.5 confirm a low contribution of combustion emissions, which are usually also major sources for HOA. Slightly enhanced HOA concentrations indicating fresh anthropogenic emissions were observed during a period when air masses were advected from the densely populated Po Valley, Italy. Detection of several secondary organic aerosol compounds (dicarboxylic acids) and their precursors (monoterpenes) confirmed the finding that secondary aerosol from natural sources was an important aerosol constituent. A sharp decrease of the short lived monoterpenes indicated that during night-time the measurement station was isolated from ground emission sources by a stable inversion layer. Nighttime values can therefore be regarded to represent regional or long range transport. New particle formation was observed almost every day with particle number concentrations exceeding 104 cm-3 (nighttime background level 1000-2000 cm-3). Closer inspection of two major events indicated that ternary H2SO4/H2O/NH3 nucleation triggered particle formation and that condensation of both organic and inorganic species contributed to particle growth.

  14. Characterizing the formation of secondary organic aerosols

    SciTech Connect

    Lunden, Melissa; Black, Douglas; Brown, Nancy

    2004-02-01

    Organic aerosol is an important fraction of the fine particulate matter present in the atmosphere. This organic aerosol comes from a variety of sources; primary organic aerosol emitted directly from combustion process, and secondary aerosol formed in the atmosphere from condensable vapors. This secondary organic aerosol (SOA) can result from both anthropogenic and biogenic sources. In rural areas of the United States, organic aerosols can be a significant part of the aerosol load in the atmosphere. However, the extent to which gas-phase biogenic emissions contribute to this organic load is poorly understood. Such an understanding is crucial to properly apportion the effect of anthropogenic emissions in these rural areas that are sometimes dominated by biogenic sources. To help gain insight on the effect of biogenic emissions on particle concentrations in rural areas, we have been conducting a field measurement program at the University of California Blodgett Forest Research Facility. The field location includes has been used to acquire an extensive suite of measurements resulting in a rich data set, containing a combination of aerosol, organic, and nitrogenous species concentration and meteorological data with a long time record. The field location was established in 1997 by Allen Goldstein, a professor in the Department of Environmental Science, Policy and Management at the University of California at Berkeley to study interactions between the biosphere and the atmosphere. The Goldstein group focuses on measurements of concentrations and whole ecosystem biosphere-atmosphere fluxes for volatile organic compounds (VOC's), oxygenated volatile organic compounds (OVOC's), ozone, carbon dioxide, water vapor, and energy. Another important collaborator at the Blodgett field location is Ronald Cohen, a professor in the Chemistry Department at the University of California at Berkeley. At the Blodgett field location, his group his group performs measurements of the

  15. International Cooperative for Aerosol Prediction Workshop on Aerosol Forecast Verification

    NASA Technical Reports Server (NTRS)

    Benedetti, Angela; Reid, Jeffrey S.; Colarco, Peter R.

    2011-01-01

    The purpose of this workshop was to reinforce the working partnership between centers who are actively involved in global aerosol forecasting, and to discuss issues related to forecast verification. Participants included representatives from operational centers with global aerosol forecasting requirements, a panel of experts on Numerical Weather Prediction and Air Quality forecast verification, data providers, and several observers from the research community. The presentations centered on a review of current NWP and AQ practices with subsequent discussion focused on the challenges in defining appropriate verification measures for the next generation of aerosol forecast systems.

  16. SAGE II aerosol data validation based on retrieved aerosol model size distribution from SAGE II aerosol measurements

    NASA Technical Reports Server (NTRS)

    Wang, Pi-Huan; Mccormick, M. P.; Mcmaster, L. R.; Chu, W. P.; Swissler, T. J.; Osborn, M. T.; Russell, P. B.; Oberbeck, V. R.; Livingston, J.; Rosen, J. M.

    1989-01-01

    Consideration is given to aerosol correlative measurements experiments for the Stratospheric Aerosol and Gas Experiment (SAGE) II, conducted between November 1984 and July 1986. The correlative measurements were taken with an impactor/laser probe, a dustsonde, and an airborne 36-cm lidar system. The primary aerosol quantities measured by the ground-based instruments are compared with those calculated from the aerosol size distributions from SAGE II aerosol extinction measurements. Good agreement is found between the two sets of measurements.

  17. Characterization of aerosols containing Legionella generated upon nebulization

    NASA Astrophysics Data System (ADS)

    Allegra, Séverine; Leclerc, Lara; Massard, Pierre André; Girardot, Françoise; Riffard, Serge; Pourchez, Jérémie

    2016-09-01

    Legionella pneumophila is, by far, the species most frequently associated with Legionnaires’ disease (LD). Human infection occurs almost exclusively by aerosol inhalation which places the bacteria in juxtaposition with alveolar macrophages. LD risk management is based on controlling water quality by applying standardized procedures. However, to gain a better understanding of the real risk of exposure, there is a need (i) to investigate under which conditions Legionella may be aerosolized and (ii) to quantify bacterial deposition into the respiratory tract upon nebulization. In this study, we used an original experimental set-up that enables the generation of aerosol particles containing L. pneumophila under various conditions. Using flow cytometry in combination with qPCR and culture, we determined (i) the size of the aerosols and (ii) the concentration of viable Legionella forms that may reach the thoracic region. We determined that the 0.26–2.5 μm aerosol size range represents 7% of initial bacterial suspension. Among the viable forms, 0.7% of initial viable bacterial suspension may reach the pulmonary alveoli. In conclusion, these deposition profiles can be used to standardize the size of inoculum injected in any type of respiratory tract model to obtain new insights into the dose response for LD.

  18. 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.

  19. Characterization of aerosols containing Legionella generated upon nebulization

    PubMed Central

    Allegra, Séverine; Leclerc, Lara; Massard, Pierre André; Girardot, Françoise; Riffard, Serge; Pourchez, Jérémie

    2016-01-01

    Legionella pneumophila is, by far, the species most frequently associated with Legionnaires’ disease (LD). Human infection occurs almost exclusively by aerosol inhalation which places the bacteria in juxtaposition with alveolar macrophages. LD risk management is based on controlling water quality by applying standardized procedures. However, to gain a better understanding of the real risk of exposure, there is a need (i) to investigate under which conditions Legionella may be aerosolized and (ii) to quantify bacterial deposition into the respiratory tract upon nebulization. In this study, we used an original experimental set-up that enables the generation of aerosol particles containing L. pneumophila under various conditions. Using flow cytometry in combination with qPCR and culture, we determined (i) the size of the aerosols and (ii) the concentration of viable Legionella forms that may reach the thoracic region. We determined that the 0.26–2.5 μm aerosol size range represents 7% of initial bacterial suspension. Among the viable forms, 0.7% of initial viable bacterial suspension may reach the pulmonary alveoli. In conclusion, these deposition profiles can be used to standardize the size of inoculum injected in any type of respiratory tract model to obtain new insights into the dose response for LD. PMID:27671446

  20. Secondary Aerosol: Precursors and Formation Mechanisms. Technical Report on Grant

    SciTech Connect

    Weinstein-Lloyd, Judith B

    2009-05-04

    This project focused on studying trace gases that participate in chemical reactions that form atmospheric aerosols. Ammonium sulfate is a major constituent of these tiny particles, and one important pathway to sulfate formation is oxidation of dissolved sulfur dioxide by hydrogen peroxide in cloud, fog and rainwater. Sulfate aerosols influence the number and size of cloud droplets, and since these factors determine cloud radiative properties, sulfate aerosols also influence climate. Peroxide measurements, in conjunction with those of other gaseous species, can used to distinguish the contribution of in-cloud reaction to new sulfate aerosol formation from gas-phase nucleation reactions. This will lead to more reliable global climate models. We constructed and tested a new 4-channel fluorescence detector for airborne detection of peroxides. We integrated the instrument on the G-1 in January, 2006 and took a test flight in anticipation of the MAX-Mex field program, where we planned to fly under pressurized conditions for the first time. We participated in the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) - Megacity Aerosol EXperiment Mexico City (MAX-Mex) field measurement campaign. Peroxide instrumentation was deployed on the DOE G-1 research aircraft based in Veracruz, and at the surface site at Tecamac University.

  1. Formation of nitrogenated organic aerosols in the Titan upper atmosphere

    PubMed Central

    Imanaka, Hiroshi; Smith, Mark A.

    2010-01-01

    Many aspects of the nitrogen fixation process by photochemistry in the Titan atmosphere are not fully understood. The recent Cassini mission revealed organic aerosol formation in the upper atmosphere of Titan. It is not clear, however, how much and by what mechanism nitrogen is incorporated in Titan’s organic aerosols. Using tunable synchrotron radiation at the Advanced Light Source, we demonstrate the first evidence of nitrogenated organic aerosol production by extreme ultraviolet–vacuum ultraviolet irradiation of a N2/CH4 gas mixture. The ultrahigh-mass-resolution study with laser desorption ionization-Fourier transform-ion cyclotron resonance mass spectrometry of N2/CH4 photolytic solid products at 60 and 82.5 nm indicates the predominance of highly nitrogenated compounds. The distinct nitrogen incorporations at the elemental abundances of H2C2N and HCN, respectively, are suggestive of important roles of H2C2N/HCCN and HCN/CN in their formation. The efficient formation of unsaturated hydrocarbons is observed in the gas phase without abundant nitrogenated neutrals at 60 nm, and this is confirmed by separately using 13C and 15N isotopically labeled initial gas mixtures. These observations strongly suggest a heterogeneous incorporation mechanism via short lived nitrogenated reactive species, such as HCCN radical, for nitrogenated organic aerosol formation, and imply that substantial amounts of nitrogen is fixed as organic macromolecular aerosols in Titan’s atmosphere. PMID:20616074

  2. "APEC Blue": Secondary Aerosol Reductions from Emission Controls in Beijing.

    PubMed

    Sun, Yele; Wang, Zifa; Wild, Oliver; Xu, Weiqi; Chen, Chen; Fu, Pingqing; Du, Wei; Zhou, Libo; Zhang, Qi; Han, Tingting; Wang, Qingqing; Pan, Xiaole; Zheng, Haitao; Li, Jie; Guo, Xiaofeng; Liu, Jianguo; Worsnop, Douglas R

    2016-01-01

    China implemented strict emission control measures in Beijing and surrounding regions to ensure good air quality during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. We conducted synchronous aerosol particle measurements with two aerosol mass spectrometers at different heights on a meteorological tower in urban Beijing to investigate the variations in particulate composition, sources and size distributions in response to emission controls. Our results show consistently large reductions in secondary inorganic aerosol (SIA) of 61-67% and 51-57%, and in secondary organic aerosol (SOA) of 55% and 37%, at 260 m and ground level, respectively, during the APEC summit. These changes were mainly caused by large reductions in accumulation mode particles and by suppression of the growth of SIA and SOA by a factor of 2-3, which led to blue sky days during APEC commonly referred to as "APEC Blue". We propose a conceptual framework for the evolution of primary and secondary species and highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing. Our results indicate that reducing the precursors of secondary aerosol over regional scales is crucial and effective in suppressing the formation of secondary particulates and mitigating PM pollution. PMID:26891104

  3. Analysis of tropospheric aerosol number density for aerosols of 0.2- to 3-micrometers diameter: Central and northeastern Canada

    NASA Technical Reports Server (NTRS)

    Gregory, Gerald L.; Anderson, Bruce E.; Barrick, John D.; Hudgins, Charles H.; Bagwell, Donald R.; Blake, Donald R.

    1994-01-01

    NASA's Atmospheric Boundary Layer Experiment conducted during the summer of 1990 focused on the distribution of trace species in central and northeastern Canada (altitudes less than 6 km) and the importance of surface sources/sinks, local emissions, distant transport, tropospheric/stratospheric exchange. Aircraft flights were based from North Bay, Ontario, and Goose Bay, Labrador, Canada. As part of the aircraft measurements, aerosol number density (0.2- to 3-micrometers diameter) was measured using an optical laser technique. Results show that summertime aerosol budgets of central and northeastern Canada can be significantly impacted by the transport of pollutants from distant source regions. Biomass burning in Alaska and western and central Canada exerts major influences on regional aerosol budgets. Urban emissions transported from the U.S./Canadian border regions are also important. Aerosol enhancements (mixed layer and free troposphere) were most prevalent in air with carbon monoxide mixing ratios greater than 110 parts per billion by volume (ppbv). When data were grouped as to the source of the air (5-day back trajectories) either north or south of the polar jet, aerosol number density in the mixed layer showed a tendency to be enhanced for air south of the jet relative to north of the jet. However, this difference was not observed for measurements at the higher altitudes (4 to 6 km). For some flights, mixed layer aerosol number densities were greater than 100 higher than free-tropospheric values (3- to 6-km altitude). The majority of the observed mixed layer enhancement was associated with transport of effluent-rich air into the Canadian regions. Aerosol emissions from natural Canadian ecosystems were relatively small when compared to transport.

  4. Effect of Sodium Fluorescein and Plating Medium on Recovery of Irradiated Escherichia coli and Serratia marcescens from Aerosols

    PubMed Central

    Dorsey, Emerson L.; Berendt, Richard F.; Neff, Everett L.

