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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. Seasonal characteristics of fine particulate matter (PM) based on high-resolution time-of-flight aerosol mass spectrometric (HR-ToF-AMS) measurements at the HKUST Supersite in Hong Kong

    NASA Astrophysics Data System (ADS)

    Li, Y. J.; Lee, B. P.; Su, L.; Fung, J. C. H.; Chan, C. K.

    2015-01-01

    Atmospheric particulate matter (PM) remains poorly understood due to the lack of comprehensive measurements at high time resolution for tracking its dynamic features and the lack of long-term observation for tracking its seasonal variability. Here, we present highly time-resolved and seasonal compositions and characteristics of non-refractory components in PM with a diameter less than 1 μm (NR-PM1) at a suburban site in Hong Kong. The measurements were made with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) at the Hong Kong University of Science and Technology (HKUST) Air Quality Research Supersite for 4 months, with one in each season of the year. The average NR-PM1 concentration of ~ 15 μg m-3 is higher than those AMS measurements made in South Korea and Japan, but lower than those in North China, the Yangtze River Delta and the nearby Pearl River Delta. The seasonal dependence of the total NR-PM1 monthly averaged concentrations was small, but that of the fractions of the species in NR-PM1 was significant. Site characteristic plays an important role in the relative fractions of species in NR-PM1 and our results are generally consistent with measurements at other non-urban sites in this regard. Detailed analyses were conducted on the AMS data in the aspects of (1) species concentrations, (2) size distributions, (3) degree of oxygenation of organics, and (4) positive matrix factorization (PMF)-resolved organic factors in a seasonal context, as well as with air mass origin from back-trajectory analysis. Sulfate had the highest fraction in NR-PM1 (> 40%), and the surrogates of secondary organic species - semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated organic aerosol (LVOOA) - prevailed (~ 80%) in the organic portion of NR-PM1. Local contributions to the organic portion of NR-PM1 at this suburban site was strongly dependent on season. The hydrocarbon-like organic aerosol (HOA) factor related to

  3. Seasonal characteristics of fine particulate matter (PM) based on high resolution time-of-flight aerosol mass spectrometric (HR-ToF-AMS) measurements at the HKUST Supersite in Hong Kong

    NASA Astrophysics Data System (ADS)

    Li, Y. J.; Lee, B. P.; Su, L.; Fung, J. C. H.; Chan, C. K.

    2014-08-01

    Atmospheric particulate matter (PM) remains poorly understood due to the lack of comprehensive measurements at high time resolution for tracking its dynamic features and the lack of long-term observation for tracking its seasonal variability. Here, we present highly time-resolved and seasonal compositions and characteristics of non-refractory components in PM with diameter less than 1 μm (NR-PM1) at a suburban site in Hong Kong. The measurements were made with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) at the Hong Kong University of Science and Technology (HKUST) Air Quality Research Supersite for four months, with one in each season of the year. The average NR-PM1 concentration of ~15 μg m-3 is higher than those AMS measurements made in South Korea and Japan, but lower than those in North China, the Yangtze River Delta and the nearby Pearl River Delta. The seasonal dependence of the total NR-PM1 monthly averaged concentrations was small but that of the fractions of the species in NR-PM1 was significant. Site characteristic plays an important role in the relative fractions of species in NR-PM1 and our results are generally consistent with measurements at other non-urban sites in this regard. Detailed analyses were conducted on the AMS data in the aspects of (1) species concentrations, (2) size distributions, (3) degree of oxygenation of organics, and (4) positive matrix factorization (PMF)-resolved organic factors in a seasonal context, as well as with air mass origin from back-trajectory analysis. Sulfate had the highest fraction in NR-PM1 (> 40%) and the surrogates of secondary organic species, semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated organic aerosol (LVOOA), prevailed (~80%) in the organic portion of NR-PM1. Local contributions to the organic portion of NR-PM1 at this suburban site was strongly dependent on season. The hydrocarbon-like organic aerosol (HOA) factor related to local

  4. Characterization of submicron aerosols during a month of serious pollution in Beijing, 2013

    NASA Astrophysics Data System (ADS)

    Zhang, J. K.; Sun, Y.; Liu, Z. R.; Ji, D. S.; Hu, B.; Liu, Q.; Wang, Y. S.

    2014-03-01

    In January 2013, Beijing experienced several serious haze events. To achieve a better understanding of the characteristics, sources and processes of aerosols during this month, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site between 1 January and 1 February 2013 to obtain the size-resolved chemical composition of non-refractory submicron particles (NR-PM1). During this period, the mean measured NR-PM1 mass concentration was 89.3 ± 85.6 μg m-3, and it peaked at 423 μg m-3. Positive matrix factorization (PMF) differentiated the organic aerosol into five components, including a highly oxidized, low-volatility oxygenated organic aerosol (LV-OOA), a less oxidized, semi-volatile oxygenated OA (SV-OOA), a coal combustion OA (CCOA), a cooking-related OA (COA), and a hydrocarbon-like OA (HOA), which on average accounted for 28%, 26%, 15%, 20% and 11% of the total organic mass, respectively. A detailed comparison between the polluted days and unpolluted days found many interesting results. First, the organic fraction was the most important NR-PM1 species during the unpolluted days (58%), while inorganic species were dominant on polluted days (59%). The OA composition also experienced a significant change; it was dominated by primary OA (POA), including COA, HOA and CCOA, on unpolluted days. The contribution of secondary OA (SOA) increased from 35% to 63% between unpolluted and polluted days. Second, meteorological effects played an important role in the heavy pollution in this month and differed significantly between the two types of days. The temperature and relative humidity (RH) were all increased on polluted days and the wind speed and air pressure were decreased. Third, the diurnal variation trend in NR-PM1 species and OA components showed some differences between the two types of days, and the OA was more highly oxidized on polluted days. Fourth, the effects of air masses were significantly different

  5. 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.

  6. 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.

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

    DOE PAGESBeta

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

    2015-04-01

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

  8. 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.

  9. Characterization of submicron aerosols during a serious pollution month in Beijing (2013) using an aerodyne high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, J. K.; Sun, Y.; Liu, Z. R.; Ji, D. S.; Hu, B.; Liu, Q.; Wang, Y. S.

    2013-07-01

    In January 2013, Beijing experienced several serious haze events. To achieve a better understanding of the characteristics, sources and processes of aerosols during this month, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at an urban site between 1 January and 1 February 2013 to obtain the size-resolved chemical composition of non-refractory submicron particles (NR-PM1). During this period, the mean measured NR-PM1 mass concentration was 87.4 μg m-3 and was composed of organics (49.8%), sulfate (21.4%), nitrate (14.6%), ammonium (10.4%), and chloride (3.8%). Moreover, inorganic matter, such as sulfate and nitrate comprised an increasing fraction of the NR-PM1 load as NR-PM1 loading increased, denoting their key roles in particulate pollution during this month. The average size distributions of the species were all dominated by an accumulation mode peaking at approximately 600 nm in vacuum aerodynamic diameter and organics characterized by an additional smaller size (∼200 nm). Elemental analyses showed that the average O/C, H/C, and N/C (molar ratio) of organic matter were 0.34, 1.44 and 0.015, respectively, corresponding to an OM/OC ratio (mass ratio of organic matter to organic carbon) of 1.60. Positive matrix factorization (PMF) analyses of the high-resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., oxygenated organic aerosols (OOA), cooking-related (COA), nitrogen-containing (NOA) and hydrocarbon-like (HOA), which on average accounted for 40.0, 23.4, 18.1 and 18.5% of the total organic mass, respectively. Back trajectory clustering analyses indicated that the WNW air masses were associated with the highest NR-PM1 pollution during the campaign. Aerosol particles in southern air masses were especially rich in inorganic and oxidized organic species, whereas northern air masses contained a large fraction of primary species.

  10. 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.

  11. 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

  12. 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

  13. 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

  14. 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

  15. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

    NASA Astrophysics Data System (ADS)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-08-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine

  16. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

    NASA Astrophysics Data System (ADS)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-11-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play

  17. Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

    NASA Astrophysics Data System (ADS)

    Hapsari Budisulistiorini, Sri; Baumann, Karsten; Edgerton, Eric S.; Bairai, Solomon T.; Mueller, Stephen; Shaw, Stephanie L.; Knipping, Eladio M.; Gold, Avram; Surratt, Jason D.

    2016-04-01

    A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA) and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 %) and sulfate (up to 31 %). Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), semi-volatile oxygenated OA (SV-OOA), low-volatility oxygenated OA (LV-OOA), isoprene-derived epoxydiols (IEPOX) OA (IEPOX-OA) and 91Fac (a factor dominated by a distinct ion at m/z 91 fragment ion previously observed in biogenic influenced areas). LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass). BBOA (15-33 % of OA mass) was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ˜ 27 %), it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27-41 %) of OA at both sites, particularly in spring and summer. An ion fragment at m/z 75 is well correlated with the m/z 82 ion associated with the aerosol mass spectrum of IEPOX-derived secondary organic aerosol (SOA). The

  18. 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.

  19. 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.

  20. 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

  1. Formation of highly oxygenated organic aerosol in the atmosphere: Insights from the Finokalia Aerosol Measurement Experiments

    NASA Astrophysics Data System (ADS)

    Hildebrandt, Lea; Kostenidou, Evangelia; Mihalopoulos, Nikos; Worsnop, Douglas R.; Donahue, Neil M.; Pandis, Spyros N.

    2010-12-01

    Aged organic aerosol (OA) was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiments (FAME-08 and FAME-09), which were part of the EUCAARI intensive campaigns. Quadrupole aerosol mass spectrometers (Q-AMSs) were employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM1), and to estimate the extent of oxidation of the OA. The experiments provide unique insights into ambient oxidation of aerosol by measuring at the same site but under different photochemical conditions. NR-PM1 concentrations were about a factor of three lower during FAME-09 (winter) than during FAME-08 (summer). The OA sampled was significantly less oxidized and more variable in composition during the winter than during the early summer. Lower OH concentrations in the winter were the main difference between the two campaigns, suggesting that atmospheric formation of highly oxygenated OA is associated with homogeneous photochemical aging.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

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

  7. 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

  8. 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

  9. 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...

  10. 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

  11. 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.

  12. 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

  13. 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

  14. Characteristics of submicron particulate matter at the urban roadside in downtown Hong Kong—Overview of 4 months of continuous high-resolution aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Lee, Berto P.; Li, Yong Jie; Yu, Jian Zhen; Louie, Peter K. K.; Chan, Chak K.

    2015-07-01

    Hong Kong, one of the world's most densely populated cities and an international financial center, has been suffering from traffic-related air pollution. This study presents the first real-time high-resolution aerosol mass spectrometry measurements of submicron nonrefractory particulate matter (NR-PM1) at the urban roadside in Hong Kong from March to July 2013 with the aim to identify major sources, to assess local and nonlocal emissions, and to characterize trends at different time scales. Organics were dominant, with fresh primary organic aerosol representing two thirds of the total measured organics. Cooking contributions in organic aerosol were assessed directly for the first time in Hong Kong and exceeded those related to vehicles although traffic was still the major PM1 source when elemental carbon was included. These findings were supported by additional measurements including traffic data, elemental/organic carbon, and VOC data. Springtime concentrations were about double of those in summer, due to a strong seasonal transition which affected meteorological conditions and street-level circulation. Local formation of secondary species was not clearly discernible in either season. The elemental composition of organic aerosol remained stable with similar elemental ratios across the covered seasons: OM/OC: 1.49 ± 0.13, O/C: 0.25 ± 0.10, H/C: 1.68 ± 0.08 for spring and OM/OC: 1.43 ± 0.14, O/C: 0.21 ± 0.11, H/C: 1.69 ± 0.08 for summer. Diurnal changes in H/C and O/C as a result of mixing of primary organic aerosol and secondary organic aerosol were evident in the van Krevelen plot.

  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. Reactive Oxygen Species in Combustion Aerosols

    NASA Astrophysics Data System (ADS)

    Balasubramanian, R.; See, S.

    2007-12-01

    Research on airborne particulate matter (PM) has received increased concern in recent years after it was identified as a major component of the air pollution mix that is strongly associated with premature mortality and morbidity. Particular attention has been paid to understanding the potential health impacts of fine particles (PM2.5), which primarily originate from combustion sources. One group of particulate-bound chemical components of health concern is reactive oxygen species (ROS), which include molecules such as hydrogen peroxide (H2O2), ions such as hypochlorite ion (OCl-), free radicals such as hydroxyl radical (·OH) and superoxide anion (·O2-) which is both an ion and a radical. However, the formation of ROS in PM is not clearly understood yet. Furthermore, the concentration of ROS in combustion particles of different origin has not been quantified. The primary objective of this work is to study the effect of transition metals on the production of ROS in PM2.5 by determining the concentrations of ROS and metals. Both soluble and total metals were measured to evaluate their respective associations with ROS. PM2.5 samples were collected from several outdoor and indoor combustion sources, including those emitted from on-road vehicles, food cooking, incense sticks, and cigarette smoke. PM2.5 samples were also collected from the background air in both the ambient outdoor and indoor environments to assess the levels of particulate-bound transition metals and ROS with no combustion activities in the vicinity of sampling locations. Results obtained from this comprehensive study on particulate-bound ROS will be presented and discussed.

  19. Real-time measurements of ambient aerosols in a polluted Indian city: Sources, characteristics, and processing of organic aerosols during foggy and nonfoggy periods

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Bhattu, Deepika; Gupta, Tarun; Tripathi, Sachchida N.; Canagaratna, Manjula R.

    2015-09-01

    A detailed time-resolved chemical characterization of ambient nonrefractory submicron aerosols (NR-PM1) was conducted for the first time in India. The measurements were performed during the winter (November 2011 to January 2012) in a heavily polluted city of Kanpur, which is situated in the Indo-Gangetic Plain. Real-time measurements provided new insights into the sources and evolution of organic aerosols (OA) that could not be obtained using previously deployed filter-based measurements at this site. The average NR-PM1 loading was very high (>100 µg/m3) throughout the study, with OA contributing approximately 70% of the total aerosol mass. Source apportionment of the OA using positive matrix factorization revealed large contributions from fresh and aged biomass burning OA throughout the entire study period. A back trajectory analysis showed that the polluted air masses were affected by local sources and distant source regions where the burning of paddy residues occurs annually during winter. Several fog episodes were encountered during the study, and the OA composition varied between foggy and nonfoggy periods, with higher oxygen to carbon (O/C) ratios during the foggy periods. The evolution of OA and their elemental ratios (O:C and H:C) were investigated for the possible effects of fog processing.

  20. 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

  1. Atmospheric Transformations of Chromium Species on Aerosol Nanoparticles

    NASA Astrophysics Data System (ADS)

    Werner, M.; Nico, P.; Guo, B.; Kennedy, I.; Anastasio, C.

    2003-12-01

    While nanoparticles can have adverse health effects, the reasons for this toxicity are unclear. One possible reason is that the particles can contain toxic metals such as chromium. Measurements of ambient aerosols in Los Angeles have shown that as particle size decreases, the concentration of chromium increases; chromium (Cr) accounts for up to 10% of the mass of the smallest diameter particles. Chromium exists in two major oxidation states: +3, which is an essential nutrient, and +6, which is highly toxic and carcinogenic. Currently little is known about what happens to the Cr(III)/Cr(VI) ratio in chromium nanoparticles during atmospheric transport. Because the atmosphere is oxidizing in nature, one might think that oxidation of Cr(III) to Cr(VI) would occur in the troposphere. However, there are many other chemical species in aerosol particles which could reduce Cr(VI) to Cr(III). Understanding whether these changes occur in the atmosphere is important because they could alter the toxicity of the particulate matter. The goal of this project is to determine how atmospheric aging of particles affects Cr speciation. To investigate this issue, we collected chromium and chromium/iron particles on Teflon filters from a combustion flame fed with hydrogen, argon, and Cr(CO)5 with and without a source of iron. The samples were cut in half and placed in a solar simulation chamber where they were exposed to sunlight, ozone, water vapor, and, in some cases, basic or acidic conditions. After the aging process, the aged and not aged samples were analyzed for Cr oxidation state using X-ray Absorption Near Edge Spectroscopy (XANES). In particles that had high initial Cr(VI)/Cr(total) ratios, the aging process reduced Cr(VI) by 20%. The Cr(VI)/Cr(total) ratio in fresh particles was reduced by 60% when Fe was added to the flame. Aging of these Cr/Fe particles resulted in an additional 60% reduction in the Cr(VI)/Cr(total) ratio. Particles that had low initial Cr

  2. 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.

  3. Characterizing Atmospheric Processing of Aerosols from Forest Fires at the Mt. Bachelor Observatory during BBOP

    NASA Astrophysics Data System (ADS)

    Zhou, S.; Collier, S.; Hee, J.; Wigder, N. L.; Jaffe, D. A.; Zhang, Q.

    2014-12-01

    This study investigates the physical and chemical characteristics and atmospheric processing of aerosols from uncontrolled forest fires across the Pacific Northwest. The measurements were made at the Mt. Bachelor Observatory (MBO) located at the summit of Mt. Bachelor in central Oregon (43.9794° N, 121.6885° W, 2,763 m asl) in summer 2013 during the DOE sponsored Biomass Burning Observation Project (BBOP) field campaign. We utilized an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) coupled with a thermodenuder. Observations during periods affected by biomass burning (BB) pollution showed elevated non-refractory submicron aerosol (NR-PM1) concentration up to 140 μg/m3. NR-PM1 correlated well with PM light scattering (up to ~ 600 Mm-1 at 550 nm) and gas phase CO (up to ~0.4 ppmv). The AMS BB tracer, f60, i.e., fraction of organic signals at m/z = 60, was also enhanced with a maximum of ~ 2%. Organic aerosol (OA) dominated the PM composition in BB plumes (94.1% of the NR-PM1 mass) with an average concentration of 13.9 μg/m3. Three distinctive BBOA factors were identified by Positive Matrix Factorization (PMF): a fresh BBOA-I factor (O/C=0.27, H/C=1.52, f60 = 2.26%) that correlates well with ammonium nitrate; an intermediately oxidized BBOA-II (O/C=0.52, H/C=1.47, f60 = 1.05%), and a highly oxidized BBOA-III (O/C=0.95, H/C=1.02) with a low f60 (< 0.01%) and enhanced tracer ions for carboxylic acids (e.g., CHO2+). During persistent BB plume events from fixed fire sources, fresh BBOA-I initially dominated the OA composition, but decreased as the more oxidized BBOA-II increased while BBOA-III remained unchanged. These events shed light on the chemical transformation of BB aerosol during atmospheric aging. We will examine the enhancement of different BBOA factors relative to CO to investigate secondary organic aerosol (SOA) formation processes in BB plumes.

  4. 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

  5. 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

  6. Time-of-flight aerosol mass spectrometry: Measuring gaseous iodine species after selective uptake in lab-generated aerosols

    NASA Astrophysics Data System (ADS)

    Kundel, Michael; Ries, Marco; Schott, Mathias; Hoffmann, Thorsten

    2010-05-01

    Reactive iodine species play an important role in the marine atmospheric chemistry. Recent studies show that iodine containing compounds (e.g. I2 and ICl) are involved in the tropospheric ozone depletion, the enrichment of iodine in marine aerosols and the formation of new particles in the marine boundary layer (MBL). Various laboratory and field measurements report that molecular iodine (I2) and organoiodine compounds (e.g. CH3I, CH2I2) are the most important precursors for reactive iodine in the MBL[1],[2]. However, the identification and quantification of reactive iodine containing compounds are still analytical challenges. Here, we present a new application of the time-of-flight aerosol mass spectrometer (ToF-AMS) for the quantification of gaseous I2 and ICl in real-time. Time-of-flight aerosol mass spectrometry enables the real-time analysis of the particle size, the particle mass and the chemical composition of non-refractory aerosols[3]. The aerosol enters the ToF-AMS through a critical orifice of 100 μm inner diameter. An aerodynamic lens system focuses the particles in a size range of 50-600 nm as a narrow beam into the vacuum system. While most of the air is removed by a skimmer, the particle beam is transmitted into the particle-sizing chamber. After passing the particle-sizing chamber, the non-refractory particles are flash-vaporized on a heated tungsten surface (500-600 °C) and then ionized by electron impact. The generated ions are extracted by an orthogonal extractor into the time-of-flight mass spectrometer, where the time resolved particle mass detection is performed. Since gaseous compounds are removed inside the ToF-AMS, a direct measurement of gaseous iodine species is not possible. Therefore gaseous iodine species have to be transferred from the gas phase to the particle phase before entering the ToF-AMS. For this purpose α-cyclodextrin (α-CD) particles were used as selective sampling probes for I2 and 1,3,5-trimethoxybenzene (1,3,5-TMB

  7. Detection of cw-related species in complex aerosol particles deposited on surfaces with an ion trap-based aerosol mass spectrometer

    SciTech Connect

    Harris, William A; Reilly, Pete; Whitten, William B

    2007-01-01

    A new type of aerosol mass spectrometer was developed by minimal modification of an existing commercial ion trap to analyze the semivolatile components of aerosols in real time. An aerodynamic lens-based inlet system created a well-collimated particle beam that impacted into the heated ionization volume of the commercial ion trap mass spectrometer. The semivolatile components of the aerosols were thermally vaporized and ionized by electron impact or chemical ionization in the source. The nascent ions were extracted and injected into the ion trap for mass analysis. The utility of this instrument was demonstrated by identifying semivolatile analytes in complex aerosols. This study is part of an ongoing effort to develop methods for identifying chemical species related to CW agent exposure. Our efforts focused on detection of CW-related species doped on omnipresent aerosols such as house dust particles vacuumed from various surfaces found in any office building. The doped aerosols were sampled directly into the inlet of our mass spectrometer from the vacuumed particle stream. The semivolatile analytes were deposited on house dust and identified by positive ion chemical ionization mass spectrometry up to 2.5 h after deposition. Our results suggest that the observed semivolatile species may have been chemisorbed on some of the particle surfaces in submonolayer concentrations and may remain hours after deposition. This research suggests that identification of trace CW agent-related species should be feasible by this technique.

  8. Modeling of photolysis rates over Europe: impact on chemical gaseous species and aerosols

    NASA Astrophysics Data System (ADS)

    Real, E.; Sartelet, K.

    2011-02-01

    This paper evaluates the impact of photolysis rate calculation on simulated European air composition and air quality. In particular, the impact of the cloud parametrisation and the impact of aerosols on photolysis rates are analysed. Photolysis rates are simulated using the Fast-JX photolysis scheme and gas and aerosol concentrations over Europe are simulated with the regional chemistry-transport model Polair3D of the Polyphemus platform. The photolysis scheme is first used to update the clear-sky tabulation of photolysis rates used in the previous Polair3D version. Important differences in photolysis rates are simulated, mainly due to updated cross-sections and quantum yields in the Fast-JX scheme. In the previous Polair3D version, clouds were taken into account by multiplying the clear-sky photolysis rates by a correction factor. In the new version, clouds are taken into account more accurately by simulating them directly in the photolysis scheme. Differences in photolysis rates inside clouds can be large but outside clouds, and especially at the ground, differences are small. To take into account the impact of aerosols on photolysis rates, Polair3D and Fast-JX are coupled. Photolysis rates are updated every hour. Large impact on photolysis rates is observed at the ground, decreasing with altitude. The aerosol specie that impact the most photolysis rates is dust especially in south Europe. Strong impact is also observed over anthropogenic emission regions (Paris, The Po and the Ruhr Valley) where mainly nitrate and sulphate reduce the incoming radiation. Differences in photolysis rates lead to changes in gas concentrations, with the largest impact simulated on OH and NO concentrations. At the ground, monthly mean concentrations of both species are reduced over Europe by around 10 to 14% and their tropospheric burden by around 10%. The decrease in OH leads to an increase of the life-time of several species such as VOC. NO2 concentrations are not strongly impacted

  9. 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.

  10. 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

  11. Modeling of photolysis rates over Europe: impact on chemical gaseous species and aerosols

    NASA Astrophysics Data System (ADS)

    Real, E.; Sartelet, K.

    2010-07-01

    This paper evaluates the impact of photolysis rate calculation on European air composition and air quality monitoring. In particular, the impact of cloud parametrisation and the impact of aerosols on photolysis rates are analysed. Photolysis rates are simulated using the Fast-JX photolysis scheme and gas and aerosol concentrations over Europe are simulated with the regional model Polair3D of the Polyphemus platform. The photolysis scheme is first use to update the clear sky tabulation used in the previous Polair3D version. Important differences in photolysis rates are simulated, mainly due to updated cross-sections in the Fast-JX scheme. In the previous Polair3D version, clouds were taken into account by multiplying the clear-sky photolysis rates using a correction factor. In a second stage, the impact of clouds is taken into account more accurately by simulating them directly in the photolysis scheme. Differences in photolysis rates inside clouds are as high as differences between simulations with and without clouds. Outside clouds, the differences are small. The largest difference in gas concentrations is simulated for OH with a mean increase of its tropospheric burden of 4 to 5%. To take into account the impact of aerosols on photolysis rates, Polair3D and Fast-JX are coupled. Photolysis rates are updated every hour. Large impact on photolysis rates is observed at the ground, decreasing with altitude. The aerosol species that impact the most photolysis rates is dust especially in South Europe. Strong impact is also observed over anthropogenic emission regions (Paris, The Po and the Ruhr Valley) where mainly nitrate and sulphate reduced the incoming radiation. Differences in photolysis rates lead to changes in gas concentrations, with the largest impact simulated for OH and NO concentrations. At the ground, monthly mean concentrations of both species are reduced over Europe by around 10 to 14% and their tropospheric burden by around 10%. The decrease in OH leads

  12. 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.

  13. 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

  14. 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.

  15. Quantification of Semi-Volatile gas-phase Organic Compounds (SVOCs) & Organic Aerosol species and the role of SVOCs in Secondary Organic Aerosol formation

    NASA Astrophysics Data System (ADS)

    Khan, M. H.; Holzinger, R.

    2013-12-01

    A Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS) with different sampling systems (multi-stage denuder for gas phase and impact on a collector for aerosol phase) has been deployed in summer 2013 during the Southern Oxidant and Aerosol Study (SOAS) at the SEARCH ground site, Centreville, Alabama for in-situ gas phase and aerosol measurements on an hourly time resolution. A bunch of DB-1 column (0.53 mm x 5.0 μm) is used in the denuder for capturing the bulk of SVOCs and a collection-thermal-desorption (CTD) cell is used for collecting aerosol particles. Several hundreds semivolatile organic compounds (SVOCs) in gas phase and aerosol phases have been detected. The high mass resolution capabilities of ~5000, low detection limit (<0.05 pptv for gas species, <0.01 ng m-3 for aerosol species) and good physical and chemical characterization of SVOCs with the TD-PTR-MS allows constraining both, the quantity and the chemical composition. The SEARCH site was highly impacted by Biogenic Volatile Organic Compounds (BVOCs) and occasionally influenced by anthropogenic pollution. BVOCs and their oxidation products are capable of partitioning into the particle phase, so their simultaneous quantification in both phases has been used to determine the gas/particle-phase partitioning. Our results show the expected diurnal variation based on the changes of air temperature for many species. The results from this study give valuable insights into sources and processing of Secondary Organic Aerosols (SOAs) that can be used to improve parameterization algorithms in regional and global climate models.

  16. Aerosol mass spectrometric analysis of the chemical composition of non-refractory PM(1) samples from school environments in Brisbane, Australia.

    PubMed

    Crilley, Leigh R; Ayoko, Godwin A; Jayaratne, E Rohan; Salimi, Farhad; Morawska, Lidia

    2013-08-01

    Long-term exposure to vehicle emissions has been associated with detrimental health effects. Children are amongst the most susceptible group and schools represent an environment where they can experience significant exposure to vehicle emissions. However, there are limited studies on children's exposure to vehicle emissions in schools. The aim of this study was to quantify the concentration of organic aerosol (OA) and in particular, vehicle emissions that children are exposed to during school hours. Therefore an Aerodyne compact time-of-flight aerosol mass spectrometer (TOF-AMS) was deployed at five urban schools in Brisbane, Australia. TOF-AMS enabled the chemical composition of the non-refractory (NR-PM1) to be analysed with a high temporal resolution to assess the concentration of vehicle emissions and other OA components during school hours. The organic fraction at each school comprised the majority of NR-PM1. Primary emissions were found to dominate the OA at only one school which had an O:C ratio of 0.17, due to fuel powered gardening equipment used near the TOF-AMS. A significant source of the OA at two of the schools was aged vehicle emissions from nearby highways. More oxidised OA was observed at the remaining two schools, which also recorded strong biomass burning influences. In general, the diurnal cycle of the total OA concentration varied between schools and was found to be at a minimum during school hours. The major organic component that school children were exposed to during school hours was secondary OA at all schools. Peak exposure of school children to vehicle emissions occurred during school drop-off and pick-up times. Unless a school is located near major roads, children are exposed predominately to regional secondary OA as opposed to local emissions during school hours in urban environments. PMID:23644356

  17. Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

    NASA Technical Reports Server (NTRS)

    Perkins, P. J.; Papathakos, L. C.

    1977-01-01

    The Global Atmospheric Sampling Program (GASP) by NASA is collecting and analyzing data on gaseous and aerosol trace species in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Advances were made in airborne sampling instrumentation. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei and mass concentrations of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to uniquely identify the source of the air mass as being typically tropospheric or stratospheric. A quantitative understanding of the tropospheric-stratospheric exchange processes leads to better knowledge of the atmospheric impact of pollution through the development of improved simulation models of the atmosphere.

  18. 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

  19. 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

  20. 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.; Peltier, R. E.; Weber, R. J.; Grover, B. D.; Eatough, D. J.; Williams, B. J.; Goldstein, A. H.; Ziemann, P. J.; Jimenez, J. L.

    2011-12-01

    Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate the chemical composition and potential sources of fine particles (PMf) in the inland region of Southern California. In this paper, we briefly summarize the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July-15 August), provide detailed intercomparisons of high-resolution aerosol mass spectrometer (HR-AMS) measurements against complementary measurements, and report the average composition of PMf including the composition of the organic fraction measured by the HR-AMS. Daily meteorology and gas-phase species concentrations were highly consistent, displaying clear diurnal cycles and weekday/weekend contrast. HR-AMS measurements of non-refractory submicron (NR-PM1) mass are consistent and highly correlated with those from a filter dynamics measurement system tapered-element oscillating microbalance (TEOM), while the correlation between HR-AMS and heated TEOM measurements is lower due to loss of high volatility species including ammonium nitrate from the heated TEOM. Speciated HR-AMS measurements are also consistent with complementary measurements as well as with measurements from a collocated compact AMS while HR-AMS OC is similar to standard semi-continuous Sunset measurements within the combined uncertainties of both instruments. A correction intended to account for the loss of semi-volatile OC from the Sunset, however, yields measurements ~30% higher than either HR-AMS or standard Sunset measurements. On average, organic aerosol (OA) was the single largest component of PMf. OA composition was investigated using both elemental analysis and positive matrix factorization (PMF) of HR-AMS OA spectra. Oxygen is the main heteroatom during SOAR-1, with O/C exhibiting a diurnal minimum of 0.28 during the morning rush hour and maximum of 0.42 during the afternoon. O/C is broadly anti

  1. Implications of the chemical transformation of Asian outflow aerosols for the long-range transport of inorganic nitrogen species

    NASA Astrophysics Data System (ADS)

    Chou, Charles C.-K.; Lee, C. T.; Yuan, C. S.; Hsu, W. C.; Lin, C.-Y.; Hsu, S.-C.; Liu, S. C.

    To improve our understanding of the chemical characteristics of aerosols transported from the Asian continent to the western North Pacific, an aerosol observation network has been established in Taiwan. From the measurements made during 2003-2005, it was found that the aerosol concentrations in the continental outflows were much higher than those of remote areas, evidently due to the long-range transport of air pollutants and dust from the Asian continent. Analysis on the chemical compositions of aerosols revealed that the Asian outflow aerosols underwent chemical transformation and, consequently, became more abundant in ammonium and nitrate when they mixed with air pollutants originating from Taiwan. The NH 4+/SO 42- ratio in fine aerosols (PM2.5) increased from 1.55 at the Cape Fuguei, the northern tip of Taiwan, to 2.30 at Penghu, in the middle of the Taiwan Strait. The increased NH 4+/SO 42- ratio implied that the acidity of the sulfate aerosols in Asian outflows was totally neutralized by ammonia as the aerosols traveled through the North Taiwan and its vicinity. In addition, the analysis indicated that the chlorine deficiency of sea salt aerosols was higher at the southern stations than at the Cape Fuguei. The chlorine deficiency was attributed to the heterogeneous reaction of NaCl and HNO 3(g), which means that the oxidation of SO 2 in sea spray droplets was inhibited. Moreover, uptake of secondary acids by the dust particles was observed. The results of this study suggested that the Asian outflow aerosols are important carriers of gaseous inorganic nitrogen species, particularly nitric acid and ammonia, in this region. Hence the atmospheric deposition of soluble inorganic nitrogen could become enhanced in the northern South China Sea, which is downwind of Taiwan during the periods of Asian winter monsoons.

  2. 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

  3. 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.

  4. Detection response of elemental species in single particles using aerosol time-of-flight mass spectrometry

    SciTech Connect

    Silva, P.J.; Gross, D.S.; Gaelli, M.E.; Prather, K.A.

    1998-12-31

    The introduction of real-time particle mass spectrometry(RTSPMS) techniques creates a powerful tool for the study of particulate pollution on the single particle level. One such technique, aerosol time-of-flight mass spectrometry (ATOFMS) provides the aerodynamic size and chemical composition of individual particles. By combining data on size and composition, identification of individual particle classes in ambient outdoor samples is possible. Chemical composition is obtained by performing laser desorption ionization of individual particles using a Nd:YAG laser with a wavelength of 266 nm. The power of RTSPMS techniques is due to the ability to analyze the chemical composition of a single particle. The application of these techniques to analysis of ambient data has been limited however, because few studies have been performed to assess the ability of RTSPMS techniques to detect a wide range of compounds present in the atmosphere on a quantitative rather than qualitative level. It is known that various elemental species will respond differently to laser desorption mass spectrometric detection due to characteristic absorption cross-section and ionization potentials. In order to determine the capability and biases of RTSPMS techniques for detection of elemental species, a series of in-laboratory and ambient experiments has been performed using controlled conditions. Particles of known concentration have been produced from solution using an aerosol generator and analyzed using ATOFMS to determine responses of individual elements on a single particle level. In addition, side-by-side analyses with traditional sampling methods such as MOUDI impactors provide data to show how ATOFMS measurements correlate with federal reference methods.

  5. 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

  6. 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

  7. [Distributions of inorganic nitrogen species in atmospheric aerosols over the East China Sea].

    PubMed

    Shi, Jin-Hui; Zhang, Yun; Li, Rui-Peng; Gao, Hui-Wang; Zhang, Jing

    2010-12-01

    33 total suspended particle samples and 7 size-segregated particle samples were collected over the East China Sea from Nov. to Dec., 2006, Feb. to Mar., 2007 and May. to Jun., 2008. Concentrations of ammonium, nitrate and nitrite in aerosols were measured to investigate their seasonal variation and size distribution. The concentrations of ammonium in aerosols ranged from 2.6 to 646.9 nmol x m(-3) ,with the higher values observed in winter and spring, and the lower values in summer. Nitrate concentrations were from 5.5 to 281.5 nmol x m(-3), presenting the seasonal trend of winter > spring approximately summer. The concentrations of nitrite were very low, less than 0.5 nmol x m(-3). The relative contributions of nitrogen species to total nitrogen varied seasonally in some extent. The contribution of nitrate was comparable with that of ammonium in winter, while the contribution of ammonium was the predominant in spring and summer. The size distribution of nitrate presented clear monthly changes. Most of nitrate existed in the fine particles less than 2.1 microm in Nov. to Dec., and it predominated in the coarse particles with the size of 1.1-4.7 microm and 2.1-7.0 microm, respectively, in Feb. to Mar. and May. to Jun. The size distributions of ammonium in different months were similar, with one peak presenting in the < 1.1 microm fine particles. The air mass back trajectories analysis indicated that the distributions of inorganic nitrogen in aerosols were significantly influenced by the sources and transport pathways of air mass. Both high nitrogen concentration per unit atmospheric volume (nmol x m(-3)) and per unit mass particle (micromol x g(-1)) occurred when the air mass passed over severe pollution region. Both low concentration in atmosphere and particle occurred when the air mass came from clean marine atmosphere. Lower concentration in atmosphere and higher concentration in particle occurred when the air mass originated from the continent and transported

  8. 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.

  9. 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

  10. 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.``

  11. 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

  12. Cleaning patient shower facilities: a novel approach to reducing patient exposure to aerosolized Aspergillus species and other opportunistic molds.

    PubMed

    Anaissie, Elias J; Stratton, Shawna L; Dignani, Maria Cecilia; Lee, Choon-Kee; Mahfouz, Tahsine H; Rex, John H; Summerbell, Richard C; Walsh, Thomas J

    2002-10-15

    We previously have demonstrated that the hospital water-distribution system could be a reservoir for airborne molds that leads to secondary aerosolization of these molds in patient shower facilities. In this report, we show that cleaning the floors of patient shower facilities in a bone marrow transplantation unit reduced the mean air concentrations of molds, including Aspergillus species (from 12 cfu/m3 to 4 cfu/m3; P=.0047). PMID:12355397

  13. 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.

  14. Particle Size Distributions of Water Soluble Species and Nutrient Elements in Aerosols over the Southern Ocean and Coastal East Antarctica

    NASA Astrophysics Data System (ADS)

    Xu, G.; Gao, Y.

    2012-12-01

    The particle size is an important parameter to determin the chemical and physical properties of aerosols of marine origin, especially the fine mode particles that may act as cloud condenstation neuclei (CCN), affecting cloud microphysics and consequently climate. The air-to-sea deposition of aerosol particles are also dependent on particle sizes, which are important for the calculation of atmospheric nutrient fluxes to the ocean. To characterize the size distributions of water-soluble inorganic, organic aerosol species (including Na+, non-sea-salt (nss) sulfate, methane sulfonate (MSA), oxalate and succinate) of marine origin and nutrient elements (inlcuding Cu, Fe, Mn, Ni and Zn and Cd) over the Southern Ocean and coastal East Antarctica, size-segregated aerosols were collected from 40°S, 100°E to 69°S, 76°E and between 69°S, 76°E and 66°S, 110°E during a cruise from November 2010 to March 2011. Results indicate that sea salt particles, a major aerosol component and generated by strong westerly winds, existed mainly in the coarse mode with a concentration peak at >3.0 μm over the Southern Ocean. However, the nss-sulfate, a secondary aerosol species, existed mainly in the fine mode, with a single peak at <0.49 μm over the Southern Ocean, and in a bimodal distribution, peaking at 0.10 - 0.18 μm and 0.32 - 0.56 μm over coastal East Antarctic seas. Over the Southern Ocean, MSA showed a bimodal distribution, a large peak at 0.32-0.56 μm and a small peak at 3.0-7.2 μm, while over coastal East Antarctica, MSA was enriched in particles of 0.32-0.56 μm. Oxalate and formate existed in the fine mode, while succinate showed a bimodal distribution. Nutrient elements including Fe, Mn and Cd showed a bimodal distribution, at both submicron and supermicron size ranges. While Zn was mainly accumulated at 1.0-3.2 μm over coastal East Antarctica, both Zn and Cd mainly existed in the fine mode with a concentration peak at <0.49 μm over the Southern Ocean. Different

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

    DOE PAGESBeta

    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

  16. 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

  17. Hygroscopicity of water-soluble organic compounds in atmospheric aerosols: amino acids and biomass burning derived organic species.

    PubMed

    Chan, Man Nin; Choi, Man Yee; Ng, Nga Lee; Chan, Chak K

    2005-03-15

    Amino acids and organic species derived from biomass burning can potentially affect the hygroscopicity and cloud condensation activities of aerosols. The hygroscopicity of seven amino acids (glycine, alanine, serine, glutamine, threonine, arginine, and asparagine) and three organic species most commonly detected in biomass burning aerosols (levoglucosan, mannosan, and galactosan) were measured using an electrodynamic balance. Crystallization was observed in the glycine, alanine, serine, glutamine, and threonine particles upon evaporation of water, while no phase transition was observed in the arginine and asparagine particles even at 5% relative humidity (RH). Water activity data from these aqueous amino acid particles, except arginine and asparagine, was used to revise the interaction parameters in UNIQUAC functional group activity coefficients to give predictions to within 15% of the measurements. Levoglucosan, mannosan, and galactosan particles did not crystallize nor did they deliquesce. They existed as highly concentrated liquid droplets at low RH, suggesting that biomass burning aerosols retain water at low RH. In addition, these particles follow a very similar pattern in hygroscopic growth. A generalized growth law (Gf = (1 - RH/100)-0.095) is proposed for levoglucosan, mannosan, and galactosan particles. PMID:15819209

  18. 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.

  19. Spatial distribution and temporal variation of chemical species in the bulk atmospheric aerosols collected at the Okinawa archipelago, Japan

    NASA Astrophysics Data System (ADS)

    Handa, D.; Somada, Y.; Ijyu, M.; Azechi, S.; Nakaema, F.; Arakaki, T.; Tanahara, A.

    2009-12-01

    The economic development and population growth in recent Asia have been increasing air pollution. A computer simulation study showed that air pollutants emitted from Asian continent could spread quickly within northern hemisphere. We initiated a study to elucidate the special distribution and chemical characterization of atmospheric aerosols around Okinawa archipelago, Japan. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location in Asia is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. We simultaneously collected bulk aerosol samples by using the same types of high volume air samplers at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS, Okinawa Island), Kume Island (ca. 160 km south-west of CHAAMS) and Minami-daitou Island (ca. 320 km south-east of CHAAMS). We determined the concentrations of water-soluble anions, cations and dissolved organic carbon (DOC) using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. We report and discuss spatial distribution and temporal variation of chemical species concentrations in bulk atmospheric aerosols collected during July, 2008 to July, 2009. We determine “background” concentration of chemical components in Okinawa archipelago. We then compare each chemical component among CHAAMS, Kume Island and Minami-daito Island to elucidate the influence of the long-range transport of chemical species from Asian continent.

  20. Estimates of aerosol species scattering characteristics as a function of relative humidity

    NASA Astrophysics Data System (ADS)

    Malm, William C.; Day, Derek E.

    The absorption of water by ambient aerosols can significantly increase the light scattering coefficient and thereby affect issues such as visibility and climate forcing. Although water absorption by inorganic compounds and mixtures of inorganic compounds can often be modeled with adequate certainty for most applications, modeling water uptake by organic aerosols at present is speculative. In this paper, we present data in the form of f (RH)=b scat(RH)/b scat,dry , where bscat(RH) is the scattering coefficient measured at some relative humidity (RH)>20% and bscat,dry is the scattering coefficient measured at RH <20%. The f(RH) has been measured at Great Smoky Mountains National Park in Tennessee and at Grand Canyon National Park in Arizona. The f(RH) curves obtained from these two sites, which show distinctly different aerosol composition and average RH values, are compared. We also present comparisons between the measured water uptake by ambient aerosol with modeled water uptake by inorganic compounds to estimate the water uptake by organic aerosol.

  1. Numerical modeling of species transport in turbulent flow and experimental study on aerosol sampling

    NASA Astrophysics Data System (ADS)

    Vijayaraghavan, Vishnu Karthik

    Numerical simulations were performed to study the turbulent mixing of a scalar species in straight tube, single and double elbow flow configurations. Different Reynolds Averaged Navier Stokes (RANS) and Large Eddy Simulation (LES) models were used to model the turbulence in the flow. Conventional and dynamic Smagorinsky sub-grid scale models were used for the LES simulations. Wall functions were used to resolve the near wall boundary layer. These simulations were run with both two-dimensional and three-dimensional geometries. The velocity and tracer gas concentration Coefficient of Variations were compared with experimental results. The results from the LES simulations compared better with experimental results than the results from the RANS simulations. The level of mixing downstream of a S-shaped double elbow was higher than either the single elbow or the U-shaped double elbow due to the presence of counter rotating vortices. Penetration of neutralized and non-neutralized aerosol particles through three different types of tubing was studied. The tubing used included standard PVC pipes, aluminum conduit and flexible vacuum hose. Penetration through the aluminum conduit was unaffected by the presence or absence of charge neutralization, whereas particle penetrations through the PVC pipe and the flexible hosing were affected by the amount of particle charge. The electric field in a space enclosed by a solid conductor is zero. Therefore charged particles within the conducting aluminum conduit do not experience any force due to ambient electric fields, whereas the charged particles within the non-conducting PVC pipe and flexible hose experience forces due to the ambient electric fields. This increases the deposition of charged particles compared to neutralized particles within the 1.5" PVC tube and 1.5" flexible hose. Deposition 2001a (McFarland et al. 2001) software was used to predict the penetration through transport lines. The prediction from the software compared

  2. 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).

  3. 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

  4. Carbon content of common airborne fungal species and fungal contribution to aerosol organic carbon in a subtropical city

    NASA Astrophysics Data System (ADS)

    Cheng, Jessica Y. W.; Chan, Chak K.; Lee, C.-T.; Lau, Arthur P. S.