    1970-01-01

    Irradiation of aerosols of either Escherichia coli or Serratia marcescens with simulated solar (xenon) radiation caused a significant decrease in viability. When sodium fluorescein was employed to determine the physical loss of organisms from the aerosol, an additional adverse effect upon survival was noted. The decay curves indicated that at least two mechanisms of inactivation were operative, one due to aerosolization, the other to irradiation. After collection from aerosols, both species of microorganisms grew better on blood agar base than on Casitone agar, but this finding did not appear to be related to the effect of irradiation. PMID:4922085

  5. AERONET: The Aerosol Robotic Network

    DOE Data Explorer

    The AERONET (AErosol RObotic NETwork) program is a federation of ground-based remote sensing aerosol networks established by NASA and LOA-PHOTONS (CNRS) and is greatly expanded by collaborators from national agencies, institutes, universities, individual scientists, and partners. The program provides a long-term, continuous and readily accessible public domain database of aerosol optical, mircrophysical and radiative properties for aerosol research and characterization, validation of satellite retrievals, and synergism with other databases. The network imposes standardization of instruments, calibration, processing and distribution. AERONET collaboration provides globally distributed observations of spectral aerosol optical Depth (AOD), inversion products, and precipitable water in diverse aerosol regimes. Aerosol optical depth data are computed for three data quality levels: Level 1.0 (unscreened), Level 1.5 (cloud-screened), and Level 2.0 (cloud screened and quality-assured). Inversions, precipitable water, and other AOD-dependent products are derived from these levels and may implement additional quality checks.[Copied from http://aeronet.gsfc.nasa.gov/new_web/system_descriptions.html

  6. Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi

    NASA Astrophysics Data System (ADS)

    Kumar, Sudhanshu

    2012-07-01

    {Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi } Tracing of aerosol sources is an important task helpful for making control strategy, and for climate change study. However, it is a difficult job as aerosols have several sources, involve in complex atmospheric processing, degradation and removal processes. Several approaches have been used for this task, e.g., models, which are based on the input of chemical species; stable- and radio-isotope compositions of certain species; chemical markers in which trace metals are the better options because they persist in atmosphere until the life of a particle. For example, K and Hg are used for biomass and coal burning tracings, respectively. Open waste burning has recently been believed to be a considerable source of aerosols in several mega cities in India and China. To better understand this source contribution in New Delhi aerosols, we have conducted aerosol sampling at a landfill site (Okhla), and in proximity (within 1 km distance) of this site. Aerosol filter samples were acid digested in microwave digestion system and analyzed using inductively coupled plasma -- high resolution mass spectrometry (ICP-HRMS) for getting metal signatures in particles. The metals, e.g., Sn, Sb and As those are found almost negligible in remote aerosols, are maximized in these waste burning aerosols. Sample collected in other location of New Delhi also shows the considerable presence of these metals in particles. Preliminary studies of isotopic ratios of these metals suggested that these metals, especially Sn can be used as marker for tracing the open waste burning sources of aerosols in New Delhi.

  7. Estimating the influence of the secondary organic aerosols on present climate using ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    O'Donnell, D.; Tsigaridis, K.; Feichter, J.

    2011-01-01

    In recent years, several field measurement campaigns have highlighted the importance of the organic fraction of aerosol mass, and with such spatial diversity that one may assert that these aerosols are ubiquitous in the troposphere, with particular importance in continental areas. Investigation of the chemical composition of organic aerosol remains a work in progress, but it is now clear that a significant portion of the total organic mass is composed of secondary organic material, that is, aerosol chemically formed from gaseous volatile organic carbon (VOC) precursors. A number of such precursors, of both biogenic and anthropogenic origin, have been identified. Experimental, inventory building and modelling studies have followed. Laboratory studies have yielded information on the chemical pathways that lead to secondary organic aerosol (SOA) formation, and provided the means to estimate the aerosol yields from a given precursor-oxidant reaction. Global inventories of anthropogenic VOC emissions, and of biogenic VOC emitter species distribution and their emission potential have been constructed. Models have been developed that provide global estimates of precursor VOC emissions, SOA formation and atmospheric burdens of these species. This paper estimates the direct and indirect effects of these aerosols using the global climate-aerosol model ECHAM5-HAM. For year 2000 conditions, we estimate a global annual mean shortwave (SW) aerosol direct effect due to SOA of -0.3 W m-2. The model predicts a positive SW indirect effect due to SOA amounting to +0.23 W m-2, arising from enlargement of particles due to condensation of SOA, together with an enhanced coagulation sink for small particles. Longwave effects are small. Finally, we indicate of areas of research into SOA that are required in order to better constrain our estimates of the influence of aerosols on the climate system.

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

    NASA Astrophysics Data System (ADS)

    Dreyfus, Matthew A.

    Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

  9. Regional aerosol properties: Comparisons of boundary layer measurements from ACE 1, ACE 2, Aerosols99, INDOEX, ACE Asia, TARFOX, and NEAQS

    NASA Astrophysics Data System (ADS)

    Quinn, Patricia K.; Bates, Timothy S.

    2005-07-01

    , which means there is a large and variable fraction of the aerosol that is not sulfate, (2) particulate organic matter (POM) makes up 1 to 51% of the submicron mass, with highest POM mass fractions observed downwind of the NE United States, (3) highest submicron mass fractions of EC and lowest single-scattering albedos were observed in biomass-burning plumes from Africa and downwind of the Indian subcontinent, (4) NO3- was found predominantly in the supermicron size range due to the interaction of gas phase oxidized nitrogen species with sea salt aerosol, and (5) mass extinction efficiencies for the individual chemical components were consistent between regions. All data presented are available as auxiliary material.

  10. Near-highway aerosol and gas-phase measurements in a high-diesel environment

    NASA Astrophysics Data System (ADS)

    DeWitt, H. L.; Hellebust, S.; Temime-Roussel, B.; Ravier, S.; Polo, L.; Jacob, V.; Buisson, C.; Charron, A.; André, M.; Pasquier, A.; Besombes, J. L.; Jaffrezo, J. L.; Wortham, H.; Marchand, N.

    2015-04-01

    Diesel-powered passenger cars currently outnumber gasoline-powered cars in many countries, particularly in Europe. In France, diesel cars represented 61% of light duty vehicles in 2011 and this percentage is still increasing (French Environment and Energy Management Agency, ADEME). As part of the September 2011 joint PM-DRIVE (Particulate Matter - DiRect and Indirect on-road Vehicular Emissions) and MOCOPO (Measuring and mOdeling traffic COngestion and POllution) field campaign, the concentration and high-resolution chemical composition of aerosols and volatile organic carbon species were measured adjacent to a major urban highway south of Grenoble, France. Alongside these atmospheric measurements, detailed traffic data were collected from nearby traffic cameras and loop detectors, which allowed the vehicle type, traffic concentration, and traffic speed to be quantified. Six aerosol age and source profiles were resolved using the positive matrix factorization model on real-time high-resolution aerosol mass spectra. These six aerosol source/age categories included a hydrocarbon-like organic aerosol (HOA) commonly associated with primary vehicular emissions, a nitrogen-containing aerosol with a diurnal pattern similar to that of HOA, oxidized organic aerosol (OOA), and biomass burning aerosol. While quantitatively separating the influence of diesel from that of gasoline proved impossible, a low HOA : black carbon ratio, similar to that measured in other high-diesel environments, and high levels of NOx, also indicative of diesel emissions, were observed. Although the measurement site was located next to a large source of primary emissions, which are typically found to have low oxygen incorporation, OOA was found to comprise the majority of the measured organic aerosol, and isotopic analysis showed that the measured OOA contained mainly modern carbon, not fossil-derived carbon. Thus, even in this heavily vehicular-emission-impacted environment, photochemical processes

  11. A comprehensive climatology of Arctic aerosol properties on the North Slope of Alaska

    NASA Astrophysics Data System (ADS)

    Creamean, Jessie; de Boer, Gijs; Shupe, Matthew; McComiskey, Allison

    2016-04-01

    Evaluating aerosol properties has implications for the formation of Arctic clouds, resulting in impacts on cloud lifetime, precipitation processes, and radiative forcing. There are many remaining uncertainties and large discrepancies regarding modeled and observed Arctic aerosol properties, illustrating the need for more detailed observations to improve simulations of Arctic aerosol and more generally, projections of the components of the aerosol-driven processes that impact sea ice loss/gain. In particular, the sources and climatic effects of Arctic aerosol particles are severely understudied. Here, we present a comprehensive, long-term record of aerosol observations from the North Slope of Alaska baseline site at Barrow. These measurements include sub- and supermicron (up to 10 μm) total mass and number concentrations, sub- and supermicron soluble inorganic and organic ion concentrations, submicron metal concentrations, submicron particle size distributions, and sub- and supermicron absorption and scattering properties. Aerosol extinction and number concentration measurements extend back to 1976, while the remaining measurements were implemented since. Corroboration between the chemical, physical, and optical property measurements is evident during periods of overlapping observations, demonstrating the reliability of the measurements. During the Arctic Haze in the winter/spring, high concentrations of long-range transported submicron sea salt, mineral dust, industrial metals, pollution (non-sea salt sulfate, nitrate, ammonium), and biomass burning species are observed concurrent with higher concentrations of particles with sizes that span the submicron range, enhanced absorption and scattering coefficients, and largest Ångström exponents. The summer is characterized by high concentrations of small biogenic aerosols (< 100 nm) and low extinction coefficients. Fall is characterized by clean conditions, with supermicron sea salt representing the dominant aerosol

  12. Aerosol growth in Titan's ionosphere.

    PubMed

    Lavvas, Panayotis; Yelle, Roger V; Koskinen, Tommi; Bazin, Axel; Vuitton, Véronique; Vigren, Erik; Galand, Marina; Wellbrock, Anne; Coates, Andrew J; Wahlund, Jan-Erik; Crary, Frank J; Snowden, Darci

    2013-02-19

    Photochemically produced aerosols are common among the atmospheres of our solar system and beyond. Observations and models have shown that photochemical aerosols have direct consequences on atmospheric properties as well as important astrobiological ramifications, but the mechanisms involved in their formation remain unclear. Here we show that the formation of aerosols in Titan's upper atmosphere is directly related to ion processes, and we provide a complete interpretation of observed mass spectra by the Cassini instruments from small to large masses. Because all planetary atmospheres possess ionospheres, we anticipate that the mechanisms identified here will be efficient in other environments as well, modulated by the chemical complexity of each atmosphere. PMID:23382231

  13. eDPS Aerosol Collection

    SciTech Connect

    Venzie, J.

    2015-10-13

    The eDPS Aerosol Collection project studies the fundamental physics of electrostatic aerosol collection for national security applications. The interpretation of aerosol data requires understanding and correcting for biases introduced from particle genesis through collection and analysis. The research and development undertaken in this project provides the basis for both the statistical correction of existing equipment and techniques; as well as, the development of new collectors and analytical techniques designed to minimize unwanted biases while improving the efficiency of locating and measuring individual particles of interest.

  14. Cloud water and aerosol studies in a background marine environment

    NASA Astrophysics Data System (ADS)

    Gioda, A.; Mayol-Bracero, O. L.; Reyes-Rodriguez, G.; Santos-Figueroa, G.; Morales-de Jesus, R.; Collett, J.; Decesari, S.; de Aquino Neto, F. R.; Klaus, C.; Bezerra, H.

    2007-12-01

    The study of aerosol and cloud water chemical composition is essential to understand cloud processing of different compounds, determining which species are more efficiently removed and which ones stay longer in the atmosphere and, therefore, are more important for aerosol climate forcing. As part of the Rain In Cumulus over the Ocean Experiment (RICO), cloud water and aerosol samples were collected in Puerto Rico. We present concentrations of water-soluble ions, total and dissolved organic carbon (TOC and DOC), total nitrogen (TN), and the speciation of nitrogen compounds (amino acids) for water and aerosol samples collected at East Peak and Cape San Juan, Puerto Rico. Mass and elemental/organic carbon (EC, OC) concentrations were also determined for the aerosol samples. The results show average concentrations of TOC and TN in cloud water of about 1.1 mg/L and for DOC about 0.9 mg/L. The DOC/TOC ratio averaged 0.78, indicating that most of the organic compounds present are dissolved in the cloud water. TOC was composed mainly of organic acids (47 percent) and TN of inorganic species (80 percent). With respect to the aerosol samples, the average mass concentration of fine particles (Dp < 1.7 um) was 2.4 ug/m3. EC was found at low-to-non detectable levels (< 0.5 ng/m3). The concentrations of OC, DOC, TOC, and TN ranged from 30 to 100 ng/m3. The size distributions showed that OC and TN were mainly present in the fine particle fractions (Dp < 1 um). The predominant ions for both cloud and aerosol samples were Cl- and Na+, the primary components of sea salt. However, when air masses arrived from Northwest Africa or from islands upwind of Puerto Rico there was a decrease in Na+ and Cl- concentrations and an increase in SO42-, NH3+ and Ca2+ concentrations, likely reflecting anthropogenic and crustal sources of these species. Overall, the average concentrations of all species are similar to those typically found in background (remote) environments; however, these

  15. Aerosol interactions between the surface and the atmosphere: Urban fluxes, forest canopy vertical exchange, and wintertime urban patterns

    NASA Astrophysics Data System (ADS)

    Grivicke, Rasa

    Atmospheric aerosols play a major role in regional atmospheric chemistry and air quality, while on a global scale, aerosol processes continue to represent the largest source of uncertainty related to climate change. An important aspect of understanding the role of aerosols in these areas is to document the vertical exchange of aerosols with the surface in both urban and rural landscapes since the vertical exchange represents important sources and sinks of aerosols on regional and global scales. In this dissertation, investigation of aerosol dynamics is described for three separate field studies. First, urban eddy covariance flux measurements were made from a building rooftop in Mexico City using a quadrupole aerosol mass spectrometer (Q-AMS) to determine the fluxes of aerosol species to/from the urban landscape. Second, conditional sampling of fine particles in updrafts and downdrafts was performed above a pine forest in Colorado using a thermal desorption chemical ionization mass spectrometer (TD-CIMS) to investigate the relative strengths of sources and sinks for speciated aerosol in a forest environment. Third, the aerosol and gas phase pollutant patterns, measured in Boise, ID during wintertime inversion conditions, were analyzed with respect to the daily evolution of the planetary boundary layer depth and surface meteorological conditions. This dissertation describes the methods used for each of the three studies and summarizes the analysis of the results.

  16. Aerosol Climate Time Series Evaluation In ESA Aerosol_cci

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  17. Chemistry of secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Yee, Lindsay Diana

    The photooxidation of volatile organic compounds (VOCs) in the atmosphere can lead to the formation of secondary organic aerosol (SOA), a major component of fine particulate matter. Improvements to air quality require insight into the many reactive intermediates that lead to SOA formation, of which only a small fraction have been measured at the molecular level. This thesis describes the chemistry of secondary organic aerosol (SOA) formation from several atmospherically relevant hydrocarbon precursors. Photooxidation experiments of methoxyphenol and phenolic compounds and C12 alkanes were conducted in the Caltech Environmental Chamber. These experiments include the first photooxidation studies of these precursors run under sufficiently low NOx levels, such that RO2 + HO2 chemistry dominates, an important chemical regime in the atmosphere. Using online Chemical Ionization Mass Spectrometery (CIMS), key gas-phase intermediates that lead to SOA formation in these systems were identified. With complementary particle-phase analyses, chemical mechanisms elucidating the SOA formation from these compounds are proposed. Three methoxyphenol species (phenol, guaiacol, and syringol) were studied to model potential photooxidation schemes of biomass burning intermediates. SOA yields (ratio of mass of SOA formed to mass of primary organic reacted) exceeding 25% are observed. Aerosol growth is rapid and linear with the organic conversion, consistent with the formation of essentially non-volatile products. Gas and aerosol-phase oxidation products from the guaiacol system show that the chemical mechanism consists of highly oxidized aromatic species in the particle phase. Syringol SOA yields are lower than that of phenol and guaiacol, likely due to unique chemistry dependent on methoxy group position. The photooxidation of several C12 alkanes of varying structure n-dodecane, 2-methylundecane, cyclododecane, and hexylcyclohexane) were run under extended OH exposure to investigate the

  18. Spectroscopic investigations of organic aerosol and its reaction with halogens, released by sea-salt activation

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Zetzsch, C.

    2009-04-01

    The release of reactive halogen species from sea-salt aerosol offers a class of reactants for heterogeneous reactions of utmost importance. These heterogeneous reactions have been overlooked so far, although they may occur with internal and external mixtures of sea-salt aerosol and organic aerosol or organic matter. Such reactions might constitute sources of gaseous organohalogen compounds or halogenated organic aerosol in the atmospheric boundary layer. Infrared and UV/VIS spectroscopy provide an insight into chemical processes at reactive sites of the organic phase on a molecular level. Model studies of heterogeneous reactions of halogens with different kinds of (secondary) organic aerosols and organic matter were performed using a 700L smog chamber with a solar simulator. The model compounds alpha-pinene, catechol and humic acid have been chosen as precursors/material for the condensed, organic phase of the aerosol. After formation of the secondary organic aerosol or preparation of the organic material and the sea-salt solution the reaction was carried out using molecular chlorine and bromine in the presence of simulated sunlight. Chemical transformation of the organic material was studied using attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) on a ZnSe crystal and diffuse reflectance UV/VIS spectroscopy. An electrostatic precipitator was developed to deposit the aerosol particles on the ATR crystal as a thin film. On the other hand, longpath-FTIR spectroscopy with a 40m White-cell allows us to monitor both the condensed and gas phase of the aerosol in situ in the smog chamber directly. These spectroscopic techniques enable us to characterize different organic aerosol particles and their functional groups at reactive sites on these particles as well as to study aerosol formation and transformation directly. The heterogeneous reaction of reactive halogen species with organic material at atmospheric conditions leads to small reactive

  19. Characterization of the seasonal cycle of south Asian aerosols: A Regional-Scale Modeling Analysis.

    SciTech Connect

    Adhikary, Bhupesh; Carmichael, Gregory; Tang, Youhua; Leung, Lai-Yung R.; Qian, Yun; Schauer, James J.; Stone, Elizabeth A.; Ramanathan, Veerabhadran; Ramana, Muvva V.

    2007-11-07

    The STEM chemical transport model is used to study the aerosol distribution, composition and seasonality over South Asia from September 2004 to August 2005. Model predictions of sulfate, black carbon, primary organic carbon, other anthropogenic particulate matter, wind blown mineral dusts and sea salt are compared at two sites in South Asia where year long experimental observations are available from the Atmospheric Brown Cloud (ABC) Project. The model predictions are able to capture both the magnitude and seasonality of aerosols over Hanimaadhoo Observatory, Maldives. However, the model is not able to explain the seasonality at the Kathmandu Observatory; but the model does capture Kathmandu’s observed annual mean concentration. The absence of seasonal brick kiln emissions within Kathmandu valley in the current inventory is a probable reason for this problem. This model study reveals high anthropogenic aerosol loading over the Ganges valley even in the monsoonal months, which needs to be corroborated by experimental observations. Modeling results also show a high dust loading over South Asia with a distinct seasonality. Model results of aerosol monthly composition are also presented at 5 cities in South Asia. Total and fine mode aerosol optical depth along with contribution from each aerosol species is presented; the results show that the anthropogenic fraction dominates in the dry season with major contributions from sulfate and absorbing aerosols. Finally comparison with observations show that model improvements are needed in the treatment of aerosol dry and wet removal processes and increase in sulfate production via heterogeneous pathways.

  20. Aerosol speciation and mass prediction from toluene oxidation under high NO x conditions

    NASA Astrophysics Data System (ADS)

    Kelly, Janya L.; Michelangeli, Diane V.; Makar, Paul A.; Hastie, Donald R.; Mozurkewich, Michael; Auld, Janeen

    2010-01-01

    A kinetically based gas-particle partitioning box model is used to highlight the importance of parameter representation in the prediction of secondary organic aerosol (SOA) formation following the photo-oxidation of toluene. The model is initialized using experimental data from York University's indoor smog chamber and provides a prediction of the total aerosol yield and speciation. A series of model sensitivity experiments were performed to study the aerosol speciation and mass prediction under high NO x conditions (VOC/NO x = 0.2). Sensitivity experiments indicate vapour pressure estimation to be a large area of weakness in predicting aerosol mass, creating an average total error range of 70 μg m -3 (range of 5-145 μg m -3), using two different estimation methods. Aerosol speciation proved relatively insensitive to changes in vapour pressure. One species, 3-methyl-6-nitro-catechol, dominated the aerosol phase regardless of the vapour pressure parameterization used and comprised 73-88% of the aerosol by mass. The dominance is associated with the large concentration of 3-methyl-6-nitro-catechol in the gas-phase. The high NO x initial conditions of this study suggests that the predominance of 3-methyl-6-nitro-catechol likely results from the cresol-forming branch in the Master Chemical Mechanism taking a significant role in secondary organic aerosol formation under high NO x conditions. Further research into the yields and speciation leading to this reaction product is recommended.

  1. Stratospheric aerosol geoengineering

    NASA Astrophysics Data System (ADS)

    Robock, Alan

    2015-03-01

    The Geoengineering Model Intercomparison Project, conducting climate model experiments with standard stratospheric aerosol injection scenarios, has found that insolation reduction could keep the global average temperature constant, but global average precipitation would reduce, particularly in summer monsoon regions around the world. Temperature changes would also not be uniform; the tropics would cool, but high latitudes would warm, with continuing, but reduced sea ice and ice sheet melting. Temperature extremes would still increase, but not as much as without geoengineering. If geoengineering were halted all at once, there would be rapid temperature and precipitation increases at 5-10 times the rates from gradual global warming. The prospect of geoengineering working may reduce the current drive toward reducing greenhouse gas emissions, and there are concerns about commercial or military control. Because geoengineering cannot safely address climate change, global efforts to reduce greenhouse gas emissions and to adapt are crucial to address anthropogenic global warming.

  2. Aerosols over Eastern Asia

    NASA Technical Reports Server (NTRS)

    2002-01-01

    This Sea-viewing Wide Field-of-view Sensor (SeaWiFS) image of eastern Asia from October 14, 2001, shows large amounts of aerosol in the air. A few possible point sources of smoke, probably fires, are visible north of the Amur River at the very top of the image. One of the larger of these plumes can be seen down river of the confluence of the Songhua and Amur rivers. At lower left, the Yangtze River plume in the East China Sea is also very prominent. Sediment suspended in the ocean water is quite brown near the shore, but becomes much greener as it diffuses into the water. The increasing greenness of the river plume is probably an indication of enhanced phytoplankton growth driven by the nutrients in the river runoff. Image courtesy the SeaWiFS Project, NASA/Goddard Space Flight Center, and ORBIMAGE

  3. Stratospheric aerosol geoengineering

    SciTech Connect

    Robock, Alan

    2015-03-30

    The Geoengineering Model Intercomparison Project, conducting climate model experiments with standard stratospheric aerosol injection scenarios, has found that insolation reduction could keep the global average temperature constant, but global average precipitation would reduce, particularly in summer monsoon regions around the world. Temperature changes would also not be uniform; the tropics would cool, but high latitudes would warm, with continuing, but reduced sea ice and ice sheet melting. Temperature extremes would still increase, but not as much as without geoengineering. If geoengineering were halted all at once, there would be rapid temperature and precipitation increases at 5–10 times the rates from gradual global warming. The prospect of geoengineering working may reduce the current drive toward reducing greenhouse gas emissions, and there are concerns about commercial or military control. Because geoengineering cannot safely address climate change, global efforts to reduce greenhouse gas emissions and to adapt are crucial to address anthropogenic global warming.

  4. Aerosol lidar ``M4``

    SciTech Connect

    Shelevoy, C.D.; Andreev, Y.M. |

    1994-12-31

    Small carrying aerosol lidar in which is used small copper vapor laser ``Malachite`` as source of sounding optical pulses is described. The advantages of metal vapor laser and photon counting mode in acquisition system of lidar gave ability to get record results: when lidar has dimensions (1 x .6 x .3 m) and weight (65 kg), it provides the sounding of air industrial pollutions at up to 20 km range in scanning sector 90{degree}. Power feed is less than 800 Wt. Lidar can be disposed as stationary so on the car, helicopter, light plane. Results of location of smoke tails and city smog in situ experiments are cited. Showed advantages of work of acquisition system in photon counting mode when dynamic range of a signal is up to six orders.

  5. Aerosol Transmission of Filoviruses

    PubMed Central

    Mekibib, Berhanu; Ariën, Kevin K.

    2016-01-01

    Filoviruses have become a worldwide public health concern because of their potential for introductions into non-endemic countries through international travel and the international transport of infected animals or animal products. Since it was first identified in 1976, in the Democratic Republic of Congo (formerly Zaire) and Sudan, the 2013–2015 western African Ebola virus disease (EVD) outbreak is the largest, both by number of cases and geographical extension, and deadliest, recorded so far in medical history. The source of ebolaviruses for human index case(s) in most outbreaks is presumptively associated with handling of bush meat or contact with fruit bats. Transmission among humans occurs easily when a person comes in contact with contaminated body fluids of patients, but our understanding of other transmission routes is still fragmentary. This review deals with the controversial issue of aerosol transmission of filoviruses. PMID:27223296

  6. Aerosol Transmission of Filoviruses.

    PubMed

    Mekibib, Berhanu; Ariën, Kevin K

    2016-01-01

    Filoviruses have become a worldwide public health concern because of their potential for introductions into non-endemic countries through international travel and the international transport of infected animals or animal products. Since it was first identified in 1976, in the Democratic Republic of Congo (formerly Zaire) and Sudan, the 2013-2015 western African Ebola virus disease (EVD) outbreak is the largest, both by number of cases and geographical extension, and deadliest, recorded so far in medical history. The source of ebolaviruses for human index case(s) in most outbreaks is presumptively associated with handling of bush meat or contact with fruit bats. Transmission among humans occurs easily when a person comes in contact with contaminated body fluids of patients, but our understanding of other transmission routes is still fragmentary. This review deals with the controversial issue of aerosol transmission of filoviruses. PMID:27223296

  7. Aerosol characterization over Sundarban mangrove forest at the north-east coast of Bay of Bengal, India

    NASA Astrophysics Data System (ADS)

    Chatterjee, Abhijit; Das, Sanat Kumar; Sarkar, Chirantan; Ghosh, Sanjay; Raha, Sibaji; Singh, Soumendra; Roy, Arindam

    2016-07-01

    A comprehensive study was conducted on chemical characterization of size segregated and cumulative aerosols during winter, 2015 and summer 2016 over a remote mangrove forest at Sundarban at the north-east coast of Bay of Bengal. Aerosols originated from the surf zone at the land-ocean boundary of Sundarban mangrove forest and aerosols advected from Kolkata and other metropolitan and urban cities at Indo-Gangetic Plain were characterized in terms of major water soluble inorganic species. Attempt was made to investigate the combined effect of locally generated sea-salt and advected anthropogenic aerosols could change the pristine marine character at this region during the above mentioned periods. Significant chloride depletion from sea-salt aerosols was observed in coarse and ultrafine mode compared to fine mode in winter whereas reverse trend was observed during summer. On an average the chloride to sodium ratio in PM10 aerosol was found to be around 0.6 which was much lower than that in sea-water. It was observed that non-sea-sulphate and nitrate aerosols were the major species depleting chloride from sea-salt aerosols. This supported the interaction between fresh marine and polluted anthropogenic aerosols. The average concentration of PM10 aerosols was 64 μg m-3 in winter and 89 μg m-3 in summer. Major water soluble ionic species were used for the source apportionment of aerosol during the two seasons. On an average it was observed that 60-70 % of total PM10 aerosols were constituted by the major water soluble ionic species. Emission flux and deposition flux of aerosols were also studied over this remote forest region. It was also observed that anthropogenic ionic species were mostly accumulated in the ultrafine and fine mode region both during winter and summer. On the other hand sea-salt species were mostly accumulated in the coarse mode region. Sulphate aerosol showed bimodal distribution with prominent peaks both at ultrafine/fine and coarse mode region

  8. Soft ionization of thermally evaporated hypergolic ionic liquid aerosols

    SciTech Connect

    University of California; ERC, Incorporated, Edwards Air Force Base; Air Force Research Laboratory, Edwards Air Force Base; National Synchrotron Radiation Research Center; Institute of Chemistry, Hebrew University; Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; Vaghjiani, Ghanshyam L.; Leone, Stephen R.