    Interest in the role and contribution of fungi to atmospheric aerosols and processes grows in the past decade. Substantial data or information such as fungal mass or carbon loading to ambient aerosols is however still lacking. This study aimed to quantify the specific organic carbon content (OC per spore) of eleven fungal species commonly found airborne in the subtropics, and estimated their contribution to organic carbon in aerosols. The specific OC contents showed a size-dependent relationship ( r = 0.64, p < 0.05) and ranged from 3.6 to 201.0 pg carbon per spore or yeast cell, giving an average of 6.0 pg carbon per spore (RSD 51%) for spore or cell size less than 10 μm. In accounting for natural variations in the composition and abundance of fungal population, weighted-average carbon content for field samples was adopted using the laboratory determined specific OC values. An average of 5.97 pg carbon per spore (RSD 3.8%) was enumerated from 28 field samples collected at the university campus. The mean fungal OC concentration was 3.7, 6.0 and 9.7 ng m -3 in PM 2.5, PM 2.5-10 and PM 10, respectively. These corresponded to 0.1%, 1.2% and 0.2% of the total OC in PM 2.5, PM 2.5-10 and PM 10, respectively. In the study period, rain provided periods with low total OC but high fungal prevalence and fungi contributed 7-32% OC in PM 2.5-10 or 2.4-7.1% OC in PM 10. More extensive studies are deserved to better understand the spatial-, temporal- and episodic dependency on the fungal OC contribution to the atmospheric aerosols.

  5. Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

    NASA Astrophysics Data System (ADS)

    Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

    2014-12-01

    Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

  6. 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

  7. 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.

  8. Year-round observations of water-soluble ionic species and trace metals in Sapporo aerosols: implication for significant contributions from terrestrial biological sources in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Fu, P.

    2013-03-01

    High aerosol loadings are prevalent in the atmosphere of East Asia, where the aerosols impact the Earth's climate system and human health; however, their sources and seasonal variations are not clearly understood. To better understand the sources of water-soluble ionic species and trace metals in Northeast Asia, we studied atmospheric aerosol samples collected in Sapporo, northern Japan for one-year period. SO42- (average 3.47 ± 1.03 μg m-3) was found as the most abundant ionic species, which accounted for on average 43 ± 15% of the measured total ionic mass followed by Cl- (13 ± 12%) ≈ NO3- ≈ Na+ > NH4+ > Ca2+ > Mg2+ > K+ > MSA-. Among the metals determined, Ca was found as the most abundant (45 ± 5.2%) followed by Fe (27 ± 4.5%), Al (21± 3.1%), Zn (3.2 ± 1.7), Ti, Mn, Ni, Pb, Cu, V, As, Cr and Cd. Based on factor analysis, linear relations of selected species with biomarkers, and backward air mass trajectories, we found that long-range atmospheric transport of soil dust (∼ 33%) from arid regions of Mongolia and/or Northeast China is a major source for Sapporo aerosols as well as terrestrial biogenic emissions (≥ 24%) including microbial activities and biomass burning mostly from distant source region(s) (e.g. Siberia). We also found that the contributions of soil dust to the aerosols maximized in early spring whereas those of vegetational emissions maximized in spring/summer. Contributions of microbial activities to aerosols peaked in autumn whereas forest fires/biomass burning peaked in autumn/winter. On the contrary, fossil fuel combustion/industrial activities and oceanic emissions to Sapporo aerosols are suggested to be rather minor. This study also suggests that fungal spores contribute to some trace metals (i.e. Ni, Cu, As) while pollen contributes to Zn in aerosols.

  9. 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.

  10. 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

  11. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

  14. Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

    NASA Astrophysics Data System (ADS)

    Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

    2014-06-01

    Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photooxidation under a range of controlled conditions (RH ∼65-89%, VOC/NOx ∼3-9 and NOx ∼2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line, chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene, but low isoprene emitter, and its emissions were observed to produce measureable amounts of SOA via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e., in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photooxidation products of the minor VOCs co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally-isoprene emitting landscapes in Southeast Asia. Moreover, in general the amount of aerosol mass produced from the emissions of the principally

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. The major species of heavy metal aerosol resulting from water cooling systems and spray dryer systems during incineration processes

    PubMed

    Wey; Yang; Wei

    1998-11-01

    Trace toxic metals in municipal solid waste may escape from the incineration process in flue gas, in dry collected ash, in wet scrubbed ash, or as a suspended aerosol. Therefore, understanding the behavior of heavy metals in the flue gas and the best controls in the air pollution control equipment are important and necessary. The control conditions of water cooling and spray dryer systems during incineration processes significantly influence the formation of heavy metal compounds. The formation of chromium (Cr), lead (Pb), and cadmium (Cd) species under various control conditions (water cooling tower and spray dryer reactor) was investigated in this study. The object of the experiment is to understand the effects of water cooling and spray dryer systems individually on the formation of heavy metal species. The operating parameters that are evaluated include different control systems, control temperatures, and chlorine content. A thermodynamic equilibrium model was also used to evaluate experimental data. In order to match real incineration conditions, a two-stage simulation was performed in this experiment. The results showed that the relationship of speciation between the simulation prediction and X-ray diffraction (XRD) analysis is consistent for Cr compounds; both indicated that Cr2O3 is the major species. The relationship is almost the same for Cd compounds, but not for Pb compounds. PMID:9846130

  20. 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.

  1. 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

  2. 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 ...

  3. Laboratory studies of the reactive uptake of biogenic species: Evidence for the direct polymerization of isoprene, terpenes and sesquiterpenes on acidic aerosols

    NASA Astrophysics Data System (ADS)

    Li, S.; Liggio, J.; Mihele, C.; Brook, J.

    2006-12-01

    Numerous studies on heterogeneous reactions have shown that polymerization of semi-volatile and volatile organic compounds occurs in aerosols. To date, most evidence suggests that gaseous hydrocarbon oxidation products containing carbonyl functionality are the prime candidates for these processes. Such processes involve primarily hydration, acetal formation, polymerization and aldol-condensation reactions, resulting in oligomer products of potential significance with respect to secondary organic aerosol formation (SOA). However, little information on the heterogeneous reactions of unsaturated hydrocarbons (olefins) is known. Given that biogenic species, many of them unsaturated, make up a considerable portion of hydrocarbons emitted globally, direct reactive uptake of these compounds on aerosols would also potentially be a major source of SOA. In the present study, individual biogenic hydrocarbons were exposed to pre-existing acidic sulfate aerosols within a 2 m3 Teflon reaction chamber under varying relative humidity conditions. An Aerosol Mass Spectrometer was used to quantify any subsequent increase in organic mass as a function of time, and to obtain information regarding the structure of products via aerosol mass spectra. A Proton Transfer Reaction Mass Spectrometer was used to measure the gas-phase concentrations of isoprene, terpenes (?-pinene, ?-pinene, limonene, and carene) and sesquiterpenes (?-caryophylene and humulene) in the reaction chamber. Results from these experiments show that a significant amount of these compounds are taken up by the acidic aerosols rapidly, in a polymerization process which was highly dependent on the particle acidity. This polymerization mechanism likely involves the oxygenation of the resulting polymers via acid catalyzed hydration. The uptake of the unsaturated hydrocarbons suggests that gas-phase oxidation of biogenics to condensable products is not the only route to SOA. Details of the polymerization and hydration

  4. Dust, Aerosol Ions and Their Interactions with Gaseous Species in East Asia During Spring 2001: A three-dimensional model Study

    NASA Astrophysics Data System (ADS)

    Tang, Y.; Carmichael, G. R.; Seinfeld, J. H.; Dabdub, D.; Weber, R. J.; Huebert, B.; Clarke, A. D.; Guazzotti, S. A.; Prather, K. A.; Sodeman, D. A.; Uno, I.; Woo, J.; Streets, D. G.; Quinn, P.; Johnson, J. E.; Song, C.; Anderson, T. L.; Sandu, A.; Talbot, R. W.; Dibb, J. E.

    2003-12-01

    A comprehensive regional chemical transport model is developed to study the aerosol-related issues for TRACE-P and ACE-ASIA experiments, which includes on-line thermodynamic module SCAPE II and on-line photolysis-rate calculation TUV, and explicitly considers dust heterogeneous reactions and chemical-aging process. The Asian outflow during March and April of 2001 is heavy polluted with high aerosol loading. Under cation-limited condition, SO2 oxidation and ammonium availability determined the nitrate size and gas-aerosol distributions. Dust was one of most important aerosol outflow during this period, which brought significant influences on other aerosols and gaseous species. A main role of dust in the equilibrium process is through the enhancement of the aerosol calcium concentration, which shifts the equilibrium balance to an anion-limited status. This status benefits the uptake of sulfate and nitrate, but repels ammonium. Dust influence on secondary aerosols and their size distributions is also determined by dust mass, size distribution and fresh ratio. The impacts of heterogeneous reactions on fresh dust involving O3, NO2, SO2 and HNO3 are studied by incorporating these reactions into the analysis. These reactions have significant influence on regional chemistry. For examples, the low O3 concentrations in the C-130 flight 6 can be explained only by the influence of heterogeneous reactions. Dust appearance significantly increased optical depth, and the radiative influence of dust can also affect the photochemical system. For example, OH levels can decrease by 20% near surface. All these dust impacts is sensitive to the dust mass, its size distribution, assumptions about its mixing state (internal vs. external), and the fraction of the aerosol mass available for heterogeneous reactions and equilibrium process.

  5. 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

  6. 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

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

    PubMed

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

    2013-11-01

    Changes in ecosystem function at Rocky Mountain National Park (RMNP) are occurring because of emissions of nitrogen and sulfate species along the Front Range of the Colorado Rocky Mountains, as well as sources farther east and west. The nitrogen compounds include both oxidized and reduced nitrogen. A year-long monitoring program of various oxidized and reduced nitrogen species was initiated to better understand their origins as well as the complex chemistry occurring during transport from source to receptor. Specifically the goals of the study were to characterize the atmospheric concentrations of nitrogen species in gaseous, particulate, and aqueous phases (precipitation and clouds) along the east and west sides of the Continental Divide; identify the relative contributions to atmospheric nitrogen species in RMNP from within and outside of the state of Colorado; identify the relative contributions to atmospheric nitrogen species in RMNP from emission sources along the Colorado Front Range versus other areas within Colorado; and identify the relative contributions to atmospheric nitrogen species from mobile sources, agricultural activities, and large and small point sources within the state of Colorado. Measured ammonia concentrations are combined with modeled releases of conservative tracers from ammonia source regions around the United States to apportion ammonia to its respective sources, using receptor modeling tools. PMID:24344569

  8. Characterisation of chemical species in PM 2.5 and PM 10 aerosols in Brisbane, Australia

    NASA Astrophysics Data System (ADS)

    Chan, Y. C.; Simpson, R. W.; McTainsh, G. H.; Vowles, P. D.; Cohen, D. D.; Bailey, G. M.

    Aerosol samples for PM 10 (particulate matter with aerodynamic diameters less than 10 um) were collected from September 1993 to August 1994 at five sites representing the major land use patterns in Brisbane, a subtropical coastal city in Australia. The samples collected were analysed by techniques such as ion beam analysis and the integrating plate laser absorption method, and the chemical composition of the samples was reconstructed from the observed elemental composition. For these PM 10 samples, the major components, on average, were crustal matter (25% by mass), organics (17%), sea salt (12%), elemental carbon (10%) and ammonium sulphate (7%). Aerosol samples of PM 2.5 (particulate matter with aerodynamic diameter less than 2.5 μm) were collected by a dichotomous sampler at one of the sites (GU), a site on university buildings located in a suburban area of Brisbane but surrounded by a buffer zone provided by a forest conservation area. A high average fine Br/Pb ratio of 0.36 in the GU samples, which is close to that in vehicle exhausts, indicates that this site probably has low background levels of lead even though there has been significant traffic in the area for 20 years, so the forest area is an effective buffer to road dust from the surrounding suburbia. Temporal trends at this site suggest that road side dust and industry-sourced crustal matter could contribute to more than half of the mass of crustal matter. Seasonal meteorological conditions which determine the dispersion of pollutants out of Brisbane and the continuous input of rural dust into Brisbane are potentially important factors influencing the level of crustal matter in Brisbane. However, major rural dust events do not considerably increase the seasonal average level of crustal matter. Also, apart from significant local influences at some sites (such as heavy road traffic network or a cement factory), the results from the GU site show a similar level of elemental and chemical components from

  9. 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

  10. 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.

  11. 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.

  12. An automatic recorder for air/firn transfer studies of chemical aerosol species at remote glacier sites

    NASA Astrophysics Data System (ADS)

    Preunkert, Susanne; Wagenbach, Dietmar

    In order to gain year round information on the relationship between major ions in atmospheric aerosol and deposited snow at ice core drill sites, an automatic station for filter pack sampling and for monitoring of snow height changes by vertical temperature profile readings was developed. The station was deployed for two years at a high elevation ice core drill site in the Alps (Colle Gnifetti, 4450 m asl) and thoroughly tested during several unattended campaigns for its long term reliability. Both devices showed a good long-term field performance, despite harsh environmental conditions, with the exception of data logger break downs induced by strong thunderstorms. Snow height evaluations from the vertical temperature profiles and their temporal changes provided a depth resolution of less than 5 cm and agreed well with concurrent readings from an ultra-sonic distance meter. Measurement of major ions in the autonomously sampled filter packs revealed (1) enhanced field blanks for nearly all species but no important increase of the NH +4 to SO 2-4 ratio during storage of exposed filters, (2) a nearly complete remobilisation of NO -3, Cl - and Br - from the front quartz filters and (3) a sufficiently large retention of gaseous NO -3, Cl - and Br - species on the back up nylon filters to allow quantification of the total concentration of these ions. Except for Na +, K + and Mg 2+ the (field blank controlled) detection limits allowed to evaluate year round atmospheric concentrations although mid-winter levels have been as low as in central Greenland during summer. The pattern and summer-winter means of atmospheric concentrations were found to be consistent with year round observations performed at a lower Alpine site as well as with the chemical snow properties at Colle Gnifetti.

  13. 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.

  14. 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.

  15. Detailed Mass Size Distributions of Aerosol Species and Trace Elements at Skukuza, South Africa, During SAFARI 2000

    NASA Astrophysics Data System (ADS)

    Schwarz, J.; Maenhaut, W.; Cafmeyer, J.; Chi, X.; Annegarn, H. J.

    2001-12-01

    Two types of cascade impactors were used to collect size-fractionated aerosol samples during August-September 2001 at Skukuza, South Africa, as part of the SAFARI 2000 final dry season campaign. The impactors were a 10-stage microorifice uniform deposit impactor (MOUDI), with cut-points down to 53 nm equivalent aerodynamic diameter (EAD), and a 12-stage small deposit area low pressure impactor (SDI), with cut-points down to 45 nm EAD. Separate day and night samples were collected, starting at about 7:00 and at about 18:00 local time, respectively. The MOUDI samples were analysed for the particulate mass (PM) by weighing, and for organic carbon (OC) and elemental carbon (EC) by a thermal-optical transmission technique. The SDI samples were analysed for 28 elements by particle-induced X-ray emission (PIXE). The total concentrations (summed over all stages) varied quite substantially during the campaign (up to a factor of 50 for certain elements), but no systematic day/night difference pattern was observed. Also the size distributions were rather similar during day and night. PM, OC, EC, S, K, Zn, As, Se, Br, Rb, and Pb had most of their mass in the submicrometer size range, with maximum typically at about 0.3 to 0.5 micrometer EAD. Several of those species and elements are good indicators for biomass burning. Mass median aerodynamic diameters (MMADs) were calculated for the various elements and compared with those obtained during SAFARI-92. During this earlier campaign, which also took place in the dry season, daily samples were taken at Skukuza with a PIXE International cascade impactor (PCI). For the crustal and sea-salt elements, fairly similar MMADs were obtained in the two campaigns. For the fine-mode elements, however, the MMADs were substantially lower during SAFARI 2000 than during SAFARI-92. During this earlier campaign, the MMADs were most likely overestimated.

  16. 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

  17. 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

  18. Detailed mass size distributions of elements and species, and aerosol chemical mass closure during fall 1999 at Gent, Belgium

    NASA Astrophysics Data System (ADS)

    Maenhaut, Willy; Cafmeyer, Jan; Dubtsov, Sergei; Chi, Xuguang

    2002-04-01

    A 10-stage microorifice uniform deposit impactor (MOUDI) and a 12-stage small deposit area low pressure impactor (SDI) were operated at Gent from 6 September to 30 October 1999. Thirty-four parallel samples (of typically 24 h) were collected. The MOUDI samples were analysed for the particulate mass (PM) by weighing, and for organic carbon (OC) and elemental carbon (EC) by a thermal-optical transmission technique. The SDI samples were analysed for 27 elements by PIXE. PM and OC exhibited typically a rather similar bimodal size distribution, with most of their mass in the submicrometer size range. EC was predominantly associated with fine particles, with maximum typically at around 0.2 μm equivalent aerodynamic diameter (EAD). Sulphur was also mainly in the fine size range, but with maximum at 0.5 μm EAD. Other elements with mainly a fine mode were V, Ni, As, Se and Pb. The crustal elements (Al, Si, Ti, Fe, Zr) exhibited mostly a unimodal coarse mode size distribution, with maximum at about 4 μm EAD. Other elements with mainly a coarse mode were Na, Mg, P, Ca, Cr, Mn, Cu, Ga and Sr. The elements K, Zn and Rb were generally bimodal. Aerosol chemical mass closure calculations indicated that organic aerosol and crustal matter were the major aerosol types in the supermicrometer size range, and that the dominant aerosol types in the submicrometer fraction were organic aerosol and sulphate. On average, 74% of the gravimetric PM was accounted for by the aerosol types considered.

  19. 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

  20. 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

  1. Impact of interannual variations in sources of insoluble aerosol species on orographic precipitation over California's central Sierra Nevada

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

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

  2. 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

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. 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 PAGESBeta

    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

  8. Atmospheric gaseous HNO 3, particulate nitrate, and aerosol size distributions of major ionic species at a rural site in western Germany

    NASA Astrophysics Data System (ADS)

    Mehlmann, Alois; Warneck, Peter

    Nitric acid and particulate nitrate in addition to other trace species were measured in the air at Deuselbach, a rural site in western Germany, in June and July 1985 under background atmospheric conditions. High-volume open face triple filter packs and cascade impactors were used together with ion-chromatographic analyses. Laboratory tests showed good correspondence between gaseous nitric acid and nitrate deposited on nylon back-up filters for low ambient aerosol concentrations as observed in the field. High aerosol loadings typically found in Mainz caused part of nitric acid to be retained together with particulate nitrate on the teflon front filter. The concentration of nitric acid observed in the field went through a maximum during the day and a minimum at night with a clear anti-correlation with relative humidity. For r.h. ⩽ 60% the average fraction of gaseous to total nitrate was 39 ± 8%. The average fraction from all data was 22%. The molar fraction of total nitrate to nitrogen dioxide was 24%. It is shown that the diurnal variation of HNO 3 is partly due to absorption by liquid water associated with the aerosol, which increases with rising relative humidity (at night). The absorption is significant only because solution pH is buffered by the presence of sulfate and the formation of bisulfate. Most of the field data showed particulate nitrate to occur primarily in the coarse size range ( ⩾ 2 μm diameter) with sodium providing the main cation. Sea salt was identified as the principal source of sodium. Ammonium nitrate occurred only sporadically in the fine particle mode ( ⩽ 2 pm diameter). Ammonium nitrate was largely absent because the product of the concentrations of nitric acid (observed) and ammonia (inferred) was below the minimum required for equilibrium concentrations of particulate NH 4NO 3 to form. In addition, there often was insufficient ammonium (and other measurable cations) present in fine particles to balance the amount of sulfate.

  9. 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.

  10. 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. PMID:25124269

  11. Size-resolved airborne particulate oxalic and related secondary organic aerosol species in the urban atmosphere of Chengdu, China

    NASA Astrophysics Data System (ADS)

    Cheng, Chunlei; Wang, Gehui; Meng, Jingjing; Wang, Qiyuan; Cao, Junji; Li, Jianjun; Wang, Jiayuan

    2015-07-01

    Size-segregated (9-stages) airborne particles during winter in Chengdu city of China were collected on a day/night basis and determined for dicarboxylic acids (diacids), ketocarboxylic acids (ketoacids), α-dicarbonyls, inorganic ions, and water-soluble organic carbon and nitrogen (WSOC and WSON). Diacid concentration was higher in nighttime (1831 ± 607 ng m- 3) than in daytime (1532 ± 196 ng m- 3), whereas ketoacids and dicarbonyls showed little diurnal difference. Most of the organic compounds were enriched in the fine mode (< 2.1 μm) with a peak at the size range of 0.7-2.1 μm. In contrast, phthalic acid (Ph) and glyoxal (Gly) presented two equivalent peaks in the fine and coarse modes, which is at least in part due to the gas-phase oxidation of precursors and a subsequent partitioning into pre-existing particles. Liquid water content (LWC) of the fine mode particles was three times higher in nighttime than in daytime. The calculated in-situ pH (pHis) indicated that all the fine mode aerosols were acidic during the sampling period and more acidic in daytime than in nighttime. Robust correlations of the ratios of glyoxal/oxalic acid (Gly/C2) and glyoxylic acid/oxalic acid (ωC2/C2) with LWC in the samples suggest that the enhancement of LWC is favorable for oxidation of Gly and ωC2 to produce C2. Abundant K+ and Cl- in the fine mode particles and the strong correlations of K+ with WSOC, WSON and C2 indicate that secondary organic aerosols in the city are significantly affected by biomass burning emission.

  12. The chemical content of raindrops as a function of drop radius, part III: A new method to measure the mean aerosol particle size of different inorganic species in the atmosphere

    NASA Astrophysics Data System (ADS)

    Ebert, P.; Baechmann, K.; Frank, G.; Tschiersch, J.

    A new method is presented to measure the mean aerosol particle size of different inorganic species in atmosphere by collecting raindrops as a function of drop radius. In previous measurements of inorganic species (e.g. Na +, Mg 2+, Cl - or SO 42-) of size classified raindrops, an interdependence was obtained between concentration of these compounds in raindrops and drop size (" c/r-dependence"). A decrease in concentration with increasing drop radius was found at the beginning of precipitation. Further measurements of size classified raindrops at later precipitation times ( t > 10 min) showed a concentration maximum at a specific drop radius. However, the same c/r-dependence was always measured for elements located on aerosol particles near ground (e.g. Al, Fe, Mn or Pb). These species show the same curve shape with no dependence on sampling time. New results concerning these elements show that this is not true. Their c/r-dependencies also changed during long precipitation times ( t > 3 h). This is caused by the changing medium particle size during long precipitation times, whereas other below-cloud processes have a strong influence on the c/r-dependence of the elements first mentioned (e.g. Na +, Mg +, Cl - or SO 42-). The rapidly changing c/r-dependence of these species at the beginning of precipitation is caused by evaporation of the smallest raindrops. Results of a tracer experiment clearly indicated that the c/r-dependence of elements located on aerosol particles near ground is mainly influenced by the size of scavenged aerosol particles on which these elements are located. This experiment establishes a connection between raindrop radius showing concentration maximum and scavenged aerosol particle size. Therefore, it is also possible to measure size classified raindrops at real rain events in order to get the mean scavenged particle size of inorganic species in atmosphere.

  13. Neutralization of calcite in mineral aerosols by acidic sullur species collected in China and Japan studied by ca K-edge X-ray absorption near-edge structure.