    2011-07-19

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N?]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca?]), are generated by vaporizing ionic liquid submicron aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Photoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N?]ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~;;0.3 eV), attributed to reduced internal energy of the isolated ion pairs. The method of ionic liquid submicron aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally ?cooler? source of isolated intact ion pairs in the gas phase compared to effusive sources.

  9. Soft Ionization of Thermally Evaporated Hypergolic Ionic Liquid Aerosols

    SciTech Connect

    Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; Vaghjiani, Ghanshyam L.; Leone, Stephen R.

    2011-04-20

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N–]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca–]), are generated by vaporizing ionic liquid submicrometer aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Also, hotoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N] ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~0.3 eV), attributed to reduced internal energy of the isolated ion pairs. Lastly, the method of ionic liquid submicrometer aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally “cooler” source of isolated intact ion pairs in the gas phase compared to effusive sources.

  10. Organic Aerosols in Rural and Remote Atmospheric Environments: Insights from Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Zhang, Q.; Jimenez, J.; Ulbrich, I.; Dunlea, E.; Decarlo, P.; Huffman, A.; Allan, J.; Coe, H.; Alfarra, R.; Canagaratna, M.; Onasch, T.; Jayne, J.; Worsnop, D.; Takami, A.; Miyoshi, T.; Shimono, A.; Hatakeyama, S.; Weimer, S.; Demerjian, K.; Drewnick, F.; Schneider, J.; Middlebrook, A.; Bahreini, R.; Cotrell, L.; Griffin, R.; Leaitch, R.; Li, S.; Hayden, K.; Rautiainen, J.

    2006-12-01

    Organic matter usually accounts for a large fraction of the fine particle mass in rural and remote atmospheres. However, little is known about the sources and properties of this material. Here we report findings on the characteristics and the major types of organic aerosols (OA) in urban downwind, high elevation, forested, and marine atmospheres based on analyses of more than 20 highly time resolved AMS datasets sampled from various locations in the mid-latitude Northern Hemisphere. Organic aerosol components are extracted from these datasets using a custom multiple component mass spectral analysis technique and the Positive Matrix Factorization (PMF) method. These components are evaluated according to their extracted mass spectra and correlations to aerosol species, such as sulfate, nitrate, and elemental carbon, and gas-phase tracer compounds, such as CO and NOx. We have identified a hydrocarbon-like organic aerosol (HOA) component similar in mass spectra to the hydrocarbon substances observed at urban locations. We have also identified several oxygenated OA (OOA) components that show different fragmentation patterns and oxygen to carbon ratios in their mass spectra. Two OOA components a highly oxygenated that has mass spectrum resembling that of fulvic acid (a model compound representative for highly processed/oxidized organics in the environment) and a less oxygenated OOA component, whose spectrum is dominated with ions that are mainly associated with carbonyls and alcohols, are very frequently observed at various rural/remote sites. The oxygenated OOA component is more prevalent at downwind sites influenced by urban transport and the less oxygenated shows correlation to biogenic chamber OA at some locations. Compared to the total OOA concentration, HOA is generally very small and accounts for < 10% of the total OA mass at rural/remote sites. The comparisons between the concentrations of HOA and primary OA (POA) that would be predicted according to inert

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

    NASA Astrophysics Data System (ADS)

    Hock, N.; Schneider, J.; Borrmann, S.; Römpp, A.; Moortgat, G.; Franze, T.; Schauer, C.; Pöschl, U.; Plass-Dülmer, C.; Berresheim, H.

    2008-02-01

    Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD) in Southern Germany. Online measurements included: Size-resolved chemical composition of submicron particles; total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm; gas-phase concentration of monoterpenes, CO, O3, OH, and H2SO4. Filter sampling and offline analytical techniques were used to determine: Fine particle mass (PM2.5), organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5), and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins). Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m-3, arithmetic mean and standard deviation) accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m-3). The relative proportions of non-refractory submicron particle components were: (23±39)% ammonium nitrate, (27±23)% ammonium sulfate, and (50±40)% organics (OM1). OM1 was closely correlated with PM1 (r2=0.9) indicating a near-constant ratio of non-refractory organics and inorganics. The average ratio of OM1 to OC2.5 was 2.1±1.4, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA) over hydrocarbon-like organic aerosol (HOA) inferred from the AMS results (4:1), and also with the high abundance of proteins (~3%) indicating a high proportion of primary biological material (~30%) in PM2.5. This finding was confirmed by low abundance of PAHs (<1 ng m-3) and EC (<1 μg m-3) in PM2.5 and detection of several secondary organic aerosol compounds (dicarboxylic acids) and their precursors (monoterpenes). New particle formation was observed almost

  12. Response of aerosol composition to different emission scenarios in Beijing, China.

    PubMed

    Zhang, Yingjie; Sun, Yele; Du, Wei; Wang, Qingqing; Chen, Chen; Han, Tingting; Lin, Jian; Zhao, Jian; Xu, Weiqi; Gao, Jian; Li, Jie; Fu, Pingqing; Wang, Zifa; Han, Yongxiang

    2016-11-15

    Understanding the response of aerosol chemistry to different emission scenarios is of great importance for air pollution mitigating strategies in megacities. Here we investigate the variations in air pollutants under three different emission scenarios, i.e., heating season, spring festival holiday and non-heating season using aerosol composition and gaseous measurements from 2 February to 1 April 2015 along with source apportionment and FLEXPART analysis in Beijing. Our results showed substantially different aerosol composition among three emission scenarios that is primarily caused by different emission sources. All aerosol and gas species showed ubiquitously higher concentrations in heating season than non-heating season with the largest enhancement for fossil OA (FOA) and chloride. On average, the particulate matter (PM) level in winter heating season can be enhanced by 70% due to coal combustion emissions. In contrast, cooking aerosols and traffic related species showed significant reductions as a response of reduced anthropogenic activities during the spring festival holiday, sulfate and secondary organic aerosol (SOA) however even increased due to enhanced aqueous-phase production. Such compensating effects resulted in small changes in PM levels for haze episodes during the holiday period despite reduced anthropogenic emissions. Our results have significant implications that local emission controls during winter severe pollution episodes can reduce primary aerosols substantially, but the mitigating effects can be significantly suppressed by enhanced secondary formation under stagnant meteorological conditions. PMID:27425439

  13. Aerosol optical depth, aerosol composition and air pollution during summer and winter conditions in Budapest.

    PubMed

    Alföldy, B; Osán, J; Tóth, Z; Török, S; Harbusch, A; Jahn, C; Emeis, S; Schäfer, K

    2007-09-20

    The dependence of aerosol optical depth (AOD) on air particulate concentrations in the mixing layer height (MLH) was studied in Budapest in July 2003 and January 2004. During the campaigns gaseous (CO, SO(2), NO(x), O(3)), solid components (PM(2.5), PM(10)), as well as ionic species (ammonium, sulfate and nitrate) were measured at several urban and suburban sites. Additional data were collected from the Budapest air quality monitoring network. AOD was measured by a ground-based sun photometer. The mixing layer height and other common meteorological parameters were recorded. A linear relationship was found between the AOD and the columnar aerosol burden; the best linear fit (R(2)=0.96) was obtained for the secondary sulfate aerosol due to its mostly homogeneous spatial distribution and its optically active size range. The linear relationship is less pronounced for the PM(2.5) and PM(10) fractions since local emissions are very heterogeneous in time and space. The results indicate the importance of the mixing layer height in determining pollutant concentrations. During the winter campaign, when the boundary layer decreases to levels in between the altitudes of the sampling stations, measured concentrations showed significant differences due to different local sources and long-range transport. In the MLH time series unexpected nocturnal peaks were observed. The nocturnal increase of the MLH coincided with decreasing concentrations of all pollutants except for ozone; the ozone concentration increase indicates nocturnal vertical mixing between different air layers.

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

    The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

  15. Elevated nitrogen isotope ratios of tropical Indian aerosols from Chennai: Implication for the origins of aerosol nitrogen in South and Southeast Asia

    NASA Astrophysics Data System (ADS)

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

    2010-09-01

    To better understand the origins of aerosol nitrogen, we measured concentrations of total nitrogen (TN) and its isotope ratios (δ 15N) in tropical Indian aerosols (PM 10) collected from Chennai (13.04°N; 80.17°E) on day- and night-time basis in winter and summer 2007. We found high δ 15N values (+15.7 to +31.2‰) of aerosol N (0.3-3.8 μg m -3), in which NH 4+ is the major species (78%) with lesser contribution from NO 3- (6%). Based on the comparison of δ 15N in Chennai aerosols with those reported for atmospheric aerosols from mid-latitudes and for the particles emitted from point sources (including a laboratory study), as well as the δ 15N ratios of cow-dung samples (this study), we found that the atmospheric aerosol N in Chennai has two major sources; animal excreta and bio-fuel/biomass burning from South and Southeast Asia. We demonstrate that a gas-to-particle conversion of NH 3 to NH 4HSO 4 and (NH 4) 2SO 4 and the subsequent exchange reaction between NH 3 and NH 4+ are responsible for the isotopic enrichment of 15N in aerosol nitrogen.

  16. The thermodynamic and kinetic impacts of organics on marine aerosols

    NASA Astrophysics Data System (ADS)

    Crahan, Kathleen

    Organics can change the manner in which aerosols scatter radiation directly as hydrated aerosols and indirectly as in-cloud activated aerosols, through changing the solution activity, the surface tension, and the accommodation coefficient of the hydrated aerosol. This work explores the kinetic and thermodynamic impacts of the organic component of marine aerosols through data collected over four field campaigns and through several models used to reproduce observations. The Rough Evaporation Duct (RED) project was conducted in the summer of 2001 off the coast of Oahu using the Twin Otter Aircraft and the Floating Instrument Platform research platform for data collection. The Cloud-Aerosol Research in the Marine Atmosphere (CARMA) campaigns were conducted over three summers (2002, 2004, 2005) off the coast of Monterey, California. During the CARMA campaigns, a thick, moist, stratocumulus deck was present during most days, and the Twin Otter Aircraft was the primary research platform used to collect data. However, the research goals and exact instrumentation onboard the Twin Otter varied from campaign to campaign, and each data set was analyzed individually. Data collected from CARMA I were used to explore the mechanism of oxalic acid production in cloud droplets. Oxalate was observed in the clouds in excess to below cloud concentrations by an average of 0.11 mug m-3, suggesting an in-cloud production. The tentative identification in cloud water of an intermediate species in the aqueous oxalate production mechanism lends further support to an in-cloud oxalate source. The data sets collected during the RED campaign and the CARMA II and CARMA III campaigns were used to investigate the impact of aerosol chemical speciation on aerosol hygroscopic behavior. Several models were used to correlate the observations in the subsaturated regime to theory including an explicit thermodynamic model, simple Kohler theory, and a parameterization of the solution activity. These models

  17. Uptake of HO2 Radicals Onto Dust Aerosols

    NASA Astrophysics Data System (ADS)

    Matthews, P. S.; Whalley, L. K.; Baeza-Romero, M. T.; Heard, D. E.

    2013-12-01

    OH and HO2 radicals play an important role in the troposphere by controlling its oxidative capacity and therefore the concentration of many trace species. Several field studies have observed significantly lower concentrations of HO2 radicals than predicted using box models (1,2). HO2 loss onto aerosols has been suggested as a possible sink. Mineral dust has an estimated annual flux of 2000 Tg year-1 (3). However, there has only been one study of HO2 uptake onto Arizona Test Dust (ATD) surfaces (4) and there are currently no published studies for dust aerosols. Therefore, the aim of this study was to measure the HO2 uptake coefficient onto ATD aerosols over a range of humidities and for different HO2 concentrations, as well as investigating the uptake as a function of the exposure time to the aerosol, for which a dependence had been observed for aqueous salt aerosols (5). Uptake coefficients were measured for ATD aerosols at atmospheric pressure and at 291 K using a Fluorescence Assay by Gas Expansion (FAGE) detector combined with a flow tube. HO2 was formed from the photolysis of water vapour and was injected into the flow tube using a moveable injector, which was placed in six different positions along the flow tube. The non stable aerosol output was produced by stirring ATD in a bottle producing a dust cloud which was entrained into a flow. The aerosol number concentration was measured using a Condensation Particle Counter (CPC) and was converted into a surface area using the average radius of one aerosol. The uptake coefficient was then able to be calculated by assuming first order kinetics. The HO2 uptake coefficient was measured at a relative humidity of between 6 and 75% and at initial HO2 concentrations of ~ 0.3 - 1 × 10^9 molecule cm-3. Average uptake coefficients of 0.018 × 0.006 and 0.031 × 0.008 were measured for the higher and lower HO2 concentrations respectively, and the impact investigated using a constrained box model. A time dependence was also

  18. An overview of geoengineering of climate using stratospheric sulphate aerosols.

    PubMed

    Rasch, Philip J; Tilmes, Simone; Turco, Richard P; Robock, Alan; Oman, Luke; Chen, Chih-Chieh; Stenchikov, Georgiy L; Garcia, Rolando R

    2008-11-13

    We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changes in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of 'acid rain' that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy

  19. An overview of geoengineering of climate using stratospheric sulphate aerosols

    SciTech Connect

    Rasch, Philip J.; Tilmes, S.; Turco, Richard P.; Robock, Alan; Oman, Luke; Chen, Chih-Chieh; Stenchikov, Georgiy; Garcia, Rolando R.

    2010-01-01

    We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changes in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of ‘acid rain’ that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy

  20. Background stratospheric aerosol reference model

    NASA Technical Reports Server (NTRS)

    Mccormick, M. P.; Wang, P.

    1989-01-01

    In this analysis, a reference background stratospheric aerosol optical model is developed based on the nearly global SAGE 1 satellite observations in the non-volcanic period from March 1979 to February 1980. Zonally averaged profiles of the 1.0 micron aerosol extinction for the tropics and the mid- and high-altitudes for both hemispheres are obtained and presented in graphical and tabulated form for the different seasons. In addition, analytic expressions for these seasonal global zonal means, as well as the yearly global mean, are determined according to a third order polynomial fit to the vertical profile data set. This proposed background stratospheric aerosol model can be useful in modeling studies of stratospheric aerosols and for simulations of atmospheric radiative transfer and radiance calculations in atmospheric remote sensing.

  1. Stratospheric aerosols and climatic change

    NASA Technical Reports Server (NTRS)

    Baldwin, B.; Pollack, J. B.; Summers, A.; Toon, O. B.; Sagan, C.; Van Camp, W.

    1976-01-01

    Generated primarily by volcanic explosions, a layer of submicron silicate particles and particles made of concentrated sulfuric acids solution is present in the stratosphere. Flights through the stratosphere may be a future source of stratospheric aerosols, since the effluent from supersonic transports contains sulfurous gases (which will be converted to H2SO4) while the exhaust from Space Shuttles contains tiny aluminum oxide particles. Global heat balance calculations have shown that the stratospheric aerosols have made important contributions to some climatic changes. In the present paper, accurate radiative transfer calculations of the globally-averaged surface temperature (T) are carried out to estimate the sensitivity of the climate to changes in the number of stratospheric aerosols. The results obtained for a specified model atmosphere, including a vertical profile of the aerosols, indicate that the climate is unlikely to be affected by supersonic transports and Space Shuttles, during the next decades.

  2. Satellite measurements of tropospheric aerosols

    NASA Technical Reports Server (NTRS)

    Griggs, M.

    1981-01-01

    This investigation uses LANDSAT 2 radiance data and ground-truth measurements of the aerosol optical thickness, obtained previously from five inland sites, to study the usefulness and limitations of the near infrared radiance over inland bodies of water. The linear relationship between LANDSAT 2 MSS7 and aerosol content found in this study can be used to estimate the aerosol content with a standard deviation of 0.42N. Analysis of the data for MSS6 and MSS7 suggest that the larger uncertainty is mostly due to water turbidity, with little contribution from the adjacency effect. The relationship found is best applied to determine an average aerosol content over a period of time at a given target, or an area average at a given time over several targets close together.

  3. Quantifying aerosol mixing state with entropy and diversity measures

    NASA Astrophysics Data System (ADS)

    Riemer, N.; West, M.

    2013-11-01

    This paper presents the first quantitative metric for aerosol population mixing state, defined as the distribution of per-particle chemical species composition. This new metric, the mixing state index χ, is an affine ratio of the average per-particle species diversity Dα and the bulk population species diversity Dγ, both of which are based on information-theoretic entropy measures. The mixing state index χ enables the first rigorous definition of the spectrum of mixing states from so-called external mixture to internal mixture, which is significant for aerosol climate impacts, including aerosol optical properties and cloud condensation nuclei activity. We illustrate the usefulness of this new mixing state framework with model results from the stochastic particle-resolved model PartMC-MOSAIC. These results demonstrate how the mixing state metrics evolve with time for several archetypal cases, each of which isolates a specific process such as coagulation, emission, or condensation. Further, we present an analysis of the mixing state evolution for a complex urban plume case, for which these processes occur simultaneously. We additionally derive theoretical properties of the mixing state index and present a family of generalized mixing state indexes that vary in the importance assigned to low-mass-fraction species.

  4. Chemical and physicochemial properties of submicron aerosol agglomerates

    SciTech Connect

    Scripsick, R.C.; Ehrman, S.; Friedlander, S.K.

    1998-12-31

    This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory. The formation of nanometer-sized aerosol particles in a premixed methane flame from both solid-phase aerosol precursors and gas-phase precursors was investigated. Techniques were developed to determine the distribution of the individual chemical species as a function of agglomerate size by using inductively coupled plasma atomic emission spectroscopy (ICP-AES). To determine the distribution of chemical species both from particle to particle and within the particles on a nanometer scale, we used the analytical electron microscopy techniques of energy dispersive x-ray spectrometry (EDS) and electron energy loss spectrometry (EELS) coupled with transmission electron microscopy (TEM). The observed distribution of individual chemical species as a function of agglomerate size was linked to the material properties of the solid-phase precursors. For aerosol formed from gas-phase precursors by gas-to-particle conversion, the distribution of species on a manometer scale was found to correspond to the equilibrium phase distribution expected from equilibrium for the system at the flame temperatures.

  5. Elucidating the Chemical Complexity of Organic Aerosol Constituents Measured During the Southeastern Oxidant and Aerosol Study (SOAS)

    NASA Astrophysics Data System (ADS)

    Yee, L.; Isaacman, G. A.; Spielman, S. R.; Worton, D. R.; Zhang, H.; Kreisberg, N. M.; Wilson, K. R.; Hering, S. V.; Goldstein, A. H.

    2013-12-01

    Thousands of volatile organic compounds are uniquely created in the atmosphere, many of which undergo chemical transformations that result in more highly-oxidized and often lower vapor pressure species. These species can contribute to secondary organic aerosol, a complex mixture of organic compounds that is still not chemically well-resolved. Organic aerosol collected on filters taken during the Southeastern Oxidant and Aerosol Study (SOAS) constitute hundreds of unique chemical compounds. Some of these include known anthropogenic and biogenic tracers characterized using standardized analytical techniques (e.g. GC-MS, UPLC, LC-MS), but the majority of the chemical diversity has yet to be explored. By employing analytical techniques involving sample derivatization and comprehensive two-dimensional gas chromatography (GC x GC) with high-resolution-time-of-flight mass spectrometry (HR-ToF-MS), we elucidate the chemical complexity of the organic aerosol matrix along the volatility and polarity grids. Further, by utilizing both electron impact (EI) and novel soft vacuum ultraviolet (VUV) ionization mass spectrometry, a greater fraction of the organic mass is fully speciated. The GC x GC-HR-ToF-MS with EI/VUV technique efficiently provides an unprecedented level of speciation for complex ambient samples. We present an extensive chemical characterization and quantification of organic species that goes beyond typical atmospheric tracers in the SOAS samples. We further demonstrate that complex organic mixtures can be chemically deconvoluted by elucidation of chemical formulae, volatility, functionality, and polarity. These parameters provide insight into the sources (anthropogenic vs. biogenic), chemical processes (oxidation pathways), and environmental factors (temperature, humidity), controlling organic aerosol growth in the Southeastern United States.

  6. AEROSOL, CLOUDS, AND CLIMATE CHANGE

    SciTech Connect

    SCHWARTZ, S.E.

    2005-09-01

    Earth's climate is thought to be quite sensitive to changes in radiative fluxes that are quite small in absolute magnitude, a few watts per square meter, and in relation to these fluxes in the natural climate. Atmospheric aerosol particles exert influence on climate directly, by scattering and absorbing radiation, and indirectly by modifying the microphysical properties of clouds and in turn their radiative effects and hydrology. The forcing of climate change by these indirect effects is thought to be quite substantial relative to forcing by incremental concentrations of greenhouse gases, but highly uncertain. Quantification of aerosol indirect forcing by satellite- or ground-based remote sensing has proved quite difficult in view of inherent large variation in the pertinent observables such as cloud optical depth, which is controlled mainly by liquid water path and only secondarily by aerosols. Limited work has shown instances of large magnitude of aerosol indirect forcing, with local instantaneous forcing upwards of 50 W m{sup 66}-2. Ultimately it will be necessary to represent aerosol indirect effects in climate models to accurately identify the anthropogenic forcing at present and over secular time and to assess the influence of this forcing in the context of other forcings of climate change. While the elements of aerosol processes that must be represented in models describing the evolution and properties of aerosol particles that serve as cloud condensation particles are known, many important components of these processes remain to be understood and to be represented in models, and the models evaluated against observation, before such model-based representations can confidently be used to represent aerosol indirect effects in climate models.

  7. Method for producing monodisperse aerosols

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  8. Characterization of Organic Nitrogen in the Atmosphere Using High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Ge, X.; Sun, Y.; Chen, M.; Zhang, Q.

    2015-12-01

    Despite extensive efforts on characterizing organic nitrogen (ON) compounds in atmospheric aerosols and aqueous droplets, knowledge of ON chemistry is still limited, mainly due to its chemical complexity and lack of highly time-resolved measurements. This work is aimed at optimizing the method of using Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) to characterize ON compounds in atmospheric aerosols. Seventy-five pure nitrogen-containing organic compounds covering a variety of functional groups were analyzed with the HR-AMS. Our results show that ON compounds commonly produce NHx+, NOx+, which are usually attributed to inorganic N species such as ammonium and nitrate, and CH2N+ at m/z = 28, which is rarely quantified in ambient aerosol due to large interference from N2+ in the air signal. As a result, using the nitrogen-to-carbon (N/C) calibration factor proposed by Aiken et al. (2008) on average leads to ~ 20% underestimation of N/C in ambient organic aerosol. A new calibration factor of 0.79 is proposed for determining the average N/C in organics. The relative ionization efficiencies (RIEs) of different ON species, on average, are found to be consistent with the default RIE value (1.4) for the total organics. The AMS mass spectral features of various types of ON species (amines, amides, amino acids, etc.) are examined and used for characterizing ON composition in ambient aerosols. Our results indicate that submicron organic aerosol measured during wintertime in Fresno, CA contains significant amounts of amino-compounds whereas more diversified ON species, including N-containing aromatic heterocycle (e.g., imidazoles), are observed in fog waters collected simultaneously. Our findings have important implications for understanding atmospheric ON behaviors via the widespread HR-AMS measurements of ambient aerosols and droplets.

  9. Mass spectrometric airborne measurements of submicron aerosol and cloud residual composition in tropic deep convection during ACRIDICON-CHUVA

    NASA Astrophysics Data System (ADS)

    Schulz, Christiane; Schneider, Johannes; Mertes, Stephan; Kästner, Udo; Weinzierl, Bernadett; Sauer, Daniel; Fütterer, Daniel; Walser, Adrian; Borrmann, Stephan

    2015-04-01

    Airborne measurements of submicron aerosol and cloud particles were conducted in the region of Manaus (Amazonas, Brazil) during the ACRIDICON-CHUVA campaign in September 2014. ACRIDICON-CHUVA aimed at the investigation of convective cloud systems in order to get a better understanding and quantification of aerosol-cloud-interactions and radiative effects of convective clouds. For that, data from airborne measurements within convective cloud systems are combined with satellite and ground-based data. We used a C-ToF-AMS (Compact-Time-of-Flight-Aerosol-Mass-Spectrometer) to obtain information on aerosol composition and vertical profiles of different aerosol species, like organics, sulphate, nitrate, ammonium and chloride. The instrument was operated behind two different inlets: The HASI (HALO Aerosol Submicrometer Inlet) samples aerosol particles, whereas the CVI (Counterflow Virtual Impactor) samples cloud droplets and ice particles during in-cloud measurements, such that cloud residual particles can be analyzed. Differences in aerosol composition inside and outside of clouds and cloud properties over forested or deforested region were investigated. Additionally, the in- and outflow of convective clouds was sampled on dedicated cloud missions in order to study the evolution of the clouds and the processing of aerosol particles. First results show high organic aerosol mass concentrations (typically 15 μg/m3 and during one flight up to 25 μg/m3). Although high amounts of organic aerosol in tropic air over rainforest regions were expected, such high mass concentrations were not anticipated. Next to that, high sulphate aerosol mass concentrations (about 4 μg/m3) were measured at low altitudes (up to 5 km). During some flights organic and nitrate aerosol was observed with higher mass concentrations at high altitudes (10-12 km) than at lower altitudes, indicating redistribution of boundary layer particles by convection. The cloud residuals measured during in

  10. Satellite Remote Sensing: Aerosol Measurements

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2013-01-01

    Aerosols are solid or liquid particles suspended in the air, and those observed by satellite remote sensing are typically between about 0.05 and 10 microns in size. (Note that in traditional aerosol science, the term "aerosol" refers to both the particles and the medium in which they reside, whereas for remote sensing, the term commonly refers to the particles only. In this article, we adopt the remote-sensing definition.) They originate from a great diversity of sources, such as wildfires, volcanoes, soils and desert sands, breaking waves, natural biological activity, agricultural burning, cement production, and fossil fuel combustion. They typically remain in the atmosphere from several days to a week or more, and some travel great distances before returning to Earth's surface via gravitational settling or washout by precipitation. Many aerosol sources exhibit strong seasonal variability, and most experience inter-annual fluctuations. As such, the frequent, global coverage that space-based aerosol remote-sensing instruments can provide is making increasingly important contributions to regional and larger-scale aerosol studies.

  11. Climate forcing by anthropogenic aerosols.

    PubMed

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

    1992-01-24

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

  12. Climate Forcing by Anthropogenic Aerosols

    NASA Astrophysics Data System (ADS)

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

    1992-01-01

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

  13. Passive Remote Sensing of Aerosols

    NASA Technical Reports Server (NTRS)

    King, Michael D.