    PubMed

    Takahashi, Yoshio; Miyoshi, Takuro; Higashi, Masayuki; Kamioka, Hikari; Kanai, Yutaka

    2009-09-01

    Calcium species in mineral aerosols collected simultaneously in Aksu (near the Taklimakan Desert), Qingdao (eastern China), and Tsukuba (Japan) during dust and nondust periods were determined using Ca K-edge X-ray absorption near-edge structure (XANES). From the fitting of XANES spectra, it was found that (i) calcite and gypsum were the main Ca species in the aerosol samples, and (ii) the gypsum fraction versus total Ca minerals [Gyp]/[Ca2+]t increased progressively in the order Aksu < Qingdao < Tsukuba. Surface-sensitive XANES in the conversion electron yield mode (CEY) showed that the gypsum is formed selectively at the surface of mineral aerosols for all the samples except for that taken in Aksu during the dust period. The decrease of the [Gyp]/[Ca2+]t ratio with an increase in particle size showed that the neutralization effect proceeds from the particle surface. For the Aksu sample in the dust period, however, (i) the [Gyp]/[Ca2+]t ratios obtained by XANES measured in the fluorescence (FL; regarded as bulk analysis) and CEY modes were similar and (ii) size dependence was not found, showing that neutralization is not important for the sample because of the large supply of mineral aerosol with little neutralization effect in Aksu. It was also found that the pH of the aerosol and the ratio of (NH4)2SO4 to gypsum were positively and negatively correlated with the Ca (or calcite) content, respectively. The speciation of Ca by XANES revealed the neutralization processes of acidic sulfur species by calcite during the long-range transport of mineral aerosols. PMID:19764213

  14. Aerosol Monosaccharide Anhydrides as Tracer Species for Identifying Wildfire Smoke Transport to California's Central Valley in August 2002

    NASA Astrophysics Data System (ADS)

    Abhyankar, M. S.; Dixon, R. W.

    2007-12-01

    The Biscuit fire burned close to 2,000 km2 of forested land in southwestern Oregon in July and August, 2002. August, 2002 also was a time in which PM2.5 concentrations were higher than typical in California Central Valley cities located several hundred kilometers to the southeast. The concentrations of two monosaccharide anhydrides, levoglucosan and mannosan, were measured in aerosol samples collected at four California Air Resource Board sites in Central Valley cities for the purpose of determining how the wildfire smoke affected air quality. Levoglucosan concentrations ranged from the detection limit of 18 ng m-3 to about 400 ng m-3. While days with high levoglucosan concentrations generally had above average to high PM2.5 concentrations, there were also days with high PM2.5 concentrations with low levoglucosan concentrations. Although mannosan was only detected in a small number of samples, the levoglucosan to mannosan ratios in these samples were consistent with smoke from softwood combustion. A wildfire source levoglucosan to PM2.5 concentration ratio was used to estimate the PM2.5 concentration originating from smoke. From this method, smoke was found to be a significant (greater than 10% of the total PM2.5 concentration) on occassions. The estimated smoke PM2.5 concentration always remained less than 10 μg m-3 and contributed to less than a third of the total PM2.5 concentration. Because the PM2.5 concentrations were higher than typical August values, either there were other factors leading to high PM2.5 concentrations in August 2002, or the smoke estimation method underestimated the smoke concentration.

  15. 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.

  16. 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

  17. 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.

  18. 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.

  19. 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

  20. 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.

  1. Integrated chemical species analysis with source-receptor modeling results to characterize the effects of terrain and monsoon on ambient aerosols in a basin.

    PubMed

    Chen, Chi-Fan; Liang, Jeng-Jong

    2013-05-01

    This study integrated estimated oxidation ratio of sulfur (SOR) and oxidation ratio of nitrogen (NOR) with source-receptor modeling results to identify the effects of terrain and monsoons on ambient aerosols in an urban area (north basin) and a rural area (south basin) of the Taichung Basin. The estimated results indicate that the conversion of sulfur mainly occurs in fine particles (PM₂.₅), whereas the conversion of nitrogen occurs in approximately equal quantities of PM₂.₅ and coarse particles (PM₂.₅-₁₀). The results show a direct relationship for PM₂.₅ between the modeling results with SOR and NOR. The high PM₂.₅ SOR, NOR, and secondary aerosol values all occurred in the upwind area during both monsoons; this shows that the photochemical reaction and the terrain effect on the pollutant transmission were significant in the basin. Additionally, the urban heat island effect on the urban area and the valley effect on the rural area were significant. The results show that secondary aerosol in PM₂.₅-₁₀ contributed approximately 10 % during both monsoons, and the difference in the contribution from secondary aerosol between both areas was small. Vehicle exhaust emissions and wind-borne dust were two crucial PM2.5-10 contributors during both monsoons; their average contributions in both areas were higher than 34 and 32 %, respectively. PMID:22996820

  2. 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 ...

  3. 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.

  4. Studies of organic aerosol and aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Duong, Hanh To

    Atmospheric aerosols can influence society and the environment in many ways including altering the planet's energy budget, the hydrologic cycle, and public health. However, the Fourth Assessment Report of the Intergovernmental Panel on Climate Change indicates that the anthropogenic radiative forcing associated with aerosol effects on clouds has the highest uncertainty in the future climate predictions. This thesis focuses on the nature of the organic fraction of ambient particles and how particles interact with clouds using a combination of tools including aircraft and ground measurements, models, and satellite data. Fine aerosol particles typically contain between 20 - 90% organic matter by mass and a major component of this fraction includes water soluble organic carbon (WSOC). Consequently, water-soluble organic species can strongly influence aerosol water-uptake and optical properties. However, the chemical composition of this fraction is not well-understood. PILS-TOC was used to characterize WSOC in ambient aerosol in Los Angeles, California. The spatial distribution of WSOC was found to be influenced by (i) a wide range of aerosol sources within this urban metropolitan area, (ii) transport of pollutants by the characteristic daytime sea breeze trajectory, (iii) topography, and (iv) secondary production during transport. Meteorology is linked with the strength of many of these various processes. Many methods and instruments have been used to study aerosol-cloud interactions. Each observational platform is characterized by different temporal/spatial resolutions and operational principles, and thus there are disagreements between different studies for the magnitude of mathematical constructs used to represent the strength of aerosol-cloud interactions. This work points to the sensitivity of the magnitude of aerosol-cloud interactions to cloud lifetime and spatial resolution of measurements and model simulations. Failure to account for above-cloud aerosol layers

  5. 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.

  6. 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

  7. 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.

  8. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  9. 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

  10. Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect

    SciTech Connect

    Wang, J. X.; Lee, Y.- N.; Daum, Peter H.; Jayne, John T.; Alexander, M. L.

    2008-11-03

    Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/ Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.2% supersaturation to those predicted based on size distribution and chemical composition using K¨ohler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization.

  11. 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

  12. 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.

  13. 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

  14. Mesoscale and synoptic scale transport of aerosols

    SciTech Connect

    Wolff, G.T.

    1980-01-01

    An overview is presented of mesoscale and synoptic-scale (macroscale) aerosol transport as observed in recent air pollution field studies. Examples of mesoscale transport systems are discussed, including urban plumes, sea breezes, the mountain-valley wind cycle, and the urban-heat-island circulation. The synoptic-scale systems considered are migrating high- and low-pressure systems. Documented cases are reviewed of aerosol transport in the various mesoscale systems, aerosol accumulation and transport in high-pressure systems, and acid precipitation in low-pressure systems. The characteristics of the transported aerosols are identified, along with the chemical species that occur primarily in aerosols in the accumulation mode (particle diameters of 0.1-3 microns). It is shown that aerosol particles in the accumulation mode are the most important in terms of synoptic-scale and mesoscale transport and that such particles are primarily responsible for visible haze.

  15. Toxicity of atmospheric aerosols on marine phytoplankton

    PubMed Central

    Paytan, Adina; Mackey, Katherine R. M.; Chen, Ying; Lima, Ivan D.; Doney, Scott C.; Mahowald, Natalie; Labiosa, Rochelle; Post, Anton 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. PMID:19273845

  16. 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.

  17. Toxicity of atmospheric aerosols on marine phytoplankton.

    PubMed

    Paytan, Adina; Mackey, Katherine R M; Chen, Ying; Lima, Ivan D; Doney, Scott C; Mahowald, Natalie; Labiosa, Rochelle; Post, Anton F

    2009-03-24

    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. PMID:19273845

  18. FOURIER TRANSFORM INFRARED SPECTROMETRY OF AMBIENT AEROSOLS

    EPA Science Inventory

    Fourier transform infrared (FTIR) spectrometry has been evaluated as a method for determining the concentration of selected species present in ambient aerosols collected on Teflon filters. The filters are analyzed by transmission measurements after collection of the fine fraction...

  19. 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.

  20. Atmospheric Aerosols

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Lawless, James G. (Technical Monitor)

    1994-01-01

    Aerosols, defined as particles and droplets suspended in air, are always present in the atmosphere. They are part of the earth-atmosphere climate system, because they interact with both incoming solar and outgoing terrestrial radiation. They do this directly through scattering and absorption, and indirectly through effects on clouds. Submicrometer aerosols usually predominate in terms of number of particles per unit volume of air. They have dimensions close to the wavelengths of visible light, and thus scatter radiation from the sun very effectively. They are produced in the atmosphere by chemical reactions of sulfur-, nitrogen- and carbon-containing gases of both natural and anthropogenic origins. Light absorption is dominated by particles containing elemental carbon (soot), produced by incomplete combustion of fossil fuels and by biomass burning. Light-scattering dominates globally, although absorption can be significant at high latitudes, particularly over highly reflective snow- or ice-covered surfaces. Other aerosol substances that may be locally important are those from volcanic eruptions, wildfires and windblown dust.

  1. 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.

  2. 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.

  3. 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

  4. 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

  5. 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

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. SAMPLING AND ANALYSIS OF ATMOSPHERIC SULFATES AND RELATED SPECIES

    EPA Science Inventory

    Sampling and analytical methods to measure atmospheric concentrations of sulfur, sulfates and related species are compared for aerosols collected in New York City, Philadelphia, PA., South Charleston, WV., St. Louis, MO., Glendora, CA., and Portland, OR. For the aerosol sampling,...

  12. 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

  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. 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%.

  15. Cloud Forming Potential of Aminium Carboxylate Aerosols

    NASA Astrophysics Data System (ADS)

    Gomez Hernandez, M. E.; McKeown, M.; Taylor, N.; Collins, D. R.; Lavi, A.; Rudich, Y.; Zhang, R.

    2014-12-01

    Atmospheric aerosols affect visibility, air quality, human health, climate, and in particular the aerosol direct and indirect forcings represent the largest uncertainty in climate projections. In this paper, we present laboratory measurements of the hygroscopic growth factors (HGf) and cloud condensation nuclei (CCN) activity of a series of aminium carboxylate salt aerosols, utilizing a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) coupled to a Condensation Particle Counter (CPC) and a CCN counter. HGf measurements were conducted for size-selected aerosols with diameters ranging from 46 nm to 151 nm and at relative humidity (RH%) values ranging from 10 to 90%. In addition, we have calculated the CCN activation diameters for the aminium carboxylate aerosols and derived the hygroscopicity parameter (k or kappa) values for all species using three methods, i.e., the mixing rule approximation, HGf, and CCN results. Our results show that variations in the ratio of acid to base directly affect the activation diameter, HGf, and (k) values of the aminium carboxylate aerosols. Atmospheric implications of the variations in the chemical composition of aminium carboxylate aerosols on their cloud forming potential will be discussed.

  16. 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...

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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

  3. Tropopsheric Aerosol Chemistry via Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Worsnop, Douglas

    2008-03-01

    A broad overview of size resolved aerosol chemistry in urban, rural and remote regions is evolving from deployment of aerosol mass spectrometers (AMS) throughout the northern hemisphere. Using thermal vaporization and electron impact ionization as universal detector of non-refractory inorganic and organic composition, the accumulation of AMS results represent a library of mass spectral signatures of aerosol chemistry. For organics in particular, mass spectral factor analysis provides a procedure for classifying (and simplifying) complex mixtures composed of the hundreds or thousands of individual compounds. Correlations with parallel gas and aerosol measurements (e.g. GC/MS, HNMR, FTIR) supply additional chemical information needed to interpret mass spectra. The challenge is to separate primary and secondary; anthropogenic, biogenic and biomass burning sources - and subsequent - transformations of aerosol chemistry and microphysics.

  4. 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...

  5. 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

  6. In Situ Chemical Characterization of Organic Aerosol Surfaces using Direct Analysis in Real Time

    NASA Astrophysics Data System (ADS)

    Chan, M.; Nah, T.; Wilson, K. R.

    2012-12-01

    Obtaining in situ information on the molecular composition of atmospheric aerosol is important for understanding the sources, formation mechanisms, aging and physiochemical properties of atmospheric aerosol. Most recently, we have used Direct Analysis in Real Time (DART), which is a "soft" atmospheric pressure ionization technique, for in situ chemical characterization of a variety of laboratory generated organic aerosol and heterogeneous processing oleic acid aerosol. A stream of aerosol particles is crossed with a thermal flow of metastable He atoms (produced by the DART source) in front of an inlet of a mass spectrometer. The thermally desorbed analytes are subsequently ionized with minimal fragmentation by reactive species in the DART ionization source (e.g., metastable He atoms). The ion signal scales with the aerosol surface area rather than aerosol volume, suggesting that aerosol particles are not completely vaporized in the ionization region. The DART can thus measure the chemical composition as a function of aerosol depth. Probing aerosol depth is determined by the thermal desorption rates of aerosol particles. Here, we investigate how the experimental parameters (e.g., DART gas temperature and residence time) and the physiochemical properties of aerosol particles (e.g., enthalpy of vaporization) affect the probing aerosol depth and the desorption-ionization mechanism of aerosol particles in the DART using a series of model organic compounds. We also demonstrate the potential application of DART for in situ chemically analyzing wet aerosol particles undergoing oxidation reactions.

  7. Aerosol variability and weather regimes over the Mediterranean region

    NASA Astrophysics Data System (ADS)

    Nabat, Pierre; Somot, Samuel; Mallet, Marc; Michou, Martine

    2015-04-01

    The Mediterranean region is characterized by the accumulation of aerosols from different sources: industrial and urban aerosols from Europe and North African towns, biomass burning, from Eastern Europe, dust aerosols from Africa, and marine particles from the sea. These aerosols show a strong spatio-temporal variability and a resulting large variety in aerosol optical properties over this basin. Maximal aerosol loads are observed in spring and summer, namely in the dry season favouring a longer residence time for atmospheric aerosols. Besides, dust outbreaks characterized by large plumes of Saharan desert dust particles, are more frequent in this season. This study realized in the framework of the ChArMEx initiative aims at explaining this aerosol variability and the relationship between aerosol loads and weather conditions. We consider here an approach based on weather regimes and regional modeling. From a multi-year (1979-2013) regional simulation carried out with the ALADIN-climate model (50 km resolution, ERA-Interim forcing) including an interactive aerosol scheme for the main species present in this region (desert dust, sea-salt, sulfates and carbonaceous particles), we have identified typical synoptic conditions that favour high aerosol loads over the Mediterranean, or on the contrary that are opposed to these high aerosol loads. These weather regimes are based on a statistical method of automated classification realized from surface pressure data. They are also related to the North Atlantic Oscillation (NAO). In this work, we characterize the presence of the different aerosol types over the Mediterranean for each weather regime, as well as their effects on climate. Thus, anomalies in the occurrence of the regimes favourable to high aerosol loads could explain the frequent dust outbreaks observed during the ChArMEx campaigns in 2012 and 2013.

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

    PubMed

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

    2016-04-01

    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 10(7)CFU of fungi/m(3)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

  9. 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

  10. Anomalies of the Asian Monsoon Induced by Aerosol Forcings

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

    Impacts of aerosols on the Asian summer monsoon are studied using the NASA finite volume General Circulation Model (fvGCM), with radiative forcing derived from three-dimensional distributions of five aerosol species i.e., black carbon, organic carbon, soil dust, and sea salt from the Goddard Chemistry Aerosol Radiation and Transport Model (GOCART). 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 & early onset of the Indian summer monsoon. Absorbing aerosols also I i enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface' temperature cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.

  11. Chemistry of organic aerosol formation in urban atmospheres. Final report

    SciTech Connect

    Seinfeld, J.H.; Flagan, R.C.

    1994-04-04

    Aerosol formation from the photooxidation of A-pinene/NOx and B-pinene/NOx mixtures has been investigated in a series of outdoor smog chamber experiments. Both hydrocarbons are potent aerosol formers and in areas containing significant vegetation, terpenes are estimated to be a significant contributor to secondary organic aerosol formation. To model organic aerosol formation, estimates of the vapor pressures of the condensable species are needed. To measure the vapor pressures of the low volatility species characteristic of organic aerosols the Tandem Differential Mobility Analyzer (TDMA) method introduced by Liu and McMurray has been further developed for this task. Initial experiments with compounds of known vapor pressure confirm the usefulness of the method.

  12. 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.

  13. 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

  14. 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.

  15. 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

  16. Mixing states of aerosols over four environmentally distinct atmospheric regimes in Asia: coastal, urban, and industrial locations influenced by dust.

    PubMed

    Ramachandran, S; Srivastava, Rohit

    2016-06-01

    Mixing can influence the optical, physical, and chemical characteristics of aerosols, which in turn can modify their life cycle and radiative effects. Assumptions on the mixing state can lead to uncertain estimates of aerosol radiative effects. To examine the effect of mixing on the aerosol characteristics, and their influence on radiative effects, aerosol mixing states are determined over four environmentally distinct locations (Karachi, Gwangju, Osaka, and Singapore) in Asia, an aerosol hot spot region, using measured spectral aerosol optical properties and optical properties model. Aerosol optical depth (AOD), single scattering albedo (SSA), and asymmetry parameter (g) exhibit spectral, spatial, and temporal variations. Aerosol mixing states exhibit large spatial and temporal variations consistent with aerosol characteristics and aerosol type over each location. External mixing of aerosol species is unable to reproduce measured SSA over Asia, thus providing a strong evidence that aerosols exist in mixed state. Mineral dust (MD) (core)-Black carbon (BC) (shell) is one of the most preferred aerosol mixing states. Over locations influenced by biomass burning aerosols, BC (core)-water soluble (WS, shell) is a preferred mixing state, while dust gets coated by anthropogenic aerosols (BC, WS) over urban regions influenced by dust. MD (core)-sea salt (shell) mixing is found over Gwangju corroborating the observations. Aerosol radiative forcing exhibits large seasonal and spatial variations consistent with features seen in aerosol optical properties and mixing states. TOA forcing is less negative/positive for external mixing scenario because of lower SSA. Aerosol radiative forcing in Karachi is a factor of 2 higher when compared to Gwangju, Osaka, and Singapore. The influence of g on aerosol radiative forcing is insignificant. Results emphasize that rather than prescribing one single aerosol mixing state in global climate models regionally and temporally varying aerosol

  17. 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.

  18. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

    Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

  20. 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.

  1. 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

  2. Online Aerosol Size and Composition Measurements in Coastal Antarctica

    NASA Astrophysics Data System (ADS)

    DeCarlo, P. F.; Giordano, M.; Kalnajs, L.; Johnson, A.; Davis, S. M.; Deshler, T.; Toohey, D. W.

    2014-12-01

    Aerosol particles play a critical role in the chemical and radiative balance of the Antarctic atmosphere. Aerosols are both a source and sink of gas phase constituents, as well as a transport mechanism for oceanic chemical species into the continental interior. The interaction between aerosols, the gas phase, sea ice and the snow pack is complex and not well understood. Recent observations of ozone depletion events coupled with submicron aerosol mass increase highlight the interaction between the gas and particle phases. These interactions can lead to aerosol formation as well as the deposition of trace elements to the snow pack. To determine the composition and source regions of aerosols in the coastal Antarctic atmosphere, a suite of instruments was deployed in the 2014 Antarctic measurement season including a High Resolution Aerodyne Aerosol Mass Spectrometer (HR-AMS), Ultra High Sensitivity Aerosol Spectrometer (UHSAS), Ozone analyzer, Scanning Electrical Mobility Sizer (SEMS), and Particle-into-Liquid Sampler (PILS). Measurements of gas phase constituents and aerosol composition were interpreted in the context of back trajectories and local meteorological conditions to link the measured air masses to their source regions.

  3. 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.

  4. 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.

  5. Iodine speciation in rain, snow and aerosols

    NASA Astrophysics Data System (ADS)

    Gilfedder, B. S.; Lai, S. C.; Petri, M.; Biester, H.; Hoffmann, T.

    2008-10-01

    Iodine oxides, such as iodate, should be the only thermodynamically stable sink species for iodine in the troposphere. However, field observations have increasingly found very little iodate and significant amounts of iodide and soluble organically bound iodine (SOI) in precipitation and aerosols. The aim of this study was to investigate iodine speciation, including the organic fraction, in rain, snow, and aerosols in an attempt to further clarify aqueous phase iodine chemistry. Diurnal aerosol samples were taken with a 5 stage cascade impactor and a virtual impactor (PM2.5) from the Mace Head research station, Ireland, during summer 2006. Rain was collected from Australia, New Zealand, Patagonia, Germany, Ireland, and Switzerland and snow was obtained from Greenland, Germany, Switzerland, and New Zealand. Aerosols were extracted from the filters with water and all samples were analysed for total soluble iodine (TSI) by inductively coupled plasma mass spectrometry (ICP-MS) and iodine speciation was determined by coupling an ion chromatography unit to the ICP-MS. The median concentration of TSI in aerosols from Mace Head was 222 pmol m-3 (summed over all impactor stages) of which the majority was associated with the SOI fraction (median day: 90±4%, night: 94±2% of total iodine). Iodide exhibited higher concentrations than iodate (median 6% vs. 1.2% of total iodine), and displayed significant enrichment during the day compared to the night. Interestingly, up to 5 additional, presumably anionic iodo-organic peaks were observed in all IC-ICP-MS chromatograms, composing up to 15% of the TSI. Soluble organically bound iodine was also the dominant fraction in all rain and snow samples, with lesser amounts of iodide and iodate (iodate was particularly low in snow). Two of the same unidentified peaks found in aerosols were also observed in precipitation from both Southern and Northern Hemispheres. This suggests that these species are transferred from the aerosols into

  6. 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.

  7. 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.

  8. Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008)

    NASA Astrophysics Data System (ADS)

    Lee, B. H.; Kostenidou, E.; Hildebrandt, L.; Riipinen, I.; Engelhart, G. J.; Mohr, C.; Decarlo, P. F.; Mihalopoulos, N.; Prevot, A. S. H.; Baltensperger, U.; Pandis, S. N.