    2005-01-01

    Remote sensing of aerosol optical and microphysical properties got a resurgence in the 1970s when John Reagan and Ben Herman initiated a program to develop and implement a surface-based sunphotometer system to monitor spectral aerosol optical thickness at the University of Arizona. In this presentation I will review the state of the technology used to monitor aerosol optical and microphysical properties, including the determination of spectral aerosol optical thickness and total ozone content. This work continued with John Reagan developed a surface-based spectral flux radiometer to implement Ben Herman's idea to determine the imaginary part of the complex refractive index of aerosols using the recently developed diffuse-direct technique. Progress made both in surface-based instrumentation, inversion theory for analyzing such data, and in satellite observations of aerosol optical and microphysical properties will be reviewed to highlight the state of knowledge after 30 years of expanded capability and introduction of novel new capabilities, both from the ground and from spacecraft.

  14. Climate forcing by anthropogenic aerosols

    NASA Technical Reports Server (NTRS)

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

    1992-01-01

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

  15. Aerosols at a mountaintop observatory in Arizona

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    2007-04-01

    This paper discusses physics of aerosols measured at the summit of Mt. Lemmon, Arizona (2790 m), from February to May 2002, where "clean" air representative of the free troposphere sometimes occurs. We confirmed Marti's findings of a persistent daily variation in the number concentration of condensation nuclei (diameter > 10 nm), with a strong maximum occurring in the afternoon and minimum in the early morning. These particles show evidence of growth at rates of 10-23 nm per hour. The diurnal variation was present even on days when the planetary boundary layer remained below the mountain. From the rate of growth and Maxwellian diffusion theory, we deduce that precursor condensable species are present in daytime concentrations of 107-108 cm-3, and that these are produced at a rate of 105-106 cm-3 s-1. Increased convection caused by solar heating of the mountain often carries contaminated air to the summit. Yet only a small (factor of 1.5) diurnal pattern was found for accumulation mode (diameter ˜ 130 nm) particles on days where the convective boundary layer passed well above the station. We hypothesize that these long-lived (e.g., several days) aerosols are pumped into the free troposphere and remain behind at night in a residual layer. The free tropospheric aerosol size distribution measured at Mt. Lemmon was similar in shape but higher in magnitude (by around 50%) than at Jungfraujoch in the Swiss Alps (3580 m). There is much greater diurnal variation in Aitken-sized particles (daily factor of from 7 to 10) at Mt. Lemmon than observed at Jungfraujoch (factor of from 1.0 to 1.6), evidently arising from stronger photochemical rate of productions of precursor gases.

  16. Assessment of the Aerosol Distribution Over Indian Subcontinent in CMIP5 Models

    NASA Astrophysics Data System (ADS)

    Sanap, S. D.; Pandithurai, G.

    2014-12-01

    This paper examines the aerosol distribution over Indian subcontinent as represented in 21 models from Coupled Model Inter-comparison Project Phase 5 (CMIP5) simulations, wherein model simulated aerosol optical depth (AOD) is compared with Moderate Resolution Imaging Spectro-radiometer (MODIS) satellite observations. The objective of the study is to provide an assessment of the capability of various global models, participating in CMIP5 project, in capturing the realistic spatial and temporal distribution of aerosol species over the Indian subcontinent. Results from our analysis show that majority of the CMIP5 models seriously underestimates the spatio-temporal variability of aerosol species over the Indian subcontinent, in particular over Indo-Gangetic Plains(IGP). Though the representation of black carbon (BC) loading in many models is fairly good, the dust loading is observed to be significantly low in majority of the models. The presence of pronounced dust activity over northern India and dust being one of the major constituent of aerosol species, the biases in dust loading has a great impact on the AOD of that region. We found that considerable biases in simulating the 850 hPa wind field (which plays important role in transport of dust from adjacent deserts) would be the possible reason for poor representation of dust AOD and in turn total AOD over Indian region in CMIP5 models. In addition, aerosol radiative forcing (ARF) underestimated/overestimated in most of the models. However, spatial distribution of ARF in multi-model ensemble mean is comparable reasonably well with observations with bias in magnitudes. This analysis emphasizes the fundamental need to improve the representation of aerosol species in current state of the art climate models. As reported in Intergovernmental Panel on Climate Change (IPCC) fourth assessment report (AR4), the level of scientific understanding (LOSU) of climatic impact of aerosols is medium-low. For better understanding of

  17. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouch, N.; Pichon, J.-M.; Prévôt, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2013-09-01

    The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA

  18. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouche, N.; Pichon, J.-M.; Bourianne, T.; Gomes, L.; Prevot, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2014-02-01

    The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation

  19. Diversity of Aerosol Optical Thickness in analysis and forecasting modes of the models from the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME)

    NASA Astrophysics Data System (ADS)

    Lynch, P.

    2014-12-01

    With the emergence of global aerosol models intended for operational forecasting use at global numerical weather prediction (NWP) centers, the International Cooperative for Aerosol Prediction (ICAP) was founded in 2010. One of the objectives of ICAP is to develop a global multi-model aerosol forecasting ensemble (ICAP-MME) for operational and basic research use. To increase the accuracy of aerosol forecasts, several of the NWP centers have incorporated assimilation of satellite and/or ground-based observations of aerosol optical thickness (AOT), the most widely available and evaluated aerosol parameter. The ICAP models are independent in their underlying meteorology, as well as aerosol sources, sinks, microphysics and chemistry. The diversity of aerosol representations in the aerosol forecast models results in differences in AOT. In addition, for models that include AOT assimilations, the diversity in assimilation methodology, the observed AOT data to be assimilated, and the pre-assimilation treatments of input data also leads to differences in the AOT analyses. Drawing from members of the ICAP latest generation of quasi-operational aerosol models, five day AOT forecasts and AOT analyses are analyzed from four multi-species models which have AOT assimilations: ECMWF, JMA, NASA GSFC/GMAO, and NRL/FNMOC. For forecast mode only, we also include the dust products from NOAA NGAC, BSC, and UK Met office in our analysis leading to a total of 7 dust models. AOT at 550nm from all models are validated at regionally representative Aerosol Robotic Network (AERONET) sites and a data assimilation grade multi-satellite aerosol analysis. These analyses are also compared with the recently developed AOT reanalysis at NRL. Here we will present the basic verification characteristics of the ICAP-MME, and identify regions of diversity between model analyses and forecasts. Notably, as in many other ensemble environments, the multi model ensemble consensus mean outperforms all of the

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

  1. Radiative Effects of Carbonaceous and Inorganic Aerosols over California during CalNex and CARES: Observations versus Model Predictions

    NASA Astrophysics Data System (ADS)

    Vinoj, V.; Fast, J. D.; Liu, Y.

    2012-12-01

    Aerosols have been identified to be a major contributor to the uncertainty in understanding the present climate. Most of this uncertainty arises due to the lack of knowledge of their micro-physical and chemical properties as well as how to adequately represent their spatial and temporal distributions. Increased process level understanding can be achieved through carefully designed field campaigns and experiments. These measurements can be used to elucidate the aerosol properties, mixing, transport and transformation within the atmosphere and also to validate and improve models that include meteorology-aerosol-chemistry interactions. In the present study, the WRF-Chem model is used to simulate the evolution of carbonaceous and inorganic aerosols and their impact on radiation during May and June of 2010 over California when two field campaigns took place: the California Nexus Experiment (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES). We merged CalNex and CARES data along with data from operational networks such as, California Air Resources Board (CARB's) air quality monitoring network, the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, the AErosol RObotic NETwork (AERONET), and satellites into a common dataset for the Aerosol Modeling Test bed. The resulting combined dataset is used to rigorously evaluate the model simulation of aerosol mass, size distribution, composition, and optical properties needed to understand uncertainties that could affect regional variations in aerosol radiative forcing. The model reproduced many of the diurnal, multi-day, and spatial variations of aerosols as seen in the measurements. However, regionally the performance varied with reasonably good agreement with observations around Los Angeles and Sacramento and poor agreement with observations in the vicinity of Bakersfield (although predictions aloft were much better). Some aerosol species (sulfate and nitrate) were better represented

  2. Holistic aerosol evaluation using synthesized aerosol aircraft measurements

    NASA Astrophysics Data System (ADS)

    Watson-Parris, Duncan; Reddington, Carly; Schutgens, Nick; Stier, Philip; Carslaw, Ken; Liu, Dantong; Allan, James; Coe, Hugh

    2016-04-01

    Despite ongoing efforts there are still large uncertainties in aerosol concentrations and loadings across many commonly used GCMs. This in turn leads to large uncertainties in the contributions of the direct and indirect aerosol forcing on climate. However, constraining these fields using earth observation data, although providing global coverage, is problematic for many reasons, including the large uncertainties in retrieving aerosol loadings. Additionally, the inability to retrieve aerosols in or around cloudy scenes leads to further sampling biases (Gryspeerdt 2015). Many in-situ studies have used regional datasets to attempt to evaluate the model uncertainties, but these are unable to provide an assessment of the models ability to represent aerosols properties on a global scale. Within the Global Aerosol Synthesis and Science Project (GASSP) we have assembled the largest collection of quality controlled, in-situ aircraft observations ever synthesized to a consistent format. This provides a global set of in-situ measurements of Cloud Condensation Nuclei (CCN) and Black Carbon (BC), amongst others. In particular, the large number of vertical profiles provided by this aircraft data allows us to investigate the vertical structure of aerosols across a wide range of regions and environments. These vertical distributions are particularly valuable when investigating the dominant processes above or below clouds where remote sensing data is not available. Here we present initial process-based assessments of the BC lifetimes and vertical distributions of CCN in the HadGEM-UKCA and ECHAM-HAM models using this data. We use point-by-point based comparisons to avoid the sampling issues associated with comparing spatio-temporal aggregations.

  3. Analysis of Anions in Ambient Aerosols by Microchip Capillary Electrophoresis

    SciTech Connect

    Liu, Yan; MacDonald, David A.; Yu, Xiao-Ying; Hering, Susanne V.; Collett, Jeffrey L.; Henry, Charles S.

    2006-10-01

    We describe a microchip capillary electrophoresis method for the analysis of nitrate and sulfate in ambient aerosols. Investigating the chemical composition of ambient aerosol particles is essential for understanding their sources and effects. Significant progress has been made towards developing mass spectrometry-based instrumentation for rapid qualitative analysis of aerosols. Alternative methods for rapid quantification of selected high abundance compounds are needed to augment the capacity for widespread routine analysis. Such methods could provide much higher temporal and spatial resolution than can be achieved currently. Inorganic anions comprise a large percentage of particulate mass with nitrate and sulfate among the most abundant species. While ion chromatography has proven very useful for analyzing extracts of time-integrated ambient aerosol samples collected on filters and for semi-continuous, on-line particle composition measurements, there is a growing need for development of new compact, inexpensive approaches to routine on-line aerosol ion analysis for deployment in spatially dense, atmospheric measurement networks. Microchip capillary electrophoresis provides the necessary speed and portability to address this need. In this report, on-column contact conductivity detection is used with hydrodynamic injection to create a simple microchip instrument for analysis of nitrate and sulfate. On-column contact conductivity detection was achieved using a Pd decoupler placed upstream from the working electrodes. Microchips containing two Au or Pd working electrodes showed a good linear range (5-500 µM) and low limits-of-detection for sulfate and nitrate with Au providing the lowest detection limits (1 µM) for both ions. The completed microchip system was used to analyze ambient aerosol filter samples. Nitrate and sulfate concentrations measured by the microchip matched the concentrations measured by ion chromatography.

  4. Reactions and mass spectra of complex particles using Aerosol CIMS

    NASA Astrophysics Data System (ADS)

    Hearn, John D.; Smith, Geoffrey D.

    2006-12-01

    Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

  5. Sarychev Volcanic Aerosol and Chemical measurements over Eureka, Canada

    NASA Astrophysics Data System (ADS)

    Perro, C. W.; Duck, T. J.; Bitar, L.; Nott, G. J.; Lesins, G. B.; O'Neill, N. T.; Eloranta, E.; Strong, K.; Carn, S. A.; Lindenmaier, R.; Batchelor, R.; Saha, A.; Pike-Thackray, C.; Drummond, J. R.

    2010-12-01

    On July 01, 2009, lidar measurements from Eureka, Canada (80°N, 85°W) detected unusually high amounts of aerosol in the lower stratosphere which are believed to have originated from the Sarychev Eruption on the Kuril Islands in Russia (48°N,153°E). The suite of instruments that are part of the Canadian Network for the Detection of Atmospheric Change (CANDAC) have been used to measure the optical and chemical properties of the volcanic plume over Eureka. Lidar measurements show significant structure in the stratospheric aerosol that reaches altitudes of approximately 17 km. Initially there were several layers of aerosol in the lower stratosphere, which began to mix vertically so that by the end of August the aerosol was mixed into one homogeneous layer in the lower stratosphere. Lidar and sun photometer measurements are used to track the change in the integrated volume backscatter cross section from July 2009, with an initial peak value of 0.007 sr-1 until March 2010 when values have returned to background levels. Lidar measurements also show the plume descending over time. Satellite data from OMI and CALIPSO are used to track the SO2 and aerosols in the plume as it travels from the Kuril Islands to Eureka. Ground based measurements from a UV-VIS Spectrophotometer detected SO2 that correlated with OMI measurements over Eureka on July 01. A fourier transform spectrometer was used to monitor a number of chemical species in the UTLS region with HCL for example spiking during the same period. Effects of the stratospheric aerosols on the incoming short wave radiation during the summer months are also examined.

  6. Test-Aerosol Generator For Calibrating Particle Counters

    NASA Technical Reports Server (NTRS)

    Mogan, Paul A.; Adams, Alois J.; Schwindt, Christian J.; Hodge, Timothy R.; Mallow, Tim J.; Duong, Anh A.; Bukauskas, Vyto V.

    1996-01-01

    Apparatus generates clean, stable aerosol stream for use in testing and calibrating laser-based aerosol-particle counter. Size and concentration of aerosol particles controlled to ensure accurate calibration. Cheap, widely available medical nebulizers used to generate aerosols.