    2010-07-01

    A variable residence time thermodenuder (TD) was combined with an Aerodyne Aerosol Mass Spectrometer (AMS) and a Scanning Mobility Particle Sizer (SMPS) to measure the volatility distribution of aged organic aerosol in the Eastern Mediterranean during the Finokalia Aerosol Measurement Experiment in May of 2008 (FAME-2008). A new method for the quantification of the organic aerosol volatility distribution was developed combining measurements of all three instruments together with an aerosol dynamics model. Challenges in the interpretation of ambient thermodenuder-AMS measurements include the potential resistances to mass transfer during particle evaporation, the effects of particle size on the evaporated mass fraction, the changes in the AMS collection efficiency and particle density as the particles evaporate partially in the TD, and finally potential losses inside the TD. Our proposed measurement and data analysis method accounts for all of these problems combining the AMS and SMPS measurements. The AMS collection efficiency of the aerosol that passed through the TD was found to be approximately 10% lower than the collection efficiency of the aerosol that passed through the bypass. The organic aerosol measured at Finokalia is approximately 2 orders of magnitude less volatile than fresh laboratory-generated biogenic secondary organic aerosol. This low volatility is consistent with its highly oxygenated AMS mass spectrum. The results are found to be highly sensitive to the mass accommodation coefficient of the evaporating species.

  9. 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.

  10. 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.

  11. HOUSTON AEROSOL CHARACTERIZATION STUDY

    EPA Science Inventory

    An intensive field study of ambient aerosols was conducted in Houston between September 14 and October 14, 1978. Measurements at 12 sites were made using (1) two relocatable monitoring systems instrumented for aerosol and gaseous pollutants, (2) a network of high volume samplers ...

  12. 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, ...

  13. 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.

  14. 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.

  15. 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

  16. 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.

  17. 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.

  18. A bio-aerosol detection technique based on tryptophan intrinsic fluorescence measurement

    NASA Astrophysics Data System (ADS)

    Cai, Shuyao; Zhang, Pei; Zhu, Linglin; Zhao, Yongkai; Huang, Huijie

    2011-12-01

    Based on the measurement of intrinsic fluorescence, a set of bio-aerosol including virus aerosols detection instrument is developed, with which a method of calibration is proposed using tryptophan as the target. The experimental results show a good linear relationship between the fluorescence voltage of the instrument and the concentration of the tryptophan aerosol. An excellent correlation (R2>=0.99) with the sensitivity of 4000PPL is obtained. The research demonstrates the reliability of the bio-aerosol detection by measuring the content of tryptophan. Further more the feasibility of prejudgment to the species of bio-aerosol particles with the multi-channel fluorescence detection technology is discussed.

  19. Research on bio-aerosol monitoring based on normalized fluorescence voltage

    NASA Astrophysics Data System (ADS)

    Zhang, Pei; Zhao, Yongkai; Xiao, Yanfen; Cai, Shuyao; Huang, Huijie

    2011-12-01

    An optical detecting technique to identify bio-aerosol particles is proposed in this paper by normalized fluorescence value which correlates to its size and intrinsic fluorescence. With the bio-aerosol detecting system developed, we test and analyze three types of aerosols, while each of them contains fluorescent microspheres of a certain size. The result indicates that different fluorescent microspheres containing the same fluorescent substances have the same normalized fluorescence voltage to unit particle size in diameter. The normalized fluorescence value of other species aerosols is tested for comparing. The research results can be applied to identification of bio-aerosols preliminarily.

  20. 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.

  1. 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.

  2. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGESBeta

    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

  3. 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

  4. 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.

  5. 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.

  6. 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.

  7. Gas/Aerosol partitioning: a simplified method for global modeling

    NASA Astrophysics Data System (ADS)

    Metzger, S. M.

    2000-09-01

    sources. This is, for example, the case for ammonium nitrate originating from gas-to-particle conversion over northern India. Our model results indicate that these particles, through convective redistribution, can be transported at altitudes of 200-300 hPa as far as Europe during the Indian summer monsoon. Verification of these results, however, would require aircraft measurements, which are presently not available. Comparison with ground-based measurements indicates that the simplified aerosol module coupled to a global atmospheric chemistry model (TM3), for the considered ammonium/sulfate/nitrate/water system, yields realistic results at locations where ammonium nitrate is important. For remote locations, the comparison also indicates that it is important to account for other aerosol species such as sea salt and mineral dust. Although these compounds have not (yet) been included in the global gas/aerosol partitioning calculations with TM3, it seems to be possible to consider them with our simplified approach, as indicated by the results of box-model calculations.

  8. The importance of aerosol composition and mixing state on predicted CCN concentration and the variation of the importance with atmospheric processing of aerosol

    SciTech Connect

    Wang, J.; Cubison, M.; Aiken, A.; Jimenez, J.; Collins, D.; Gaffney, J.; Marley, N.

    2010-03-15

    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 are complex and heterogeneous mixtures 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 and mixing state are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban super-site in Mexico City during MILAGRO are analyzed. 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 biases associated with these simplifications are compared for different supersaturations, and the variation of the biases is examined as a function of aerosol age. The results show that the simplification of internally mixed, size

  9. 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.

  10. Secondary organic material formed by methylglyoxal in aqueous aerosol mimics - Part 2: Product identification using Aerosol-CIMS

    NASA Astrophysics Data System (ADS)

    Sareen, N.; Shapiro, E. L.; Schwier, A. N.; McNeill, V. F.

    2009-07-01

    We used chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol-CIMS) to characterize secondary organic material formed by methylglyoxal with ammonium sulfate in aqueous aerosol mimics. Bulk reaction mixtures were diluted and atomized to form submicron aerosol particles. Organics were detected using Aerosol-CIMS in positive and negative ion mode using I- and H3O+·(H2O)n as reagent ions. The results are consistent with aldol condensation products, carbon-nitrogen species, sulfur-containing compounds, and oligomeric species up to 759 amu. These results support previous observations by us and others that ammonium sulfate plays a critical role in the SOA formation chemistry of dicarbonyl compounds.

  11. 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.

  12. Temporal variation of aerosol properties at a rural continental site and study of aerosol evolution through growth law analysis

    NASA Astrophysics Data System (ADS)

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

    2006-09-01

    Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) on board 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 m. 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.

  13. 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.

  14. 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.

  15. 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.

  16. Aerosol lenses propagation model.

    PubMed

    Tremblay, Grégoire; Roy, Gilles

    2011-09-01

    We propose a model based on the properties of cascading lenses modulation transfer function (MTF) to reproduce the irradiance of a screen illuminated through a dense aerosol cloud. In this model, the aerosol cloud is broken into multiple thin layers considered as individual lenses. The screen irradiance generated by these individual layers is equivalent to the point-spread function (PSF) of each aerosol lens. Taking the Fourier transform of the PSF as a MTF, we cascade the lenses MTF to find the cloud MTF. The screen irradiance is found with the Fourier transform of this MTF. We show the derivation of the model and we compare the results with the Undique Monte Carlo simulator for four aerosols at three optical depths. The model is in agreement with the Monte Carlo for all the cases tested. PMID:21886230

  17. Susceptibility of Stored-Product Psocids to Aerosol Insecticides

    PubMed Central

    Opit, George P.; Arthur, Frank H.; Throne, James E.; Payton, Mark E.

    2012-01-01

    The efficacies of commercial methoprene and esfenvalerate aerosols for control of stored-product psocid pests were evaluated in simulated field studies. The efficacies of methoprene, esfenvalerate EC, the carrier Isopar-M™, and a combination of methoprene and esfenvalerate aerosols for control of Liposcelis decolor (Pearman) (Psocoptera: Liposcelididae) and Liposcelis entomophila (Enderlein) nymphs were assessed, and the effects of direct and indirect exposure of Liposcelis bostrychophila Badonnel, L. decolor, and Liposcelis paeta Pearman adults to esfenvalerate EC aerosol were evaluated. The greatest nymphal mortality attained was 76%, indicating that the four aerosols tested were ineffective against L. decolor and L. entomophila nymphs. In the direct and indirect exposure studies, the greatest adult mortalities attained for the three psocid species were 62 and 32%, respectively. Based on these data, esfenvalerate aerosol is ineffective for control of L. bostrychophila, L. decolor, L. entomophila, and L. paeta psocid species. This study shows that methoprene, esfenvalerate EC, and a combination of methoprene and esfenvalerate aerosols were ineffective against the four psocid species tested when applied at rates that are usually effective against other stored-product insect pests. PMID:23463916

  18. 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.

  19. Secondary organic material formed by methylglyoxal in aqueous aerosol mimics

    NASA Astrophysics Data System (ADS)

    Sareen, N.; Schwier, A. N.; Shapiro, E. L.; Mitroo, D.; McNeill, V. F.

    2010-02-01

    We show that methylglyoxal forms light-absorbing secondary organic material in aqueous ammonium sulfate and ammonium nitrate solutions mimicking tropospheric aerosol particles. The kinetics were characterized using UV-Vis spectrophotometry. The results suggest that the bimolecular reaction of methylglyoxal with an ammonium or hydronium ion is the rate-limiting step for the formation of light-absorbing species, with kNH4+II=5×10-6 M-1 min-1 and kH3O+II≤10-3 M-1 min-1. Evidence of aldol condensation products and oligomeric species up to 759 amu was found using chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol-CIMS). Tentative identifications of carbon-nitrogen species and a sulfur-containing compound were also made using Aerosol-CIMS. Aqueous solutions of methylglyoxal, with and without inorganic salts, exhibit significant surface tension depression. These observations add to the growing body of evidence that dicarbonyl compounds may form secondary organic material in the aerosol aqueous phase, and that secondary organic aerosol formation via heterogeneous processes may affect seed aerosol properties.

  20. Susceptibility of stored-product psocids to aerosol insecticides.

    PubMed

    Opit, George P; Arthur, Frank H; Throne, James E; Payton, Mark E

    2012-01-01

    The efficacies of commercial methoprene and esfenvalerate aerosols for control of stored-product psocid pests were evaluated in simulated field studies. The efficacies of methoprene, esfenvalerate EC, the carrier Isopar-M™, and a combination of methoprene and esfenvalerate aerosols for control of Liposcelis decolor (Pearman) (Psocoptera: Liposcelididae) and Liposcelis entomophila (Enderlein) nymphs were assessed, and the effects of direct and indirect exposure of Liposcelis bostrychophila Badonnel, L. decolor, and Liposcelis paeta Pearman adults to esfenvalerate EC aerosol were evaluated. The greatest nymphal mortality attained was 76%, indicating that the four aerosols tested were ineffective against L. decolor and L. entomophila nymphs. In the direct and indirect exposure studies, the greatest adult mortalities attained for the three psocid species were 62 and 32%, respectively. Based on these data, esfenvalerate aerosol is ineffective for control of L. bostrychophila, L. decolor, L. entomophila, and L. paeta psocid species. This study shows that methoprene, esfenvalerate EC, and a combination of methoprene and esfenvalerate aerosols were ineffective against the four psocid species tested when applied at rates that are usually effective against other stored-product insect pests. PMID:23463916

  1. Secondary organic aerosol in the global aerosol - chemical transport model Oslo CTM2

    NASA Astrophysics Data System (ADS)

    Hoyle, C. R.; Berntsen, T.; Myhre, G.; Isaksen, I. S. A.

    2007-11-01

    The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA). Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics). A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr-1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA) values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA) is the dominant OA component) than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%-60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes. Reducing the yield

  2. 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

  3. 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

  4. Online Simulations and Forecasts of the Global Aerosol Distribution in the NASA GEOS-5 Model

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2006-01-01

    We present an analysis of simulations of the global aerosol system in the NASA GEOS-5 transport, radiation, and chemistry model. The model includes representations of all major tropospheric aerosol species, including dust, sea salt, black carbon, particulate organic matter, and sulfates. The aerosols are run online for the period 2000 through 2005 in a simulation driven by assimilated meteorology from the NASA Goddard Data Assimilation System. Aerosol surface mass concentrations are compared with existing long-term surface measurement networks. Aerosol optical thickness is compared with ground-based AERONET sun photometry and space-based retrievals from MODIS, MISR, and OMI. Particular emphasis is placed here on consistent sampling of model and satellite aerosol optical thickness to account for diurnal variations in aerosol optical properties. Additionally, we illustrate the use of this system for providing chemical weather forecasts in support of various NASA and community field missions.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. Aerosol Radiative Forcing over North India during Pre-Monsoon Season using WRF-Chem

    NASA Astrophysics Data System (ADS)

    Misra, A.; Kumar, K.; Michael, M.; Tripathi, S. N.

    2013-12-01

    Study of aerosols is important for a fair understanding of the Earth climate system. This requires knowledge of the physical, chemical, optical, and morphological properties of aerosols. Aerosol radiative forcing provides information on the effect of aerosols on the Earth radiation budget. Radiative forcing estimates using model data provide an opportunity to examine the contribution of individual aerosol species to overall radiative forcing. We have used Weather Research and Forecast with Online Chemistry (WRF-Chem) derived aerosol concentration data to compute aerosol radiative forcing over north India during pre-monsoon season of 2008, 2009, and 2010. WRF-Chem derived mass concentrations are converted to number concentrations using standard procedure. Optical Properties of Aerosol and Cloud (OPAC) software package is used to compute extinction and scattering coefficients, and asymmetry parameter. Computations are performed at different altitudes and the obtained values are integrated to get the column optical properties. Santa Barbara Discrete Ordinate Radiative Transfer (SBDART) model is used to calculate the radiative forcing at surface and top-of-atmosphere. Higher values of aerosol radiative forcing are observed over desert region in western Indian state of Rajasthan, and Punjab of Pakistan. Contribution of individual aerosol species to atmospheric radiative forcing is also assessed. Dust radiative forcing is high over western India. Radiative forcing due to BC and water-soluble (WASO) aerosols are higher over north-west Indian states of Punjab and Haryana, and the Indo-Gangetic Basin. A pool of high WASO optical depth and radiative forcing is observed over the Indo-Bangladesh border. The findings of aerosol optical depth and radiative forcing are consistent with the geography and prevailing aerosol climatology of various regions. Heating rate profiles due to total aerosols and only due to BC have been evaluated at selected stations in north India. They show

  10. 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

  11. AEROSOL CHARACTERIZATION WITH CENTRIFUCAL AEROSOL SPECTROMETERS: THEORY AND EXPERIMENT

    EPA Science Inventory

    A general mathematical model describing the motion of particles in aerosol centrifuges has been developed. t has been validated by comparisons of theoretically predicted calibration sites with experimental data from tests sizing aerosols in instruments of three different spiral d...

  12. 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.

  13. Introduction of the aerosol feedback process in the model BOLCHEM

    NASA Astrophysics Data System (ADS)

    Russo, Felicita; Maurizi, Alberto; D'Isidoro, Massimo; Tampieri, Francesco

    2010-05-01

    The effect of aerosols on the climate is still one of the least understood processes in the atmospheric science. The use of models to simulate the interaction between aerosols and climate can help understanding the physical processes that rule this interaction and hopefully predicting the future effects of anthropogenic aerosols on climate. In particular regional models can help study the effect of aerosols on the atmospheric dynamics on a local scale. In the work performed here we studied the feedback of aerosols in the radiative transfer calculation using the regional model BOLCHEM. The coupled meteorology-chemistry model BOLCHEM is based on the BOLAM meteorological model. The BOLAM dynamics is based on hydrostatic primitive equations, with wind components u and v, potential temperature ?, specific humidity q, surface pressure ps, as dependent variables. The vertical coordinate σ is terrain-following with variables distributed on a non-uniformly spaced staggered Lorentz grid. In the standard configuration of the model a collection of climatological aerosol optical depth values for each aerosol species is used for the radiative transfer calculation. In the feedback exercise presented here the aerosol optical depth was calculated starting from the modeled aerosol concentrations using an approximate Mie formulation described by Evans and Fournier (Evans, B.T.N. and G.R. Fournier, Applied Optics, 29, 1990). The calculation was done separately for each species and aerosol size distribution. The refractive indexes for the different species were taken from P. Stier's work (P. Stier et al., Atmos. Chem. Phys., 5, 2005) and the aerosol extinction obtained by Mie calculation were compared with the results reported by OPAC (M. Hess et al., Bull. Am. Met. Soc., 79, 1998). Two model runs, with and without the aerosol feedback, were performed to study the effects of the feedback on meteorological parameters. As a first setup of the model runs we selected a domain over the

  14. Prospects of real-time single-particle biological aerosol analysis: A comparison between laser-induced breakdown spectroscopy and aerosol time-of-flight mass spectrometry

    NASA Astrophysics Data System (ADS)

    Beddows, D. C. S.; Telle, H. H.

    2005-08-01

    In this paper we discuss the prospects of real-time, in situ laser-induced breakdown spectroscopy applied for the identification and classification of bio-aerosols (including species of potential bio-hazard) within common urban aerosol mixtures. In particular, we address the issues associated with the picking out of bio-aerosols against common background aerosol particles, comparing laser-induced breakdown spectroscopy measurements with data from a mobile single-particle aerosol mass spectrometer (ATOFMS). The data from the latter provide statistical data over an extended period of time, highlighting the variation of the background composition. While single-particle bio-aerosols are detectable in principle, potential problems with small (˜ 1 μm size) bio-aerosols have been identified; constituents of the air mass other than background aerosols, e.g. gaseous CO 2 in conjunction with common background aerosols, may prevent unique recognition of the bio-particles. We discuss whether it is likely that laser-induced breakdown spectroscopy on its own can provide reliable, real-time identification of bio-aerosol in an urban environment, and it is suggested that more than one technique should be or would have to be used. A case for using a combination of laser-induced breakdown spectroscopy and Raman (and/or) laser-induced fluorescence spectroscopy is made.

  15. The organic aerosols of Titan

    NASA Technical Reports Server (NTRS)

    Khare, B. N.; Sagan, C.; Thompson, W. R.; Arakawa, E. T.; Suits, F.; Callcott, T. A.; Williams, M. W.; Shrader, S.; Ogino, H.; Willingham, T. O.

    1984-01-01

    The optical properties and chemical composition of thiolin, an organic solid synthesized by high-energy-electron irradiation in a plasma discharge (Sagan et al., 1984) to simulate the high-altitude aerosols of Titan, are investigated experimentally using monochromators, ellipsometers, and spectrometers (on thin films deposited by continuous dc discharge) and sequential and nonsequential pyrolytic gas chromatography/mass spectrometry (of the volatile component), respectively. The results are presented in tables and graphs and characterized. The real and imaginary elements of the complex refractive index in the visible are estimated as 1.65 and 0.004-0.08, respectively, in agreement with observations of Titan, and the IR absorption features include the nitrile band at 4.6 microns. The molecules identified in the volatile part of thiolin include complex species considered important in theoretical models of the origin of life on earth.

  16. 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.

  17. 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

  18. 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.

  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. 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.

  1. 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.

  2. Aerosol chemistry in GLOBE

    NASA Technical Reports Server (NTRS)

    Clarke, Antony D.; Rothermel, Jeffry; Jarzembski, Maurice A.

    1993-01-01

    This task addresses the measurement and understanding of the physical and chemical properties of aerosol in remote regions that are responsible for aerosol backscatter at infrared wavelengths. Because it is representative of other clean areas, the remote Pacific is of extreme interest. Emphasis is on the determination size dependent aerosol properties that are required for modeling backscatter at various wavelengths and upon those features that may be used to help understand the nature, origin, cycling and climatology of these aerosols in the remote troposphere. Empirical relationships will be established between lidar measurements and backscatter derived from the aerosol microphysics as required by the NASA Doppler Lidar Program. This will include the analysis of results from the NASA GLOBE Survey Mission Flight Program. Additional instrument development and deployment will be carried out in order to extend and refine this data base. Identified activities include participation in groundbased and airborne experiments. Progress to date includes participation in, analysis of, and publication of results from Mauna Loa Backscatter Intercomparison Experiment (MABIE) and Global Backscatter Experiment (GLOBE).

  3. 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.

  4. SURVIVAL OF BACTERIA DURING AEROSOLIZATION

    EPA Science Inventory

    One form of commercial application of microorganisms, including genetically engineered microorganisms is as an aerosol. To study the effect of aerosol-induced stress on bacterial survival, nonrecombinant spontaneous antibiotic-resistant mutants of four organisms, Enterobacter clo...

  5. Other medications for aerosol delivery.

    PubMed

    Rubin, Bruce K

    2006-01-01

    Although aerosol therapy is most commonly used to treat asthma and COPD, there are a large number of aerosol medications now used or in development for other diseases. Mucoactive agents have long been available by aerosol, but now we have truly effective drugs to improve effective airway clearance including dornase alfa, hyperosmolar saline, and aerosol surfactant. Inhaled antibiotics are available for the treatment of cystic fibrosis, bronchiectasis and other chronic airway infections. With the development of devices that can target aerosol to the deep lung, the opportunity to deliver medications systemically by the aerosol route has become a reality. Insulin, recently approved in the US as aerosol therapy, and other peptides are systemically absorbed from the distal airway and alveolus. Aerosol gene transfer therapy to correct abnormalities associated with cystic fibrosis, primary ciliary dyskinesia and other airway diseases also holds great potential. PMID:16798603

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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 ...

  12. 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.

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

    PubMed

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

    2016-03-25

    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. PMID:27013731

  14. Rethinking organic aerosols: semivolatile emissions and photochemical aging.

    PubMed

    Robinson, Allen L; Donahue, Neil M; Shrivastava, Manish K; Weitkamp, Emily A; Sage, Amy M; Grieshop, Andrew P; Lane, Timothy E; Pierce, Jeffrey R; Pandis, Spyros N

    2007-03-01

    Most primary organic-particulate emissions are semivolatile; thus, they partially evaporate with atmospheric dilution, creating substantial amounts of low-volatility gas-phase material. Laboratory experiments show that photo-oxidation of diesel emissions rapidly generates organic aerosol, greatly exceeding the contribution from known secondary organic-aerosol precursors. We attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species. Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations. Controlling organic particulate-matter concentrations will require substantial changes in the approaches that are currently used to measure and regulate emissions. PMID:17332409

  15. Mexico City Aerosol Transect

    NASA Astrophysics Data System (ADS)

    Lewandowski, P. A.; Eichinger, W. E.; Prueger, J.; Holder, H. L.

    2007-12-01

    A radiative impact study was conducted in Mexico City during MILAGRO/MIRAGE campaign in March of 2006. On a day when the predominant wind was from the north to the south, authors measured radiative properties of the atmosphere in six locations across the city ranging from the city center, through the city south limits and the pass leading out of the city (causing pollutants to funnel through the area). A large change in aerosol optical properties has been noticed. The aerosol optical depth has generally increased outside of the city and angstrom coefficient has changed significantly towards smaller values. Aerosol size distribution was calculated using SkyRadPack. The total optical depths allowed coincidental lidar data to calculate total extinction profiles for all the locations for 1064nm.