  7. Are anthropogenic aerosols affecting rainfall?

    NASA Astrophysics Data System (ADS)

    Junkermann, Wolfgang; Hacker, Jorg

    2013-04-01

    Modification of cloud microphysics by anthropogenic aerosols is well known since several decades. Whether the underlying processes leads to changes in precipitation is by far less confirmed. Several different factors affect the production of rain in a way that a causality between increasing aerosol load in the atmosphere and a change of annual rainfall is very difficult to confirm. What would be expected as an effect of additional cloud condensation nuclei is a shift in the spatial and temporal rainfall distribution towards a lower number of days with low rain intensity and more frequent or more vigorous single events. In fact such a shift has been observed in several locations worldwide and has been suggested to be caused by increasing aerosol load, however, without further specification of the nature and number of the aerosols involved. Measurements of aerosols which might be important for cloud properties are extremely sparse and no long term monitoring data sets are available up to now. The problem of missing long term aerosol data that could be compared to available long term meteorological data sets can possibly be resolved in certain areas where well characterized large anthropogenic aerosol sources were installed in otherwise pristine areas without significant changes in land use over several decades. We investigated aerosol sources and current aerosol number, size and spatial distributions with airborne measurements in the planetary boundary layer over two regions in Australia that are reported to suffer from extensive drought despite the fact that local to regional scale water vapor in the atmosphere is slowly and constantly increasing. Such an increase of the total water in the planetary boundary layer would imply also an increase in annual precipitation as observed in many other locations elsewhere. The observed decline of rainfall in these areas thus requires a local to regional scale physical process modifying cloud properties in a way that rain

  8. Hydrogen bonding at the aerosol interface

    SciTech Connect

    Zhang, J.X.; Aiello, D.; Aker, P.M. )

    1995-01-12

    Morphology-dependent stimulated Raman scattering (MDSRS) has been used to monitor the degree of hydrogen bonding in water aerosols generated by a vibrating orifice aerosol generator (VOAG). The results show that aerosols created by a VOAG suffer extensive structural disruption and that the disruption is most pronounced at the aerosol surface. Laboratory aerosols prepared in this way do not appropriately mimic those found in the atmosphere, and the mass accommodation coefficients measured using such aerosols should not be used in global climate modeling calculations. 25 refs., 10 figs.

  9. Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module

    NASA Astrophysics Data System (ADS)

    Andersson, Emma; Kahnert, Michael

    2016-05-01

    A new aerosol-optics model is implemented in which realistic morphologies and mixing states are assumed, especially for black carbon particles. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey-shell" model. Simulated results of aerosol optical properties, such as aerosol optical depth, backscattering coefficients and the Ångström exponent, as well as radiative fluxes are computed with the new optics model and compared with results from an older optics-model version that treats all particles as externally mixed homogeneous spheres. The results show that using a more detailed description of particle morphology and mixing state impacts the aerosol optical properties to a degree of the same order of magnitude as the effects of aerosol-microphysical processes. For instance, the aerosol optical depth computed for two cases in 2007 shows a relative difference between the two optics models that varies over the European region between -28 and 18 %, while the differences caused by the inclusion or omission of the aerosol-microphysical processes range from -50 to 37 %. This is an important finding, suggesting that a simple optics model coupled to a chemical transport model can introduce considerable errors affecting radiative fluxes in chemistry-climate models, compromising comparisons of model results with remote sensing observations of aerosols, and impeding the assimilation of satellite products for aerosols into chemical-transport models.

  10. Toward new techniques to measure heterogeneous oxidation of aerosol: Electrodynamic Balance-Mass Spectrometry (EDB-MS) and Aerosol X-ray Photoelectron Spectroscopy

    NASA Astrophysics Data System (ADS)

    Jacobs, M. I.; Heine, N.; Xu, B.; Davies, J. F.; Kirk, B. B.; Kostko, O.; Alayoglu, S.; Wilson, K. R.; Ahmed, M.

    2015-12-01

    The chemical composition and physical properties of aerosol can be changed via heterogeneous oxidation with the OH radical. However, the physical state of the aerosol influences the kinetics of this reaction; liquid particles with a high diffusion coefficient are expected to be well mixed and homogenously oxidized, while oxidation of solid, diffusion-limited aerosol is expected to occur primarily on the surface, creating steep chemical gradients within the particle. We are working to develop several new techniques to study the heterogeneous oxidation of different types of aerosol. We are developing a "modular" electrodynamic balance (EDB) that will enable us to study heterogeneous oxidation at aqueous interfaces using a mass-spectrometer (and potentially other detection techniques). Using a direct analysis in real time (DART) interface, preliminary droplet train measurements have demonstrated single-droplet mass spectrometry to be possible. With long reaction times in our EDB, we will be able to study heterogeneous oxidation of a wide variety of organic species in aqueous droplets. Additionally, we are working to use aerosol photoemission and velocity map imaging (VMI) to study the surface of aerosol particles as they undergo heterogeneous oxidation. With VMI, we're able to collect electrons with a 4π collection efficiency over conventional electron energy analyzers. Preliminary results looking at the ozonolysis of squalene using ultraviolet photoelectron spectroscopy (UPS) show that heterogeneous oxidation kinetic data can be extracted from photoelectron spectra. By moving to X-ray photoemission spectroscopy (XPS), we will determine elemental and chemical composition of the aerosol surface. Thus, aerosol XPS will provide information on the steep chemical gradients that form as diffusion-limited aerosol undergo heterogeneous oxidation.

  11. The Effect of Aerosol Formation on Stable Isotopes Ratio in Titan's Atmosphere

    NASA Astrophysics Data System (ADS)

    Gautier, Thomas; Trainer, Melissa G.; Sebree, Joshua; Wold, Allison; Stern, Jennifer

    2016-10-01

    The formation of large amounts of aerosol in Titan atmosphere induces a significant sink for carbon and nitrogen in the atmosphere. Due to the high complexity of the chemistry leading to aerosol formation, there may be isotopic fractionation along the formation pathways of the aerosol. So far several stable isotopes have been measured in Titan atmosphere including the 13C/12C, 15N/14N and D/H ratios for different gaseous species. However, the fractionation effect of the aerosol formation and its impact on atmospheric stable isotope ratios has yet to be fully understood. Two experimental studies were recently published on the stable carbon [1] and nitrogen [1,2] isotope fractionation during aerosol formation in N2-CH4 reactant mixture. To better constrain the fractionation effect of aerosol formation on the Titan atmosphere we have measured the isotopic fractionation induced in laboratory aerosol analogues produced exploring the space of parameters that are expected to have an effect on fractionation processes. Parameters studied include pressure and temperature of aerosol formation and the reactant gas phase composition, including the standard "Titan" mixture of CH4/N2 as well as other trace species such as benzene (C6H6).[1] Sebree, J.A., Stern, J.C., Mandt, K.E., Domagal-Goldman, S.D., and Trainer, M.G.: C and N Fractionation of CH /N Mixtures during Photochemical Aerosol Formation: Relevance to Titan, (2016) Icarus 270:421-428[2] Kuga, M., Carrasco, N., Marty, B., Marrochi, Y., Bernard, S., Rigaudier, T., Fleury, B., Tissandier, L.: Nitrogen isotopic fractionation during abiotic synthesis of organic solid particles, (2014) EPSL 393:2-13

  12. Organics Substantially Reduce HO2 Uptake onto Aerosols Containing Transition Metal ions.

    PubMed

    Lakey, Pascale S J; George, Ingrid J; Baeza-Romero, Maria T; Whalley, Lisa K; Heard, Dwayne E

    2016-03-10

    A HO2 mass accommodation coefficient of α = 0.23 ± 0.07 was measured onto submicron copper(II)-doped ammonium sulfate aerosols at a relative humidity of 60 ± 3%, at 293 ± 2 K and at an initial HO2 concentration of ∼ 1 × 10(9) molecules cm(-3) by using an aerosol flow tube coupled to a sensitive fluorescence assay by gas expansion (FAGE) HO2 detection system. The effect upon the HO2 uptake coefficient γ of adding different organic species (malonic acid, citric acid, 1,2-diaminoethane, tartronic acid, ethylenediaminetetraacetic acid (EDTA), and oxalic acid) into the copper(II)-doped aerosols was investigated. The HO2 uptake coefficient decreased steadily from the mass accommodation value to γ = 0.008 ± 0.009 when EDTA was added in a one-to-one molar ratio with the copper(II) ions, and to γ = 0.003 ± 0.004 when oxalic acid was added into the aerosol in a ten-to-one molar ratio with the copper(II). EDTA binds strongly to copper(II) ions, potentially making them unavailable for catalytic destruction of HO2, and could also be acting as a surfactant or changing the viscosity of the aerosol. The addition of oxalic acid to the aerosol potentially forms low-volatility copper-oxalate complexes that reduce the uptake of HO2 either by changing the viscosity of the aerosol or by causing precipitation out of the aerosol forming a coating. It is likely that there is a high enough oxalate to copper(II) ion ratio in many types of atmospheric aerosols to decrease the HO2 uptake coefficient. No observable change in the HO2 uptake coefficient was measured when the other organic species (malonic acid, citric acid, 1,2-diaminoethane, and tartronic acid) were added in a ten-to-one molar ratio with the copper(II) ions.

  13. 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

  14. The Amazon tall tower observatory (ATTO) site - Multi-year aerosol observations and scientific key questions

    NASA Astrophysics Data System (ADS)

    Pöhlker, C.; Barbosa, H. M.; Brito, J.; Carbone, S.; Chi, X.; Kesselmeier, J.; Ditas, F.; Pöhlker, M. L.; Manzi, A. O.; Moran, D.; Poeschl, U.; Ruckteschler, N.; Saturno, J.; Soergel, M.; Su, H.; Walter, D.; Wang, Q.; Wang, Z.; Weber, B.; Wolff, S.; Yanez-Serrano, A. M.; Artaxo, P.; Andreae, M. O.

    2015-12-01

    The Amazon tall tower observatory site is located 150 km NE of Manaus in undisturbed rain forest areas. It serves as a remote measurement station in the Amazon forest with continuous aerosol, trace gas, micrometeorological, and ecological measurements. During part of the rainy season, the atmospheric state approximates pre-industrial conditions, in strong contrast to the dry season, which is dominated by significant pollution from deforestation fires and urban emissions. This presentation will focus on aerosol studies of the past three years. It aims to provide a brief overview of the characteristic seasonality of the aerosol burden at the ATTO site. Moreover, it will discuss the following key questions and current results of the ongoing observations: (i) During the wet season and in the absence of long-range advection of African aerosols, atmospheric conditions at the ATTO site approximate a pristine state, which reveals the genuine contribution of biogenic aerosols. Biogenic particles in the super- and submicron range have been observed and their properties as well as potential sources will be discussed. (ii) In contrast to the classical new particle formation, the occurrence of ultrafine particles is comparably sparse and mainly occurs as short 'bursts', indicating a rather localized character. Our current understanding of this phenomenon and its significance for the overall aerosol burden will be addressed. (iii) Aerosol absorptivity is mainly caused by black carbon, however, indications for the presence of other light absorbing aerosol species have been found. Current results on light absorbing aerosol under clean and polluted conditions will be presented. (iv) Aerosol particles at the ATTO site are typically strongly aged and comprise pronounced internal mixtures, with important implications for their properties. Microspectroscopic analysis helps to obtain insights into atmospheric processing and its impact on particle morphology and phase state.

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

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, Ph.; Platt, U.; Zetzsch, C.

    2012-07-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS, released from simulated natural halogen sources like salt pans. Subsequently, the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which results in new functional groups (FTIR spectroscopy), changes UV/VIS absorption, chemical composition (ultrahigh resolution mass spectroscopy (ICR-FT/MS)), or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  16. Resuspension of Aerosol Particles from Evaporated Rain Drops to the Coarse Mode

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Ganguly, D.; Singh, B.; Rasch, P. J.

    2015-12-01

    Precipitation scavenging (i.e., wet removal) has long been recognized as one of the major removal processes for tropospheric aerosol particles, and the dominant one for accumulation-mode size particles. When rain drops evaporate, the aerosol material contained in drops is resuspended, and this process has received much less attention. Unlike the resuspension from evaporated cloud droplets, the aerosol particles resuspended from evaporated rain drops have much larger sizes than most of the aerosol particles that acted as cloud condensation nuclei (CCN), became cloud borne, and then were collected by rain drops, because each rain drop generally collects thousands of cloud droplets. Here we present some aspects of this resuspension process obtained from modeling studies. First, we investigate some details of the process using a simple drop-size resolved model of raindrop evaporation in sub-saturated air below cloud base. Using these results, we then investigate different treatments of this process in a global aerosol and climate model that employs a modal aerosol representation. Compared to the model's original treatment of this process in which rain-borne aerosol is resuspended to the mode that it came from with its original size, the new treatment that resuspends to the coarse mode produces notable reductions in global CCN concentrations, as well as sulfate, black carbon, and organic aerosol mass, because the resuspended aerosol particles have much shorter lifetimes due to their larger sizes. Somewhat surprisingly, there are also notable reductions in coarse-mode sea salt and mineral dust burdens. These species are resuspended to the coarse mode in both the original and new treatments, but these resuspended particles are fewer in number and larger in size in the new treatment. This finding highlights some issues of the modal aerosol treatment for coarse mode particles.