  16. 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

  17. 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

  18. 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

  19. Aerosol processing of materials: Aerosol dynamics and microstructure evolution

    NASA Astrophysics Data System (ADS)

    Gurav, Abhijit Shankar

    ) via vapor condensation at 400-650sp°C using Nsb2 carrier gas. In general, during laboratory-scale aerosol processing of materials containing a volatile component, significant evaporative losses and formation of new ultrafine particles were observed at synthesis temperatures at which the saturation vapor pressure of the volatile species exceeded about 0.1-0.5 mTorr. Spray calcination synthesis of pigment-size titania from titanium hydrolysate (TiOsb{x}(SOsb4)sb{y}(OH)sb{z}) using fuel additives such as ethyl alcohol, sugar and urea was also investigated. When pure water was used as a medium of suspension, agglomerates of 0.5 to 1.5 mum were produced by spray calcination. Use of pure ethanol as a solvent as well as small amounts (5-10 wt.%) urea additions to the suspension of Ti-hydrolysate in water were successful in producing predominantly unagglomerated, single crystalline titania particles of 0.1 to 0.3 mum size. Such additions of fuels such as alcohols, sugar and urea to suspensions and solutions used in spray processes are promising for making powders having smaller sizes and unagglomerated, denser morphologies.

  20. Global Aerosol Climatology Project.

    NASA Astrophysics Data System (ADS)

    Mishchenko, Michael; Penner, Joyce; Anderson, Donald

    2002-02-01

    This paper is concerned with uncertainties in the Advanced Very High Resolution Radiometer (AVHRR)-based retrieval of optical depth for heavy smoke aerosol plumes generated from forest fires that occurred in Canada due to a lack of knowledge on their optical properties (single-scattering albedo and asymmetry parameter). Typical values of the optical properties for smoke aerosols derived from such field experiments as Smoke, Clouds, and Radiation-Brazil (SCAR-B); Transport and Atmospheric Chemistry near the Equator-Atlantic (TRACE-A); Biomass Burning Airborne and Spaceborne Experiment in the Amazonas (BASE-A); and Boreal Ecosystem-Atmosphere Study (BOREAS) were first assumed for retrieving smoke optical depths. It is found that the maximum top-of-atmosphere (TOA) reflectance values calculated by models with these aerosol parameters are less than observations whose values are considerably higher. A successful retrieval would require an aerosol model that either has a substantially smaller asymmetry parameter (g < 0.4 versus g > 0.5), or higher single-scattering albedo ( 0.9 versus < 0.9), or both (e.g., g = 0.39 and = 0.91 versus g = 0.57 and = 0.87) than the existing models. Several potential causes were examined including small smoke particle size, low black carbon content, humidity effect, calibration errors, inaccurate surface albedo, mixture of cloud and aerosol layers, etc. A more sound smoke aerosol model is proposed that has a lower content of black carbon (mass ratio = 0.015) and smaller size (mean radius = 0.02 m for dry smoke particles), together with consideration of the effect of relative humidity. Ground-based observations of smoke suggest that for < 2.5 there is an increasing trend in and a decreasing trend in g with increases in , which is consistent with the results of satellite retrievals. Using these relationships as constraints, more plausible values of can be obtained for heavy smoke aerosol. The possibility of smoke-cloud mixtures is also

  1. 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.

  2. Highly stable aerosol generator

    DOEpatents

    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.

  3. 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

  4. Impacts of Aminium Sulfates on Atmospheric Aerosol Properties

    NASA Astrophysics Data System (ADS)

    Qiu, C.; Zhang, R.

    2012-12-01

    Atmospheric aerosols influence our environment significantly by interacting with the solar radiation and modifying cloud formation processes. Amines are emitted into the atmosphere from various anthropogenic and biogenic sources. Recent studies have shown that atmospheric amines can enter the particle-phase as salts like aminium sulfates by reacting with aerosol constituents including sulfuric acid and ammonium salts. However, little knowledge is available about the properties of these aminium salts and their impacts on aerosol properties. We have conducted laboratory experiments to measure the hygroscopicity, thermostability, and density of five representative alkylaminium sulfates, using an integrated aerosol analytical system including a tandem differential mobility analyzer and an aerosol particle mass analyzer. When exposed to increasing RH, alkylaminium sulfate aerosols show monotonic growth in size without a well-defined deliquescence point. Aerosols of mixed ammonium-alkylaminium sulfates have deliquescence points lower than that of ammonium sulfate. The measurements of thermostability reveal that dimethylaminium sulfate is the most stable species upon heating. Trimethyl- and triethyl-aminium sulfates volatilize similarly to ammonium sulfate, but exhibit lower volatility than monomethyl- and diethyl-aminium sulfates. The density of alkylaminium sulfates ranges from 1.2 to 1.5 g cm-3, and can be predicted from an empirical model on the basis of the mole ratio of alkyl carbons to total sulfate. Our results suggest that the properties of aerosols may be considerably altered by the incorporation of atmospheric amines through heterogeneous reactions. In particular, these processes may lead to an enhanced water uptake at low RH and considerably change the contribution of aerosols to climate forcing.

  5. 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

  6. 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

  7. Biogenic amines in submicron marine aerosol (Invited)

    NASA Astrophysics Data System (ADS)

    Facchini, M.

    2010-12-01

    Ammonium salts of dimethyl and diethyl amine (DMA+ and DEA+) have been detected in size segregated marine samples collected in the North Atlantic over open ocean and at a coastal site. DMA+ and DEA+ peak in the accumulation mode range while very low concentration, close to detection limit, are observed in the coarse size fractions, as well as in sea spray aerosol artificially generated in the laboratory using sea water. These results indicate a secondary formation pathway. DMA+ and DEA+ represent up to 20% of secondary organic aerosol (SOA) in our samples , and to our knowledge they are the most abundant organic species besides MSA ever detected in clean marine aerosol . Maximum concentrations have been observed during spring and summer when the biological activity is high and in clean marine air masses, thus indicating biogenic sources. Total organic nitrogen (ON) concentration also peaks in the accumulation mode range and represents in our samples a fraction from 32 to 54 % of the total SOA. Ammonium salt formation from biogenic amines might be an important source of marine SOA and atmospheric nitrogen at the global scale with a seasonal variation connected to the oceanic biological productivity and an atmospheric cycle parallel to that of the organosulfur species.

  8. 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.

  9. Contribution of sulfate and organic aerosols to cloud condensation nuclei at Point Reyes, California

    SciTech Connect

    Rivera-Carpio, C.A.; Corrigan, C.E.; Novakov, T.; Penner, J.E.

    1995-12-01

    We have determined mass size distributions of major aerosol species by the Micro Orifice Uniform Deposit Impactor (MOUDI) and simultaneously measured aerosol number size distributions and CCN number concentrations (at 0.5% supersaturation) at a Pacific coastal site (Point Reyes, California). Number size distributions were calculated from the impactor data from which the mass contributions of sulfate, organic, and seasalt aerosols to CCN number concentrations were estimated. The derived and measured size distributions and the derived and measured CCN number concentrations were found to be in good agreement. Our results demonstrate that organic aerosols, depending on the meteorological conditions, may contribute a variable and often dominant fraction to the CCN concentrations.

  10. 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.

  11. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Croft, B.; Lohmann, U.; Martin, R. V.; Stier, P.; Wurzler, S.; Feichter, J.; Hoose, C.; Heikkilä, U.; van Donkelaar, A.; Ferrachat, S.

    2010-02-01

    A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90%) scavenged by cloud nucleation processes for all aerosol species, except for dust (50%). The aerosol number scavenged is primarily (>90%) attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20-30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds), mid

  12. Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Kerminen, V.-M.; Korhonen, H.; Lehtinen, K. J.; Makkonen, R.; Arola, A.; Mielonen, T.; Romakkaniemi, S.; Kulmala, M.; Kokkola, H.

    2011-12-01

    We present the implementation and evaluation of a sectional aerosol microphysics model SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by keeping the number of variables needed to describe the size and composition distribution to the minimum. The aerosol size distribution is described using 20 size sections with 10 size sections in size space which cover diameters ranging from 3 nm to 10 μm divided to three subranges each having distinct optimised process and compound selection. The ability of the module to describe the global aerosol properties was evaluated by comparison against (1) measured continental and marine size distributions, (2) observed variability of continental modal number concentrations, (3) measured sulphate, organic carbon, black carbon and sea salt mass concentrations, (4) observations of AOD and other aerosol optical properties from satellites and AERONET network, (5) global aerosol budgets and concentrations from previous model studies, and (6) model results using M7 which is the default aerosol microphysics module in ECHAM5-HAM. The evaluation shows that the global aerosol properties can be reproduced reasonably well using the coarse resolution of 10 size sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sea salt, sulphate and carbonaceous species have an annual mean within a factor of five of the observations, while the simulated sea salt concentrations reproduce the observations less accurately and show high variability. Regionally, AOD is in relatively good agreement with the observations (within a factor of two). At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and dust regions the modeled AOD is

  13. Aerosol impacts in the Met Office global NWP model

    NASA Astrophysics Data System (ADS)

    Mulcahy, Jane P.; Brooks, Malcolm E.; Milton, Sean F.

    2010-05-01

    carbon, biogenic, sea salt, biomass-burning, mineral dust, and nitrate aerosol particles (Bellouin et al., 2007). As a first step, monthly mean climatologies of these species are implemented in the model. Stage two involves running the CLASSIC scheme in a prognostic mode where the aerosols are fully interactive with the model meteorological and radiation fields. Here we present an evaluation of both stages of the aerosol implementation procedure. An objective verification of the model output fields is carried out against forecast analyses and a wide range of satellite and in situ data. The model aerosol optical depth (AOD) is evaluated against ground-based AERONET observations and satellite aerosol retrievals available through the MACC project (e.g., MODIS, SEVIRI). The impacts on model performance, in terms of the general circulation patterns and in addressing the model radiation biases will also be presented. References: Bellouin, N. et al. (2007), Improved representation of aerosols for HadGEM2, Tech. Note 73, Hadley Centre, Met Office, Exeter, U. K. Cusack, S. et al. (1998), The radiative impact of a simple aerosol climatology on the Hadley Centre atmospheric GCM, Q. J. R. Meteorol. Soc., 124, 2517-2526. Haywood, J. M. et al. (2005), Can desert dust explain the outgoing longwave radiation anomaly over the Sahara during July 2003, J. Geophys. Res. 110, D05105, doi:10.1029/2004JD005232. Milton, S. F. et al. (2008), Modeled and observed atmospheric radiation balance during the West African dry season: Role of mineral dust, biomass burning aerosol and surface albedo, J. Geophys. Res., 113, D00C02, doi:10.1029/2007JD009741.

  14. 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.

  15. 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. __________________________________________________

  16. Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008)

    NASA Astrophysics Data System (ADS)

    Lee, B. H.; Kostenidou, E.; Hildebrandt, L.; Riipinen, I.; Engelhart, G. J.; Mohr, C.; Decarlo, P. F.; Mihalopoulos, N.; Prevot, A. S. H.; Baltensperger, U.; Pandis, S. N.

    2010-12-01

    A variable residence time thermodenuder (TD) was combined with an Aerodyne Aerosol Mass Spectrometer (AMS) and a Scanning Mobility Particle Sizer (SMPS) to measure the volatility distribution of aged organic aerosol in the Eastern Mediterranean during the Finokalia Aerosol Measurement Experiment in May of 2008 (FAME-2008). A new method for the quantification of the organic aerosol volatility distribution was developed combining measurements of all three instruments together with an aerosol dynamics model. Challenges in the interpretation of ambient thermodenuder-AMS measurements include the potential resistances to mass transfer during particle evaporation, the effects of particle size on the evaporated mass fraction, the changes in the AMS collection efficiency and particle density as the particles evaporate partially in the TD, and finally potential losses inside the TD. Our proposed measurement and data analysis method accounts for all of these problems combining the AMS and SMPS measurements. The AMS collection efficiency of the aerosol that passed through the TD was found to be approximately 10% lower than the collection efficiency of the aerosol that passed through the bypass. The organic aerosol measured at Finokalia is approximately 2 or more orders of magnitude less volatile than fresh laboratory-generated monoterpene (α-pinene, β-pinene and limonene under low NOx conditions) secondary organic aerosol. This low volatility is consistent with its highly oxygenated AMS mass spectrum. The results are found to be highly sensitive to the mass accommodation coefficient of the evaporating species. This analysis is based on the assumption that there were no significant reactions taking place inside the thermodenuder.

  17. 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

  18. Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Kerminen, V.-M.; Korhonen, H.; Lehtinen, K. J.; Makkonen, R.; Arola, A.; Mielonen, T.; Romakkaniemi, S.; Kulmala, M.; Kokkola, H.

    2012-06-01

    using a coarse resolution of 10 sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sulphate and carbonaceous species have an annual mean within a factor of two of the observations. The simulated sea-salt concentrations reproduce the observations within a factor of two, apart from the Southern Ocean over which the concentrations are within a factor of five. Regionally, AOD is in a relatively good agreement with the observations (within a factor of two). At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and dust regions the modelled AOD is significantly lower than observed. Regarding most of the investigated aerosol properties, the SALSA and the modal aerosol module M7 perform comparably well against observations. However, SALSA reproduces the observed number concentrations and the size distribution of CCN sized particles much more accurately than M7, and is therefore a good choice for aerosol-cloud interaction studies in global models. Our study also shows that when activation type nucleation in the boundary layer is included, the observed concentration of particles under 50 nm in diameter are reproduced much better compared to when only binary nucleation in the free troposphere is assumed.

  19. ACID AEROSOL MEASUREMENT WORKSHOP

    EPA Science Inventory

    This report documents the discussion and results of the U.S. EPA Acid Aerosol Measurement Workshop, conducted February 1-3, 1989, in Research Triangle Park, North Carolina. t was held in response to recommendations by the Clean Air Scientific Advisory Committee (CASAC) regarding ...

  20. EXPOSURES TO ACIDIC AEROSOLS

    EPA Science Inventory

    Ambient monitoring of acid aerosol in four U.S. cities and in a rural region of southern Ontario clearly show distinct periods of strong acidity. easurements made in Kingston, TN, and Stuebenville, OH, resulted in 24-hr H+ ion concentrations exceeding 100 nmole/m3 more than 10 ti...

  1. FORMATION OF PHOTOCHEMICAL AEROSOLS

    EPA Science Inventory

    The objective was to develop a better understanding of smog aerosol formation with particular reference to haze in the Southern California area. This study combined laboratory work with ambient air studies. Counting of particles by light scattering was the principle physical tech...

  2. 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.

  3. 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

  4. 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

  5. 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.

  6. Observations of aerosol light scattering, absorption, and particle morphology changes as a function of relative humidity

    NASA Astrophysics Data System (ADS)

    Arnott, W. P.; Lewis, K.; Paredes-Miranda, G.; Winter, S.; Day, D.; Chakrabarty, R.; Moosmuller, H.; Jimenez, J. L.; Ulbrich, I.; Huffman, A.; Onasch, T.; Trimborn, A.; Kreidenweis, S.; Carrico, C.; Wold, C.; Lincoln, E.; Freeborn, P.; Hao, W.; McMeeking, G.

    2006-12-01

    A very interesting case of smoke aerosol with very low single scattering albedo, yet very large hygroscopic growth for scattering is presented. Several samples of chamise (Adenostoma fasciculatum), a common and often dominant species in California chaparral, were recently burned at the USFS Fire Science Laboratory in Missoula Montana, and aerosol optics and chemistry were observed, along with humidity-dependent light scattering, absorption, and particle morphology. Photoacoustic measurements of light absorption by two instruments at 870 nm, one on the dry channel, one on the humidified channel, showed strong reduction of aerosol light absorption with RH above 65 percent, and yet a strong increase in light scattering was observed both at 870 nm and 550 nm with nephelometers. Multispectral measurements of aerosol light absorption indicated an Angstrom coefficient for absorption near unity for the aerosols from chamise combustion. It is argued that the hygroscopic growth of scattering is due to uptake of water by the sulfur bearing aerosol. Furthermore, the reduction of aerosol light absorption is argued to be due to the collapse of chain aggregate aerosol as the RH increases wherein the interior of aerosol does no longer contribute to absorption. Implications for biomass burning in general are that humidity processing of aerosols from this source and others like it tends to substantially increase its single scattering albedo, probably in a non-reversible manner. The chemical pathway to hygroscopicity will be addressed.

  7. 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

  8. Effect of aerosol radiative forcing on the seasonal variation of snow over the northern hemisphere

    NASA Astrophysics Data System (ADS)

    Kim, M.; Lau, W. K.; Lee, W.; Kim, K.

    2009-12-01

    In this study, the effect of aerosol radiative forcing on the seasonal variation of snow is studied based on GCM simulation with prescribed aerosols. Numerical experiments are conducted using NASA fvGCM with McRAS. Monthly mean distribution of five aerosol species (black carbon, organic carbon, dust, sulfate, and sea salt) is obtained from GOCART model. In the control run, all five aerosol species are included. For sensitivity test, we carry out an experiment without any aerosol radiative forcing and three additional runs, which are identical to the control run, except for exclusion of black carbon, of dust, and of sulfate, to show the effect of different types of aerosols. The results show that atmospheric warming by absorbing aerosols, dust and black carbon, initiate the elevated heat pump (EHP) and subsequently warm the atmosphere and land surface, especially over Tibetan Plateau (TP). As a results snow over TP reduced greatly in April and May, and the reduction of snow cover decrease surface albedo. Surface energy balance analysis shows that the surface warming due to absorbing aerosol cause early snow melting and further increase surface-atmosphere warming through snow/ice albedo feedback. The similar relations between aerosol radiative forcing and snow melt are also found over other higher latitude region in the Northern Hemisphere. The intensity and duration of earlier snow melt by black carbon aerosol is more significant than that of dust aerosol over the higher latitude in the Northern Hemisphere while over the Tibetan Plateau both black carbon and dust aerosol are important in driving earlier snow melt.

  9. Description and evaluation of GMXe: a new aerosol submodel for global simulations (v1)

    NASA Astrophysics Data System (ADS)

    Pringle, K. J.; Tost, H.; Metzger, S.; Steil, B.; Giannadaki, D.; Nenes, A.; Fountoukis, C.; Stier, P.; Vignati, E.; Lelieveld, J.

    2010-05-01

    We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations.

  10. Description and evaluation of GMXe: a new aerosol submodel for global simulations (v1)

    NASA Astrophysics Data System (ADS)

    Pringle, K. J.; Tost, H.; Message, S.; Steil, B.; Giannadaki, D.; Nenes, A.; Fountoukis, C.; Stier, P.; Vignati, E.; Lelieveld, J.

    2010-09-01

    We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations.

  11. 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

  12. Photochemical aging of light-absorbing secondary organic aerosol material.

    PubMed

    Sareen, Neha; Moussa, Samar G; McNeill, V Faye

    2013-04-11

    Dark reactions of methylglyoxal with NH4(+) in aqueous aerosols yield light-absorbing and surface-active products that can influence the physical properties of the particles. Little is known about how the product mixture and its optical properties will change due to photolysis as well as oxidative aging by O3 and OH in the atmosphere. Here, we report the results of kinetics and product studies of the photochemical aging of aerosols formed by atomizing aqueous solutions of methylglyoxal and ammonium sulfate. Experiments were performed using aerosol flow tube reactors coupled with an aerosol chemical ionization mass spectrometer (Aerosol-CIMS) for monitoring gas- and particle-phase compositions. Particles were also impacted onto quartz windows in order to assess changes in their UV-visible absorption upon oxidation. Photooxidation of the aerosols leads to the formation of small, volatile organic acids including formic acid, acetic acid, and glyoxylic acid. The atmospheric lifetime of these species during the daytime is predicted to be on the order of minutes, with photolysis being an important mechanism of degradation. The lifetime with respect to O3 oxidation was observed to be on the order of hours. O3 oxidation also leads to a net increase in light absorption by the particles due to the formation of additional carbonyl compounds. Our results are consistent with field observations of high brown carbon absorption in the early morning. PMID:23506538

  13. Cluster analysis on mass spectra of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Spindler, C.; Kiendler-Scharr, A.; Kleist, E.; Mensah, A.; Mentel, T.; Tillmann, R.; Wildt, J.

    2009-04-01

    Biogenic secondary organic aerosols (BSOA) are of high importance in the atmosphere. The formation of SOA from the volatile organic compound (VOC) emissions of selected trees was investigated in the JPAC (Jülich Plant Aerosol Chamber) facility. The VOC (mainly monoterpenes) were transferred into a reaction chamber where vapors were photo-chemically oxidized and formed BSOA. The aerosol was characterized by aerosol mass spectrometry (Aerodyne Quadrupol-AMS). Inside the AMS, flash-vaporization of the aerosol particles and electron impact ionization of the evaporated molecules cause a high fragmentation of the organic compounds. Here, we present a classification of the aerosol mass spectra via cluster analysis. Average mass spectra are produced by combination of related single mass spectra to so-called clusters. The mass spectra were similar due to the similarity of the precursor substances. However, we can show that there are differences in the BSOA mass spectra of different tree species. Furthermore we can distinguish the influence of the precursor chemistry and chemical aging. BSOA formed from plants exposed to stress can be distinguished from BSOA formed under non stressed conditions. Significance and limitations of the clustering method for very similar mass spectra will be demonstrated and discussed.

  14. 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).

  15. Aerosol Production in a Mixed Deciduous/Coniferous Forest

    NASA Astrophysics Data System (ADS)

    Slade, N.; Mielke, L.; Alaghmand, M.; Galloway, M.; Kammrath, A.; Keutsch, F.; Hansen, R.; Griffith, S.; Dusanter, S.; Stevens, P.; Carroll, M.; Bertman, S.; Shepson, P.

    2008-12-01

    Aerosols are of fundamental concern because of their impacts on air quality, human health and radiative forcing. Recent studies have focused on secondary organic aerosol (SOA) production due to oxidation of volatile organic compounds (VOCs), and more importantly biogenic-VOCs (BVOCs), in particular, isoprene. However, the SOA precursors are not well understood because the mechanisms have shown that isoprene oxidation can contribute to aerosol production through multiple generation oxidation products. For terpenes, it is more likely that primary or secondary oxidation products lead to particle formation. In the present study, we measured the aerosol size distribution, along with O3, HOx, NOx, NOy and BVOCs, in a mixed deciduous forest that is undergoing successional transition to a conifer-dominated species mix. This study was conducted in a rural forest environment in northern Michigan as a part of the summer 2008 PROPHET campaign at the University of Michigan Biological Station (UMBS). We examine here the potential BVOC contribution to aerosol formation. A TSI, inc. Scanning Mobility Particle Sizer (SMPS) was used to measure aerosol number density in the size range, 15 nm < x < 711 nm and a Proton Transfer Reaction - Linear Ion Trap (PTR-LIT) mass spectrometer for quantifying isoprene and other BVOCs, including methyl vinyl ketone and methacrolein, and total monoterpenes. Preliminary results show periods of new particle production. Here we use a unique set of BVOC, HOx, NOx, NOy, O3 and meteorological data to examine conditions leading to new particle production.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  18. 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.

  19. Modeling study on the transport of summer dust and anthropogenic aerosols over the Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Liu, Y.; Sato, Y.; Jia, R.; Xie, Y.; Huang, J.; Nakajima, T.

    2015-11-01

    The Tibetan Plateau (TP) is located at the juncture of several important natural and anthropogenic aerosol sources. Satellites have observed substantial dust and anthropogenic aerosols in the atmosphere during summer over the TP. These aerosols have distinct effects on the earth's energy balance, microphysical cloud properties, and precipitation rates. To investigate the transport of summer dust and anthropogenic aerosols over the TP, we combined the Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS) with a non-hydrostatic regional model (NHM). The model simulation shows heavily loaded dust aerosols over the northern slope and anthropogenic aerosols over the southern slope and the east of the TP. The dust aerosols are primarily mobilized around the Taklimakan Desert, where a portion of the aerosols are transported eastward due to the northwesterly current; simultaneously, a portion of the particles are transported southward when a second northwesterly current becomes northeasterly because of the topographic blocking of the northern slope of the TP. Because of the strong upward current, dust plumes can extend upward to approximately 7-8 km a.s.l. over the northern slope of the TP. When a dust event occurs, anthropogenic aerosols that entrained into the southwesterly current via the Indian summer monsoon are transported from India to the southern slope of the TP. Simultaneously, a large amount of anthropogenic aerosol is also transported from eastern China to the east of the TP by easterly winds. An investigation on the transport of dust and anthropogenic aerosols over the plateau may provide the basis for determining aerosol impacts on summer monsoons and climate systems.

  20. Modeling study on the transport of summer dust and anthropogenic aerosols over the Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Liu, Y.; Sato, Y.; Jia, R.; Xie, Y.; Huang, J.; Nakajima, T.

    2015-05-01

    The Tibetan Plateau (TP) is located at the juncture of several important natural and anthropogenic aerosol sources. Satellites have observed substantial dust and anthropogenic aerosols in the atmosphere during summer over the TP. These aerosols have distinct effects on the earth's energy balance, microphysical cloud properties, and precipitation rates. To investigate the transport of summer dust and anthropogenic aerosols over the TP, we combined the Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS) with a non-hydrostatic regional model (NHM). The model simulation shows heavily loaded dust aerosols over the northern slope and anthropogenic aerosols over the southern slope and to the east of the TP. The dust aerosols are primarily mobilized around the Taklimakan Desert, where a portion of the aerosols are transported eastward due to the northwesterly current; simultaneously, a portion of the particles are transported northward when a second northwesterly current becomes northeasterly because of the topographic blocking of the northern slope of the TP. Because of the strong upward current, dust plumes can extend upward to approximately 7-8 km a.s.l. over the northern slope of the TP. When a dust event occurs, anthropogenic aerosols that entrain into the southwesterly current via the Indian summer monsoon are transported from India to the southern slope of the TP. Simultaneously, a large amount of anthropogenic aerosols is also transported from eastern China to east of the TP by easterly winds. An investigation on the transport of dust and anthropogenic aerosols over the plateau may provide the basis for determining aerosol impacts on summer monsoons and climate systems.

  1. 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

  2. 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

  3. 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.

  4. 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

  5. ANISORROPIA: the adjoint of the aerosol thermodynamic model ISORROPIA

    NASA Astrophysics Data System (ADS)

    Capps, S. L.; Henze, D. K.; Hakami, A.; Russell, A. G.; Nenes, A.

    2011-08-01

    We present the development of ANISORROPIA, the discrete adjoint of the ISORROPIA thermodynamic equilibrium model that treats the Na+-SO42--HSO4--NH4+-NO3--Cl--H2O aerosol system, and we demonstrate its sensitivity analysis capabilities. ANISORROPIA calculates sensitivities of an inorganic species in aerosol or gas phase with respect to the total concentrations of each species present with only a two-fold increase in computational time over the forward model execution. Due to the highly nonlinear and discontinuous solution surface of ISORROPIA, evaluation of the adjoint required a new, complex-variable version of the the model, which determines first-order sensitivities with machine precision and avoids cancellation errors arising from finite difference calculations. The adjoint is verified over an atmospherically relevant range of concentrations, temperature, and relative humidity. We apply ANISORROPIA to recent field campaign results from Atlanta, GA, USA, and Mexico City, Mexico, to characterize the inorganic aerosol sensitivities of these distinct urban air masses. The variability in the relationship between PM2.5 mass and precursor concentrations shown has important implications for air quality and climate. ANISORROPIA enables efficient elucidation of aerosol concentration dependence on aerosol precursor emissions in the context of atmospheric chemical transport model adjoints.

  6. Study of atmospheric aerosol processing using confocal Raman microspectroscopy

    NASA Astrophysics Data System (ADS)

    Laskina, O.; Grassian, V. H.

    2012-12-01

    Aerosols undergo aging and heterogeneous chemistry as they are transported through the atmosphere. This leads to changes in their properties and their effects on climate, biogeochemistry and human health. Chemical imaging of individual particles may be used to directly investigate the heterogeneity of composition within atmospheric aerosol particles. Single-particle Raman microspectroscopy is a powerful method for chemical imaging and non-destructive physico-chemical characterization of aerosol particles. In this study we investigate the effect of chemical processing on the distribution of chemical species in single particles of mineral dust aerosol using Raman spectral imaging. Raman mapping was used to show the distribution of humic substances and organic acids on some major components of mineral dust (quartz, clays and calcium carbonate). It was shown that humic materials form coating on the surface of particles, whereas interactions of calcium carbonate with organic acids (oxalic and acetic acids) lead to reactions that cause a heterogeneous distribution of components within the reacted particle. Additionally, in a newly designed flow system aerosol can be equilibrated at different relative humidities to study hygroscopicity and phase transitions within these particles. These types of studies are important as the distribution of species in a single particle determines its reactivity, water uptake, and optical properties and thus defines its impact on climate and environment.

  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. 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

  9. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  12. Aircraft measurement of organic aerosols over China.

    PubMed

    Wang, Gehui; Kawamura, Kimitaka; Hatakeyama, Shiro; Takami, Akinori; Li, Hong; Wang, Wei

    2007-05-01

    Lower to middle (0.5-3.0 km altitude) tropospheric aerosols (PM2.5) collected by aircraft over inland and east coastal China were, for the first time, characterized for organic molecular compositions to understand anthropogenic, natural, and photochemical contribution to the air quality. n-Alkanes, fatty acids, sugars, polyacids are detected as major compound classes, whereas lignin and resin products, sterols, polycyclic aromatic hydrocarbons, and phthalic acids are minor species. Average concentrations of all the identified compounds excluding malic acid correspond to 40-50% of those reported on the ground sites. Relative abundances of secondary organic aerosol (SOA) components such as malic acid are much higher in the aircraft samples, suggesting an enhanced photochemical production over China. Organic carbon (OC) concentrations in summer (average, 24.3 microg m(-3)) were equivalent to those reported on the ground sites. Higher OC/EC (elemental carbon) ratios in the summer aircraft samples also support a significant production of SOA over China. High loadings of organic aerosols in the Chinese troposphere may be responsible to an intercontinental transport of the pollutants and potential impact on the regional and global climate changes. PMID:17539513

  13. Assimilation of Aerosol Optical Depths

    NASA Astrophysics Data System (ADS)

    Verver, Gé; Henzing, Bas

    Climate predictions are hampered by the large uncertainties involved in the estima- tion of the effects of atmospheric aerosol (IPCC,2001). These uncertainties are caused partly because sources and sinks as well as atmospheric processing of the different types of aerosol are not accurately known. Moreover, the climate impact (especially the indirect effect) of a certain distribution of aerosol is hard to quantify. There have been different approaches to reduce these uncertainties. In recent years intensive ob- servational campaigns such as ACE and INDOEX have been carried out, aiming to in- crease our knowledge of atmospheric processes that determine the fate of atmospheric aerosols and to quantify the radiation effects. With the new satellite instruments such as SCIAMACHY and OMI it will be possible in the near future to derive the ge- ographical distribution of the aerosol optical depths (AOD) and perhaps additional information on the occurrence of different aerosol types. The goal of the ARIA project (started in 2001) is to assimilate global satellite de- rived aerosol optical depth (AOD) in an off-line chemistry/transport model TM3. The TM3 model (Jeuken et al. 2001) describes sources, sinks, transformation and transport processes of different types of aerosol (mineral dust, carbon, sulfate, nitrate) that are relevant to radiative forcing. All meteorological input is provided by ECMWF. The assimilation procedure constrains the aerosol distribution produced by the model on the basis of aerosol optical depths observed by satellite. The product, i.e. an optimal estimation of global aerosol distribution, is then available for the calculation of radia- tive forcing. Error analyses may provide valuable information on deficiencies of the model. In the ARIA project it is tried to extract additional information on the type of aerosol present in the atmosphere by assimilating AOD at multiple wavelengths. First results of the ARIA project will be presented. The values

  14. 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.

  15. 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

  16. Stratospheric aerosols - Observation and theory

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Whitten, R. C.; Toon, O. B.

    1982-01-01

    Important chemical and physical roles of aerosols are discussed, and properties of stratospheric aerosols as revealed by experimental data are described. In situ measurements obtained by mechanical collection and scattered-light detection yield the overall size distribution of the aerosols, and analyses of preserved aerosol precursor gases by wet chemical, cryogenic and spectroscopic techniques indicate the photochemical sources of particle mass. Aerosol chemical reactions including those of gaseous precursors, those in aqueous solution, and those on particle surfaces are discussed, in addition to aerosol microphysical processes such as nucleation, condensation/evaporation, coagulation and sedimentation. Models of aerosols incorporating such chemical and physical processes are presented, and simulations are shown to agree with measurements. Estimates are presented for the potential aerosol changes due to emission of particles and gases by aerospace operations and industrial consumption of fossil fuels, and it is demonstrated that although the climatic effects of existing levels of stratospheric aerosol pollution are negligible, potential increases in those levels might pose a future threat.

  17. 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

  18. 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.

  19. Results and code prediction comparisons of lithium-air reaction and aerosol behavior tests

    SciTech Connect

    Jeppson, D.W.

    1986-03-01

    The Hanford Engineering Development Laboratory (HEDL) Fusion Safety Support Studies include evaluation of potential safety and environmental concerns associated with the use of liquid lithium as a breeder and coolant for fusion reactors. Potential mechanisms for volatilization and transport of radioactive metallic species associated with breeder materials are of particular interest. Liquid lithium pool-air reaction and aerosol behavior tests were conducted with lithium masses up to 100 kg within the 850-m/sup 3/ containment vessel in the Containment Systems Test Facility. Lithium-air reaction rates, aerosol generation rates, aerosol behavior and characterization, as well as containment atmosphere temperature and pressure responses were determined. Pool-air reaction and aerosol behavior test results were compared with computer code calculations for reaction rates, containment atmosphere response, and aerosol behavior. The volatility of potentially radioactive metallic species from a lithium pool-air reaction was measured. The response of various aerosol detectors to the aerosol generated was determined. Liquid lithium spray tests in air and in nitrogen atmospheres were conducted with lithium temperatures of about 427/sup 0/ and 650/sup 0/C. Lithium reaction rates, containment atmosphere response, and aerosol generation and characterization were determined for these spray tests.

  20. 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

  1. 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.

  2. Collection and analysis of inorganic and water soluble organic aerosols over Maryland and Virginia

    NASA Astrophysics Data System (ADS)

    Brent, L. C.; Ziemba, L. D.; Beyersdorf, A. J.; Phinney, K.; Conny, J.; Dickerson, R. R.

    2012-12-01

    Aerosols aloft have slower removal than those near the ground, in part, because dry and wet deposition rates result in longer lifetimes and greater range of influence. Knowledge of deposition rates and range of transport for different species are important for developing local and regional air quality policy. Currently, the vertical distribution of organic aerosols (OA's) and their polar, oxidized fraction is largely unknown. Comprehensive methods to analyze aerosol composition collected in the boundary layer and the lower free troposphere are lacking. During DISCOVER AQ 2011, both the NASA P3 and Cessna 402B collected aerosols, through shrouded aerosol inlets, onto Teflon and quartz fiber filters. Collection occurred in both the boundary layer and lower free troposphere over Maryland and Virginia, USA. After extraction with water and optimizing separation via ion chromatography, commonly identified secondary organic aerosols can be separated based on their functionality as mono-, di-, or polycarboxylic acids. Inorganic aerosol components can simultaneously be separated and identified with the same method. Individual organic acid compound analysis with detection limits in the low ppb range can be achieved when conductivity/ultraviolet/ and mass spectrometric detectors are placed in tandem. Additionally, thermo optical analysis can be used to determine the mass fraction of water soluble organic carbon versus the total collected mass. This research is designed to provide information on the vertical distribution of particulate organic carbon in the atmosphere, its optical properties, information on aerosol transport in the lower free troposphere, and to provide water soluble organic aerosol structural characterization.

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

  4. 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

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

    NASA Astrophysics Data System (ADS)

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

    2011-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-07-01

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

  7. 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.

  8. 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.

  9. 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.

  10. 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

  11. 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

  12. 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

  13. Aerosol Absorption and Radiative Forcing

    NASA Technical Reports Server (NTRS)

    Stier, Philip; Seinfeld, J. H.; Kinne, Stefan; Boucher, Olivier

    2007-01-01

    We present a comprehensive examination of aerosol absorption with a focus on evaluating the sensitivity of the global distribution of aerosol absorption to key uncertainties in the process representation. For this purpose we extended the comprehensive aerosol-climate model ECHAM5-HAM by effective medium approximations for the calculation of aerosol effective refractive indices, updated black carbon refractive indices, new cloud radiative properties considering the effect of aerosol inclusions, as well as by modules for the calculation of long-wave aerosol radiative properties and instantaneous aerosol forcing. The evaluation of the simulated aerosol absorption optical depth with the AERONET sun-photometer network shows a good agreement in the large scale global patterns. On a regional basis it becomes evident that the update of the BC refractive indices to Bond and Bergstrom (2006) significantly improves the previous underestimation of the aerosol absorption optical depth. In the global annual-mean, absorption acts to reduce the shortwave anthropogenic aerosol top-of-atmosphere (TOA) radiative forcing clear-sky from -0.79 to -0.53 W m(sup -2) (33%) and all-sky from -0.47 to -0.13W m(sup -2 (72%). Our results confirm that basic assumptions about the BC refractive index play a key role for aerosol absorption and radiative forcing. The effect of the usage of more accurate effective medium approximations is comparably small. We demonstrate that the diversity in the AeroCom land-surface albedo fields contributes to the uncertainty in the simulated anthropogenic aerosol radiative forcings: the usage of an upper versus lower bound of the AeroCom land albedos introduces a global annual-mean TOA forcing range of 0.19W m(sup -2) (36%) clear-sky and of 0.12W m(sup -2) (92%) all-sky. The consideration of black carbon inclusions on cloud radiative properties results in a small global annual-mean all-sky absorption of 0.05W m(sup -2) and a positive TOA forcing perturbation of 0

  14. Contributions of Acid-Catalysed Processes to Secondary Organic Aerosol Mass - A Modelling pproach

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Feingold, G.; Kreidenweis, S. M.

    2005-12-01

    A significant fraction of secondary organic aerosol (SOA) mass is formed by chemical and/or physical processes. However, the amount of organic material found in ambient organic aerosols cannot be explained with current models. Recently, several laboratory studies have been published which suggest that also acid-catalyzed processes that occur either in particles or at their surfaces (heterogeneous) might contribute significantly to mass formation. However, to date there is no general conclusion about the efficiency of such processes due to the great diversity of species and experimental conditions. We present a compilation of literature data (thermodynamic and kinetic) of these processes. The aerosol yields of (i) additional species which are thought previously not contribute to SOA formation (e.g. isoprene, aliphatic aldehydes) and (ii) species which form apparently higher SOA masses on acidic seed aerosols are reported and compared to input data of previous SOA models. Available kinetic data clearly exclude aldol condensation as a significant process for SOA formation on a time scale of typical aerosol life times. Using aerosol size distributions and gas phase concentrations measured during NEAQS2002 as model input data, we show that (even under assumption of equilibrium conditions) these additional processes only contribute a minor fraction to the organic aerosol mass.

  15. 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

  16. 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

  17. 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.

  18. 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 ...

  19. AEROSOL EXPOSURE, PHYSICS, AND CHEMISTRY

    EPA Science Inventory

    A brief review is given of the "Knowledge" and the "Gaps in Knowledge" of aerosol exposure, physics and chemistry relevant to health effects of aerosols, and presented or discussed in platform or poster presentations at the Symposium on Particulate Air Pollution - Associations wi...

  20. Nanotechnology and pharmaceutical inhalation aerosols.

    PubMed

    Patel, A R; Vavia, P R

    2007-02-01

    Pharmaceutical inhalation aerosols have been playing a crucial role in the health and well being of millions of people throughout the world for many years. The technology's continual advancement, the ease of use and the more desirable pulmonary-rather-than-needle delivery for systemic drugs has increased the attraction for the pharmaceutical aerosol in recent years. But administration of drugs by the pulmonary route is technically challenging because oral deposition can be high, and variations in inhalation technique can affect the quantity of drug delivered to the lungs. Recent advances in nanotechnology, particularly drug delivery field have encouraged formulation scientists to expand their reach in solving tricky problems related to drug delivery. Moreover, application of nanotechnology to aerosol science has opened up a new category of pharmaceutical aerosols (collectively known as nanoenabled-aerosols) with added advantages and effectiveness. In this review, some of the latest approaches of nano-enabled aerosol drug delivery system (including nano-suspension, trojan particles, bioadhesive nanoparticles and smart particle aerosols) that can be employed successfully to overcome problems of conventional aerosol systems have been introduced. PMID:17375556

  1. 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.

  2. Preliminary aerosol generator design studies

    NASA Technical Reports Server (NTRS)

    Stampfer, J. F., Jr.

    1976-01-01

    The design and construction of a prototype vaporization generator for highly dispersed sodium chloride aerosols is described. The aerosol generating system is to be used in the Science Simulator of the Cloud Physics Laboratory Project and as part of the Cloud Physics Laboratory payload to be flown on the shuttle/spacelab.

  3. 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...

  4. Mount St. Helens aerosol evolution

    NASA Technical Reports Server (NTRS)

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

    1982-01-01

    Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mount 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.

  5. Mount St. Helens aerosol evolution

    SciTech Connect

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

    1982-09-01

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

  6. Mount St. Helens aerosol evolution

    SciTech Connect

    Oberbeck, V.R.; Farlow, N.H.

    1982-08-01

    Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mount 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.

  7. 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

  8. 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.

  9. Aerosol phage therapy efficacy in Burkholderia cepacia complex respiratory infections.

    PubMed

    Semler, Diana D; Goudie, Amanda D; Finlay, Warren H; Dennis, Jonathan J

    2014-07-01

    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

  10. 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.

  11. 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.

  12. 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

  13. 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

  14. The Aerosol Coarse Mode Initiative

    NASA Astrophysics Data System (ADS)

    Arnott, W. P.; Adhikari, N.; Air, D.; Kassianov, E.; Barnard, J.

    2014-12-01

    Many areas of the world show an aerosol volume distribution with a significant coarse mode and sometimes a dominant coarse mode. The large coarse mode is usually due to dust, but sea salt aerosol can also play an important role. However, in many field campaigns, the coarse mode tends to be ignored, because it is difficult to measure. This lack of measurements leads directly to a concomitant "lack of analysis" of this mode. Because, coarse mode aerosols can have significant effects on radiative forcing, both in the shortwave and longwave spectrum, the coarse mode -- and these forcings -- should be accounted for in atmospheric models. Forcings based only on fine mode aerosols have the potential to be misleading. In this paper we describe examples of large coarse modes that occur in areas of large aerosol loading (Mexico City, Barnard et al., 2010) as well as small loadings (Sacramento, CA; Kassianov et al., 2012; and Reno, NV). We then demonstrate that: (1) the coarse mode can contribute significantly to radiative forcing, relative to the fine mode, and (2) neglecting the coarse mode may result in poor comparisons between measurements and models. Next we describe -- in general terms -- the limitations of instrumentation to measure the coarse mode. Finally, we suggest a new initiative aimed at examining coarse mode aerosol generation mechanisms; transport and deposition; chemical composition; visible and thermal IR refractive indices; morphology; microphysical behavior when deposited on snow and ice; and specific instrumentation needs. Barnard, J. C., J. D. Fast, G. Paredes-Miranda, W. P. Arnott, and A. Laskin, 2010: Technical Note: Evaluation of the WRF-Chem "Aerosol Chemical to Aerosol Optical Properties" Module using data from the MILAGRO campaign, Atmospheric Chemistry and Physics, 10, 7325-7340. Kassianov, E. I., M. S. Pekour, and J. C. Barnard, 2012: Aerosols in Central California: Unexpectedly large contribution of coarse mode to aerosol radiative forcing

  15. Complex Coupling of Air Quality and Climate-Relevant Aerosols in a Chemistry-Aerosol Microphysics Model

    NASA Astrophysics Data System (ADS)

    Yoshioka, M.; Carslaw, K. S.; Reddington, C.; Mann, G.

    2013-12-01

    Controlling emissions of aerosols and their precursors to improve air quality will impact the climate through direct and indirect radiative forcing. We have investigated the impacts of changes in a range of aerosol and gas-phase emission fluxes and changes in temperature on air quality and climate change metrics using a global aerosol microphysics and chemistry model, GLOMAP. We investigate how the responses of PM2.5 and cloud condensation nuclei (CCN) are coupled, and how attempts to improve air quality could have inadvertent effects on CCN, clouds and climate. The parameter perturbations considered are a 5°C increase in global temperature, increased or decreased precursor emissions of anthropogenic SO2, NH3, and NOx, and biogenic monoterpenes, and increased or decreased primary emissions of organic and black carbon aerosols from wildfire, fossil fuel, and biofuel. To quantify the interactions, we define a new sensitivity metric in terms of the response of CCN divided by the response of PM in different regions. .Our results show that the coupled chemistry and aerosol processes cause complex responses that will make any co-benefit policy decision problematic. In particular, we show that reducing SO2 emissions effectively reduces surface-level PM2.5 over continental regions in summer when background PM2.5 is high, with a relatively small reduction in marine CCN (and hence indirect radiative cooling over ocean), which is beneficial for near-term climate. Reducing NOx emissions does not improve summertime air quality very effectively but leads to a relatively high reduction of marine CCN. Reducing NH3 emissions has moderate effects on both PM2.5 and CCN. These three species are strongly coupled chemically and microphysically and the effects of changing emissions of one species on mass and size distributions of aerosols are very complex and spatially and temporally variable. For example, reducing SO2 emissions leads to reductions in sulphate and ammonium mass

  16. 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.

  17. 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

  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. PMID:17695910

  19. 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.

  20. "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

  1. Trace gas and aerosol measurements at Whiteface Mountain, New York

    SciTech Connect

    Kelly, T.J.