  17. Characterizing interactions between aerosols and cloud droplets in marine boundary layer clouds

    NASA Astrophysics Data System (ADS)

    Andersen, Hendrik; Cermak, Jan

    2016-04-01

    This contribution presents a method to characterize the nonlinearities of interactions between aerosols and cloud droplets in marine boundary layer clouds based on global MODIS observations. Clouds play a crucial role in the climate system as their radiative properties and precipitation patterns significantly impact the Earth's energy balance. Cloud properties are determined by environmental conditions, as cloud formation requires the availability of water vapour ("precipitable water") and condensation nuclei in sufficiently saturated conditions. The ways in which aerosols as condensation nuclei in particular influence the optical, micro- and macrophysical properties of clouds are one of the largest remaining uncertainties in climate-change research. In particular, cloud droplet size is believed to be impacted, and thereby cloud reflectivity, lifetime, and precipitation susceptibility. However, the connection between aerosols and cloud droplets is nonlinear, due to various factors and processes. The impact of aerosols on cloud properties is thought to be strongest with low aerosol loadings, whereas it saturates with high aerosol loadings. To gain understanding of the processes that govern low cloud water properties in order to increase accuracy of climate models and predictions of future changes in the climate system is thus of great importance. In this study, global Terra MODIS L3 data sets are used to characterize the nonlinearities of the interactions between aerosols and cloud droplets in marine boundary layer clouds. MODIS observations are binned in classes of aerosol loading to identify at what loading aerosol impact on cloud droplets is the strongest and at which loading it saturates. Results are connected to ERA-Interim and MACC data sets to identify connections of detected patterns to meteorology and aerosol species.

  18. 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.

  19. Toward a Minimal Representation of Aerosols in Climate Models: Comparative Decomposition of Aerosol Direct, Semidirect, and Indirect Radiative Forcing

    SciTech Connect

    Ghan, Steven J.; Liu, Xiaohong; Easter, Richard C.; Zaveri, Rahul A.; Rasch, Philip J.; Yoon, Jin-Ho; Eaton, Brian

    2012-10-01

    The authors have decomposed the anthropogenic aerosol radiative forcing into direct contributions from each aerosol species to the planetary energy balance through absorption and scattering of solar radiation, indirect effects of anthropogenic aerosol on solar and infrared radiation through droplet and crystal nucleation on aerosol, and semidirect effects through the influence of solar absorption on the distribution of clouds. A three-mode representation of the aerosol in version 5.1 of the Community Atmosphere Model (CAM5.1) yields global annual mean radiative forcing estimates for each of these forcing mechanisms that are within 0.1 W m–2 of estimates using a more complex seven-mode representation that distinguishes between fresh and aged black carbon and primary organic matter. Simulating fresh black carbon particles separately from internally mixed accumulation mode particles is found to be important only near fossil fuel sources. In addition to the usual large indirect effect on solar radiation, this study finds an unexpectedly large positive longwave indirect effect (because of enhanced cirrus produced by homogenous nucleation of ice crystals on anthropogenic sulfate), small shortwave and longwave semidirect effects, and a small direct effect (because of cancelation and interactions of direct effects of black carbon and sulfate). Differences between the threemode and seven-mode versions are significantly larger (up to 0.2 W m–2) when the hygroscopicity of primary organic matter is decreased from 0.1 to 0 and transfer of the primary carbonaceous aerosol to the accumulation mode in the seven-mode version requires more hygroscopic material coating the primary particles. Radiative forcing by cloudborne anthropogenic black carbon is only 20.07 W m–2.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  1. Speciation of arsenic in ambient aerosols collected in Los Angeles.

    PubMed

    Rabano, E S; Castillo, N T; Torre, K J; Solomon, P A

    1989-01-01

    First-time measurements of the potentially toxic inorganic species of arsenic (arsenite and arsenate) have been obtained in fine (less than 2.5 microns AD) and coarse (greater than 2.5 microns AD) atmospheric particles in the Los Angeles area. A recently developed method that includes procedures for sample collection, preparation, and analysis was used in this study. Size-fractionated aerosol samples were collected with a high-volume dichotomous virtual impactor that employed polytetrafluoroethylene filters. Results were obtained for the recovery of arsenic standards added to unexposed and collected filters. Data from this study, indicated that the recently developed speciation method can be used to determine concentrations of As(III) and As(V) in atmospheric particulate matter samples. Size-fractionated aerosol samples were collected in the city of Industry during January and February 1987. In most samples, As(III) and As(V) were above the detection limit (approximately 1 ng m-3 of either species) in both aerosol size fractions. A greater portion (about 75 percent) of the two species were observed in the fine particles. The As(III)/As(V) ratio for both particle sizes was close to 1 (i.e., an equal mixture of both species). Comparison of total suspended particulate arsenic measured by the speciation method to that measured by a routine California Air Resources Board-approved procedure showed good agreement (r = 0.94), indicating both methods were approximately equivalent for the collection and analysis of aerosol arsenic. PMID:2709077

  2. Climate-aerosol interactions over the Mediterranean region: a regional coupled modelling approach

    NASA Astrophysics Data System (ADS)

    Nabat, Pierre; Somot, Samuel; Mallet, Marc

    2015-04-01

    The Mediterranean basin is affected by numerous and various aerosols which have a high spatio-temporal variability. These aerosols directly interact with solar and thermal radiation, and indirectly with clouds and atmospheric dynamics. Therefore they can have an important impact on the regional climate. This work, located at the boundary between the ChArMEx and HyMeX programs, considers a coupled regional modeling approach in order to address the questions of the aerosol-radiation-cloud interactions with regards to the climate variability over the Mediterranean. In order to improve the characterization of Mediterranean aerosols, a new interannual monthly climatology of aerosol optical depth has been developed from a blended product based on both satellite-derived and model-simulated datasets. This dataset, available for every regional climate model over the Mediterranean for the 1979-2012 period, has been built to obtain the best possible estimate of the atmospheric aerosol content for the five species at stake (sulfate, black carbon, organic matter, desert dust and sea salt particles). Simulation ensembles, which have been carried out over the 2003-2009 period with and without aerosols, show a major impact on the regional climate. The seasonal cycle and the spatial patterns of the Mediterranean climate are significantly modified, as well as some specific situations such as the heat wave in July 2006 strengthened by the presence of desert dust particles. The essential role of the Mediterranean sea surface temperature is highlighted, and enables to understand the induced changes on air-sea fluxes and the consequences on regional climate. Oceanic convection is also strengthened by aerosols. In addition, the decrease in anthropogenic aerosols observed for more than thirty years is shown to significantly contribute to the observed Euro-Mediterranean climatic trends in terms of surface radiation and temperature. Besides, an interactive aerosol scheme has been developed

  3. Simulations of aerosols and their effects on photolysis and ozone formation in Mexico City

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

    Atmospheric aerosols, formed from natural and anthropogenic sources, are believed to be associated with adverse human effects at high levels in polluted urban areas. They also play a key role in climate through direct and indirect effects. Therefore, accurate simulations of aerosol composition and distribution in the atmospheric models are important in evaluating their impact on environment and climate. In the present study, a flexible gas phase chemical module with SAPRC mechanism and the CMAQ/models3 aerosol module developed by EPA have been implemented into the WRF-CHEM model. Additionally, to further improve the aerosol, especially the secondary organic aerosol (SOA) simulations, an advanced SOA module [Tsimpidi et al., 2009] has been incorporated into the WRF-CHEM model. The new SOA module is based on the volatility basis-set approach in which both primary and secondary organic components are assumed to be semivolatile and photochemically reactive [Lane et al., 2008]. Gas phase species and aerosol simulation results are compared with the available measurements obtained during the MILAGRO 2006 campaign. When the advanced SOA mechanism is employed, the SOA simulations are significantly improved. Furthermore, the aerosol impacts on the photochemistry in Mexico City have been evaluated using the FTUV [Tie et al., 2005]. Aerosol optical properties are calculated using the Mie theory and compared with available observations in Mexico City [Paredes-Miranda et al., 2008]. Aerosols, principally black carbon, reduce the photolysis frequencies of J[O3(1D)] and J[NO2] in the planetary boundary layer and hence decrease the ground-level ozone concentration. Our study demonstrates that the impact of aerosols on photochemistry is significant in polluted urban atmosphere. References: Lane, T. E., N. M. Donahue, and S. N. Pandis (2008), Simulating secondary organic aerosol formation using the volatility basis-set approach in a chemical transport model, PMCAMx, Atmos. Environ

  4. Impact of Asian Aerosols on Precipitation Over California: An Observational and Model Based Approach

    NASA Technical Reports Server (NTRS)

    Naeger, Aaron R.; Molthan, Andrew L.; Zavodsky, Bradley T.; Creamean, Jessie M.

    2015-01-01

    -Chem model simulations. After validating the capability of the WRF-Chem in realistically simulating the aerosol-cloud precipitation interactions, we conduct sensitivity studies where the AOD is doubled to diagnose whether an increasing concentration of Asian aerosols over the western United States will lead to further impacts on the cloud and precipitation processes over California. We also perform sensitivity studies where the aerosols will be partitioned into dust-only and pollution-only in order to separate the impacts of the differing Asian aerosol species. The results of our WRF-Chem model simulations aim to show that the trans-Pacific transport of Asian aerosols influence the precipitation associated with atmospheric river events that can ultimately impact the regional climate of the western United States. 1 University

  5. Exploration of the link between Emiliania huxleyi bloom dynamics and aerosol fluxes to the lower Atmosphere

    NASA Astrophysics Data System (ADS)

    Trainic, M.

    2013-12-01

    Phytoplankton blooms are responsible for about 50% of the global photosynthesis, thus are a key component of the major nutrient cycles in the ocean. These blooms can be a significant source for flux of volatiles and aerosols, affecting physical chemical processes in the atmosphere. One of the most widely distributed and abundant phytoplankton species in the oceans is the coccolithophore Emiliania huxleyi. In this research, we explore the influence of the different stages of E. huxleyi bloom on the emission of primary aerosols. For this purpose, we conducted a series of controlled lab experiments to measure aerosol emissions during the growth of E. huxleyi. The cultures were grown in a specially designed growth chamber, and the aerosols were generated in a bubbling system. We collected the emitted aerosol particles on filters, and conducted a series of analysis. Scanning electron microscopy (SEM) analysis of the aerosols emitted from E.huxleyi 1216 cultures demonstrate emission of CaCO3 platelets from their exoskeleton into the air, while coccolithophores cells were absent. The results suggest that while healthy coccolithophore cells are too heavy to aerosolize, during cell lysis the coccoliths shed from the coccolithophore cells are emitted into the atmosphere. Therefore, aerosol production during bloom demise may be greater than from healthy E.huxleyi populations. We also investigated the size distribution of the aerosols at various stages of E. huxleyi growth. The presence of calcified cells greatly effects the size distribution of the emitted aerosol population. This work motivated us to explore aerosols emitted during E. huxleyi spring bloom, in a laboratory we constructed onboard the R/V Knorr research vessel, as part of the North Atlantic Virus Infection of Coccolithophore Expedition (June-July 2012). These results have far-reaching implications on the effect of E. huxleyi bloom dynamics on aerosol properties. We not only show that the E. huxleyi calcite

  6. YAG aerosol lidar

    NASA Technical Reports Server (NTRS)

    Sullivan, R.

    1988-01-01

    The Global Atmospheric Backscatter Experiment (GLOBE) Mission, using the NASA DC-8 aircraft platform, is designed to provide the magnitude and statistical distribution of atmospheric backscatter cross section at lidar operating wavelengths. This is a fundamental parameter required for the Doppler lidar proposed to be used on a spacecraft platform for global wind field measurements. The prime measurements will be made by a CO2 lidar instrument in the 9 to 10 micron range. These measurements will be complemented with the Goddard YAG Aerosol Lidar (YAL) data in two wavelengths, 0.532 and 1.06 micron, in the visible and near-infrared. The YAL, is being designed to utilize as much existing hardware, as feasible, to minimize cost and reduce implementation time. The laser, energy monitor, telescope and detector package will be mounted on an optical breadboard. The optical breadboard is mounted through isolation mounts between two low boy racks. The detector package will utilize a photomultiplier tube for the 0.532 micron channel and a silicon avalanche photo detector (APD) for the 1.06 micron channel.

  7. Aerosol measurements over the Pacific Ocean in support of the IR aerosol backscatter program

    NASA Technical Reports Server (NTRS)

    Prospero, Joseph M.; Savoie, Dennis L.

    1995-01-01

    The major efforts under NASA contract NAG8-841 included: (1) final analyses of the samples collected during the first GLOBE survey flight that occurred in November 1989 and collections and analysis of aerosol samples during the second GLOBE survey flight in May and June 1990. During the first GLOBE survey flight, daily samples were collected at four stations (Midway, Rarotonga, American Samoa, and Norfolk Island) throughout the month of November 1989. Weekly samples were collected at Shemya, Alaska, and at Karamea, New Zealand. During the second GLOBE survey flight, daily samples were collected at Midway, Oahu, American Samoa, Rarotonga, and Norfolk Island; weekly samples were collected at Shemya. These samples were all analyzed for sodium (sea-salt), chloride, nitrate, sulfate, and methanesulfonate at the University of Miami and for aluminum at the University of Rhode Island (under a subcontract). (2) Samples continued to be collected on a weekly basis at all stations during the periods between and after the survey flights. These weekly samples were also analyzed at the University of Miami for the suite of water-soluble species. (3) In August 1990, the results obtained from the above studies were submitted to the appropriate personnel at NASA Marshall Space Flight Center to become part of the GLOBE data base for comparison with data from instruments used aboard the aircraft. In addition, the data will be compared with data previously obtained at these stations as part of the Sea-Air Exchange (SEAREX) Program. This comparison will provide valuable information on the representativeness of the periods in terms of the longer term aerosol climatology over the Pacific Ocean. (4) Several publications have been written using data from this grant. The data will continue to be used in the future as part of a continuing investigation of the long-term trends and interannual variations in aerosol species concentrations over the Pacific Ocean.

  8. Aerosols, Chemistry, and Radiative Forcing: A 3-D Model Analysis of Satellite and ACE-Asia data (ACMAP)

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Torres, Omar; Zhao, Xue-Peng

    2005-01-01

    We propose a research project to incorporate a global 3-D model and satellite data into the multi-national Ae