    1985-09-01

    This report presents the results of a 12-month program of atmospheric chemical measurements performed at Whiteface Mountain, New York. The purpose of this program was to study the concentrations and seasonal variability of several atmospheric chemical species which are of importance in the acid deposition issue. Whiteface Mountain (WFM) was chosen as the site of these measurements because it lies in the Adirondack Mountains of New York State, one of the areas considered susceptible to ecological damage from acid deposition. These measurements were the first long term study of atmospheric chemistry in the Adirondacks. Continuous real-time measurements of SO/sub 2/ and NO/sub x/ were made with commercial instruments modified for increased sensitivity and stability, and aerosol composition, HNO/sub 3/ and SO/sub 2/ were measured with a three-stage filter pack. The main conclusions of this work are (1) that concentrations of gaseous SO/sub 2/ and NO/sub x/ are highest in the winter months, whereas their oxidation products SO/sub 4//sup 2 -/ and HNO/sub 3/ were highest in summer; (2) that aerosol acidity is closely associated with SO/sub 4//sup 2 -/, aerosol NO/sub 3//sup -/ concentrations being very low in all seasons; (3) and that the relative importance of aerosol acidity and HNO/sub 3/ vary with season, because the strong seasonal variation in SO/sub 4//sup 2 -/ results in a very strong seasonal variation in aerosol acidity.

  2. Mechanistic understanding of aerosol emissions from a brazing operation.

    PubMed

    Zimmer, A T; Biswas, P

    2000-01-01

    Welding operations produce gaseous and aerosol by-products that can have adverse health effects. A laboratory furnace study was conducted to aid understanding of the chemical and aerosol behavior of a widely used, self-fluxing brazing alloy (89% Cu, 6% Ag, 5% P) that is also used with a supplemental fluxing compound to prevent oxidation at the molten metal surface. The results indicate that the aerosols generated by the alloy are transient (produced over a short duration of time) and are associated with mass transfer of phosphorus species from the molten metal surface to the surrounding gas. In contrast, when the alloy was used in conjunction with the supplemental fluxing compound, a relatively nontransient, submicron-size aerosol was generated that was several orders of magnitude higher in concentration. Thermodynamic equilibrium analysis suggests that fluoride (a major constituent in the fluxing compound) played a significant role in reacting with the brazing alloy metals to form gas phase metal fluoride compounds that had high vapor pressures when compared with their elemental or oxide forms. As these metal-fluoride vapors cooled, submicron-size particles were formed mainly through nucleation and condensation growth processes. In addition, the equilibrium results revealed the potential formation of severe pulmonary irritants (HF and BF3) from heating the supplemental fluxing compound. These results demonstrated the importance of fluxing compounds in the formation of brazing fumes, and suggest that fluxing compounds could be selected that serve their metallurgical intention and suppress the formation of aerosols. PMID:10885884

  3. 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

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

    NASA Astrophysics Data System (ADS)

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

    2014-03-01

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

  5. 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.

  6. 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.

  7. Estimating the direct and indirect effects of secondary organic aerosols using ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

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

    2011-08-01

    Secondary organic aerosol (SOA) has been introduced into the global climate-aerosol model ECHAM5/HAM. The SOA module handles aerosols originating from both biogenic and anthropogenic sources. The model simulates the emission of precursor gases, their chemical conversion into condensable gases, the partitioning of semi-volatile condenable species into the gas and aerosol phases. As ECHAM5/HAM is a size-resolved model, a new method that permits the calculation of partitioning of semi-volatile species between different size classes is introduced. We compare results of modelled organic aerosol concentrations against measurements from extensive measurement networks in Europe and the United States, running the model with and without SOA. We also compare modelled aerosol optical depth against measurements from the AERONET network of grond stations. We find that SOA improves agreement between model and measurements in both organic aerosol mass and aerosol optical depth, but does not fully correct the low bias that is present in the model for both of these quantities. Although many models now include SOA, any overall estimate of the direct and indirect effects of these aerosols is still lacking. This paper makes a first step in that direction. The model is applied to estimate the direct and indirect effects of SOA under simulated year 2000 conditions. The modelled SOA spatial distribution indicates that SOA is likely to be an important source of free and upper tropospheric aerosol. We find a negative shortwave (SW) forcing from the direct effect, amounting to -0.31 Wm-2 on the global annual mean. In contrast, the model indicates a positive indirect effect of SOA of +0.23 Wm-2, arising from the enlargement of particles due to condensation of SOA, together with an enhanced coagulation sink of small particles. In the longwave, model results are a direct effect of +0.02 Wm-2 and an indirect effect of -0.03 Wm-2.

  8. 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.

  9. Aerosol Climate Interactions in Climate System Models

    NASA Astrophysics Data System (ADS)

    Kiehl, J. T.

    2002-12-01

    Aerosols are widely recognized as an important process in Earth's climate system. Observations over the past decade have improved our understanding of the physical and chemical properties of aerosols. Recently, field observations have highlighted the pervasiveness of absorbing aerosols in the atmosphere. These aerosols are of particular interest, since they alter the vertical distribution of shortwave radiative heating between the surface and atmosphere. Given this increased knowledge of aerosols from various field programs, interest is focusing on how to integrate this understanding into global climate models. These types of models provide the best tool available to comprehensively study the potential effects of aerosols on Earth's climate system. Results from climate system model simulations that include aerosol effects will be presented to illustrate key aerosol climate interactions. These simulations employ idealized and realistic distributions of absorbing aerosols. The idealized aerosol simulations provide insight into the role of aerosol shortwave absorption on the global hydrologic cycle. The realistic aerosol distributions provide insight into the local response of aerosol forcing in the Indian subcontinent region. Emphasis from these simulations will be on the hydrologic cycle, since water availability is of emerging global environmental concern. This presentation will also consider what more is needed to significantly improve our ability to model aerosol processes in climate system models. Uncertainty in aerosol climate interactions remains a major source of uncertainty in our ability to project future climate change. Focus will be on interactions between aerosols and various physical, chemical and biogeochemical aspects of the Earth system.

  10. 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.

  11. 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.

  12. 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

  13. 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

  14. 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

  15. 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

  16. 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.

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

    2012-03-16

    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.

  18. ANISORROPIA: the adjoint of the aerosol thermodynamic model ISORROPIA

    NASA Astrophysics Data System (ADS)

    Capps, S. L.; Henze, D. K.; Hakami, A.; Russell, A. G.; Nenes, A.

    2012-01-01

    We present the development of ANISORROPIA, the discrete adjoint of the ISORROPIA thermodynamic equilibrium model that treats the Na+-SO42-- HSO4--NH4+ -NO3--Cl--H2O aerosol system, and we demonstrate its sensitivity analysis capabilities. ANISORROPIA calculates sensitivities of an inorganic species in aerosol or gas phase with respect to the total concentrations of each species present with less than a two-fold increase in computational time over the concentration calculations. Due to the highly nonlinear and discontinuous solution surface of ISORROPIA, evaluation of the adjoint required a new, complex-variable version of the model, which determines first-order sensitivities with machine precision and avoids cancellation errors arising from finite difference calculations. The adjoint is verified over an atmospherically relevant range of concentrations, temperature, and relative humidity. We apply ANISORROPIA to recent field campaign results from Atlanta, GA, USA, and Mexico City, Mexico, to characterize the inorganic aerosol sensitivities of these distinct urban air masses. The variability in the relationship between fine mode inorganic aerosol mass and precursor concentrations shown has important implications for air quality and climate.

  19. 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

  20. 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

  1. Speciated local aerosol characteristics and radiative forcing at a rural midwestern site

    NASA Astrophysics Data System (ADS)

    Dillner, Ann Marie

    2000-11-01

    In this research, physical and chemical properties of ambient aerosols were measured at a rural perturbed mid- latitude site (Bondville, IL) and used to calculate the aerosol optical properties and the resulting direct radiative forcing. Size-segregated aerosol samples were collected during the summer of 1997 using three parallel MOUDIs operating at ambient relative humidity. Two sample sets were used to obtain sulfate, organic carbon (OC), elemental carbon (EC), carbonate and total aerosol mass. The third sample set was used to obtain the size-specific and wavelength-dependent extinction efficiency of EC. The measured submicrometer mass concentration was 11.4 +/- 4.0 μg m-3. Ammonium sulfate comprised nearly half of the submicrometer aerosol and OC plus EC comprised 25%. Water content for ammonium sulfate and OC was estimated using both Köhler theory and parameterized water uptake curves from the literature. Water content for internally mixed aerosols was determined using a ZSR method. Aerosol optical properties (extinction efficiency, asymmetry parameter, single scatter albedo) were calculated from measured size distributions and wavelength dependent refractive indexes for each species and for internal and external mixtures using Mie theory. A technique, utilizing transmission measurements through extracts of size segregated ambient aerosol samples, was developed to obtain the extinction efficiency of EC. Measured EC extinction efficiencies ranged from 7.3 to 1.7 m2 g-1 at 550 nm, depending on particle diameter. Normalized direct aerosol radiative forcing (W g-1 ) was calculated using the Column Radiation Module (CRM) of the National Center for Atmospheric Research (NCAR) Community Climate Model (CCM3). Aerosol optical properties, used in the model, were assumed to be uniform throughout the lowest one kilometer of the atmosphere. The normalized forcing due to ammonium sulfate was -340 +/- 10 W g-1. OC was 1/3 larger and residue was 1/3 smaller. EC within an

  2. Four dimensional variational assimilation of in-situ and remote-sensing aerosol data

    NASA Astrophysics Data System (ADS)

    Nieradzik, L. P.; Elbern, H.

    2012-04-01

    Aerosols play an increasingly important role in atmospheric modelling. They have a strong influence on the radiative transfer balance and a significant impact on human health. Their origin is various and so are its effects. Most of the measurement sites in Europe account for an integrated aerosol load PMx (Particulate Matter of less than x μm in diameter) which does not give any qualitative information on the composition of the aerosol. Since very different constituents contribute to PMx, like e.g. mineral dust derived from desert storms or sea salt, it is necessary to make aerosol forecasts not only of load, but also type resolved. The method of four dimensional variational data assimilation (4Dvar) is a widely known technique to enhance forecast skills of CTMs (Chemistry-Transport-Models) by ingesting in-situ and, especially, remote-sensing measurements. The EURAD-IM (EURopean Air pollution Dispersion - Inverse Model), containing a full adjoint gas-phase model, has been expanded with an adjoint of the MADE (Modal Aerosol Dynamics model for Europe) to optimise initial and boundary values for aerosols using 4Dvar. A forward and an adjoint radiative transfer model is driven by the EURAD-IM as mapping between BLAOT (Boundary Layer Aerosol Optical Thickness) and internal aerosol species. Furthermore, its condensation scheme has been bypassed by an HDMR (High-Dimensional-Model-Representation) to ensure differentiability. In this study both in-situ measured PMx as well as satellite retrieved aerosol optical thicknesses have been assimilated and the effect on forecast performance has been investigated. The source of BLAOT is the aerosol retrieval system SYNAER (SYNergetic AErosol Retrieval) from DLR-DFD that retrieves AOT by making use of both AATSR/SCIAMACHY and AVHRR/GOME-2 data respectively. Its strengths are a large spatial coverage, near real-time availability, and the classification of five intrinsic aerosol species, namely water-solubles, water-insolubles, soot

  3. Aerosol particles at a high-altitude site on the Southeast Tibetan Plateau, China: Implications for pollution transport from South Asia

    NASA Astrophysics Data System (ADS)

    Zhao, Zhuzi; Cao, Junji; Shen, Zhenxing; Xu, Baiqing; Zhu, Chongshu; Chen, L.-W. Antony; Su, Xiaoli; Liu, Suixin; Han, Yongming; Wang, Gehui; Ho, Kinfai

    2013-10-01

    aerosol samples were collected from 16 July 2008 to 26 July 2009 at Lulang, a high-altitude (>3300m above sea level) site on the southeast Tibetan Plateau (TP); objectives were to determine chemical characteristics of the aerosol and identify its major sources. We report aerosol (total suspended particulate, TSP) mass levels and the concentrations of selected elements, carbonaceous species, and water-soluble inorganic ions. Significant buildup of aerosol mass and chemical species (organic carbon, element carbon, nitrate, and sulfate) occurred during the premonsoon, while lower concentrations were observed during the monsoon. Seasonal variations in aerosol and chemical species were driven by precipitation scavenging and atmospheric circulation. Two kinds of high-aerosol episodes were observed: one was enriched with dust indicators (Fe and Ca2+), and the other was enhanced with organic and elemental carbon (OC and EC), SO42-, NO3-, and Fe. The TSP loadings during the latter were 3 to 6 times those on normal days. The greatest aerosol optical depths (National Centers for Environmental Protection/National Center for Atmospheric Research reanalysis) occurred upwind, in eastern India and Bangladesh, and trajectory analysis indicates that air pollutants were transported from the southwest. Northwesterly winds brought high levels of natural emissions (Fe, Ca2+) and low levels of pollutants (SO42-, NO3-, K+, and EC); this was consistent with high aerosol optical depths over the western deserts and Gobi. Our work provides evidence that both geological and pollution aerosols from surrounding regions impact the aerosol population of the TP.

  4. The Importance of Water Uptake by Aerosols in the Climate Change Problem

    NASA Astrophysics Data System (ADS)

    Ramaswamy, V.; Ginoux, P.; Randles, C.; Schwarzkopf, M. D.

    2007-12-01

    It is well understood that aerosol species have and are continuing to play a central role in the radiative forcing of the climate system. While the role of single-scattering properties of aerosols on climate is generally well- recognized, a key factor that governs the aerosol optical property viz., the hygroscopic growth has received insufficient attention particularly in terms of its role in the climatic impacts due to aerosols. A sensitivity investigation is performed that quantitatively highlights the consequence of the growth of sea-salt-organic carbon mixtures for radiative forcing. Next, we employ the GFDL coupled atmosphere-ocean model to study specifically the aerosol radiative forcing and climate response arising due to the hygroscopic features of sulfate aerosols as they have increased from preindustrial to present-day. We make use of observations of optical depth and surface concentrations to evaluate the reliability of the simulated hygroscopic growth. Regional climate responses in Europe, Asia and Africa are examined, with a focus on temperature, hydrological cycle and surface energy budgets. The importance of hygroscopicity in the climate change problem is put in perspective by comparing the climatic effects with those due to aerosol absorption as well as with those caused by the infrared-absorbing long- lived greenhouse gases. Further, we explore the climate consequence arising from the scenarios of the future emissions of aerosols and the associated hygroscopicity effects.

  5. 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.

  6. Air detoxification with nanosize TiO2 aerosol tested on mice.

    PubMed

    Besov, A S; Krivova, N A; Vorontsov, A V; Zaeva, O B; Kozlov, D V; Vorozhtsov, A B; Parmon, V N; Sakovich, G V; Komarov, V F; Smirniotis, P G; Eisenreich, N

    2010-01-15

    A method for fast air purification using high concentration aerosol of TiO(2) nanoparticles is evaluated in a model chemical catastrophe involving toxic vapors of diisopropyl fluorophosphate (DFP). Mice are used as human model in a closed 100 dm(3) chamber. Exposure of mice to 37 ppm of DFP vapor for 15 min resulted in acute poisoning. Spraying TiO(2) aerosol in 2 min after the start of exposure to DFP vapors resulted in quick removal of DFP vapors from the chamber's air. Animals did not show signs of poisoning after the decontamination experiment and exposure to TiO(2) aerosol alone. Reactive oxygen species (ROS) and antioxidant activity (AOA) of mice blood plasma were measured for animals exposed to sound of aerosol generator, DFP vapors, TiO(2) aerosol and DFP vapors+TiO(2) aerosol. Reduced ROS and increased AOA were found for mice exposure to sound, DFP and TiO(2) aerosol. Exposure to DFP and decontamination with TiO(2) nanoparticles resulted in decreased AOA in 48 h following the exposure. The results suggest that application of TiO(2) aerosol is a powerful method of air purification from toxic hydrolysable compounds with moderate health aftermaths and requires further study and optimization. PMID:19765900

  7. 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.

  8. 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.

  9. Development of a Global Tropospheric Aerosol Chemical Transport Model MASINGAR and its Application to the Dust Storm Forecasting

    NASA Astrophysics Data System (ADS)

    Tanaka, T. Y.

    2002-12-01

    We are developing a new three-dimensional aerosol chemical transport model coupled with the MRI/JMA98 GCM, named Model of Aerosol Species IN the Global AtmospheRe (MASINGAR), for the study of atmospheric aerosols and related trace species. MASINGAR treats four major aerosol species that include nss-sulfate, carbonaceous, mineral dust, and sea-salt aerosols. The model accounts for large-scale advective transport, subgrid-scale eddy diffusive and convective transport, surface emission and deposition, wet deposition, as well as chemical reactions. The advective transport is calculated using the semi-Lagrangian transport scheme. Parameterization of convective transport is based on the convective mass flux by Arakawa-Schubert scheme. The space and time resolution of the model are variable, with a standard resolution of T42 (2.8ox2.8o) and 30 levels (up to 0.8hPa). In addition, the model has a built-in four-dimensional data assimilation with assimilated meteorological field, which enables the model to perform a realistic simulation on a specific period and short-period forecast of aerosols. The model was applied to the numerical forecasting of dust storm in spring, 2002, when the first intensive observational period of Aeolian Dust Experiment on the Climatic impact (ADEC) project was conducted. The model simulation of mineral dust aerosol suggests that the synoptic scale aerosol events can be simulated by MASINGAR.

  10. Chemical characteristics of aerosol mists in phosphate fertilizer manufacturing facilities.

    PubMed

    Hsu, Yu-Mei; Wu, Chang-Yu; Lundgren, Dale A; Nall, J Wesley; Birky, Brian K

    2007-01-01

    Of the carcinogens listed by the National Toxicology Program (NTP), strong inorganic mists containing sulfuric acid were identified as a known human carcinogen. In this study, aerosol sampling was conducted at 24 locations in eight Florida phosphoric acid and concentrated fertilizer manufacturing plants and two locations as background in Winter Haven and Gainesville, Florida, using dichotomous samplers. The locations were selected where sulfuric acid mist may potentially exist, including sulfuric acid pump tank areas, belt or rotating table phosphoric acid filter floors, sulfuric acid truck loading/unloading stations, phosphoric acid production reactors (attack tanks), and a concentrated fertilizer granulator during scrubbing with a weak sulfuric acid mixture. An ion chromatography system was used to analyze sulfate and other water soluble ion species. In general, sulfate, fluoride, ammonium, and phosphate were the major species in the fertilizer facilities. For the rotating table/belt phosphoric acid filter floor, phosphate and fluoride were the dominant species for PM10, and the maximum concentrations were 170 and 106 microg/m3, respectively. For the attack tank, fluoride was the dominant species for PM10, and the maximum concentration was 462 microg/m3. At the sulfuric acid pump tank, sulfate was the dominant species, and the maximum PM10 sulfate concentration was 181 microg/m3. The concentration of PM10 sulfate including ammonium sulfate, calcium sulfate, and sulfuric acid were lower than 0.2 mg/m3 at all locations. The aerosols at the filter floor and the attack tank were acidic. The coarse mode aerosol at the sulfuric acid pump tank (an outdoor location) was acidic, whereas the fine mode aerosol was neutral to basic. PMID:17162477

  11. 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

  12. A fixed frequency aerosol albedometer.

    PubMed

    Thompson, Jonathan E; Barta, Nick; Policarpio, Danielle; Duvall, Richard

    2008-02-01

    A new method for the measurement of aerosol single scatter albedo (omega) at 532 nm was developed. The method employs cavity ring-down spectroscopy (CRDS) for measurement of aerosol extinction coefficient (b(ext)) and an integrating sphere nephelometer for determination of aerosol scattering coefficient (b(scat)). A unique feature of this method is that the extinction and scattering measurements are conducted simultaneously, on the exact same sample volume. Limits of detection (3s) for the extinction and scattering channel were 0.61 Mm(-1) and 2.7 Mm(-1) respectively. PMID:18542299

  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. 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

  15. 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

  16. Wavelength dependence of aerosol extinction coefficient for stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Yue, Glenn K.

    1986-01-01

    A simple empirical formula for the wavelength dependence of the aerosol extinction coefficient is proposed. The relationship between the constants in the formula and the variable parameter in the aerosol size distribution is explicitly expressed. Good agreement is found between the extinction coefficients calculated from the proposed formula and that calculated from Mie theory. The proposed expression is shown to be better than the Angstroem formula commonly used by atmospheric scientists.

  17. Coupling aerosol optics to the chemical transport model MATCH (v5.5.0) and aerosol dynamics module SALSA (v1)

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

    Modelling aerosol optical properties is a notoriously difficult task due to the particles' complex morphologies and compositions. Yet aerosols and their optical properties are important for Earth system modelling and remote sensing applications. Operational optics models often make drastic and non realistic approximations regarding morphological properties, which can introduce errors. In this study a new aerosol optics model is implemented, in which more realistic morphologies and mixing states are assumed, especially for black carbon aerosols. 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 radiative fluxes, backscattering coefficients and the Ångström exponent from the new optics model are compared with results from another model simulating particles as externally mixed homogeneous spheres. To gauge the impact on the optical properties from the new optics model, the known and important effects from using aerosol dynamics serves as a reference. The results show that using a more detailed description of particle morphology and mixing states influences the optical properties to the same degree as aerosol dynamics. This is an important finding suggesting that over-simplified optics models coupled to a chemical transport model can introduce considerable errors; this can strongly effect simulations of radiative fluxes in Earth-system models, and it can compromise the use of remote sensing observations of aerosols in model evaluations and chemical data assimilation.

  18. 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.

  19. 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.

  20. 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

  1. 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

  2. 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

  3. 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

  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. 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.

  6. Wintertime aerosol in Las Vegas, Nevada

    NASA Astrophysics Data System (ADS)

    Brown, Steven G.

    Numerous studies have found adverse health effects in subjects who live next to major roadways due to air pollution; in particular, there can be severe impacts on lung function and development in children living and/or attending school next to major roadways due to their exposure to air pollutants, including particulate matter (PM) or aerosol. The composition of aerosol at an elementary school next to a major freeway in Las Vegas, Nevada during winter 2008 was measured using a suite of measurements. An Aerodyne High Resolution Aerosol Mass Spectrometer (HR-AMS) was used to quantify the composition of non-refractory PM1 aerosol, including organic matter (OM); an Aethalometer was used to quantify black carbon (BC); a Sunset OCEC analyzer was used to measure organic and elemental carbon (OC, EC); and a particle-into-liquid system (PILS) coupled to two ion chromatographs (IC) was used to measure fine particle ions. Hi-volume PM2.5 samplers were used to collect aerosol on quartz fiber filters at between 2 and 24 hour intervals during the study, a subset of which were analyzed for PAHs and the biomass burning tracer levoglucosan. Data were analyzed by positive matrix factorization (PMF) to determine the amount of fresh, hydrocarbon-like organic aerosol (HOA), more oxidized OA (low-volatility and semi-volatile OA [LV-OOA, SV-OOA]) and biomass burning OA (BBOA). PM1 aerosol was predominantly carbonaceous, with OM plus BC accounting for 74% of the overall average 6.9 mug/m3 of PM measured. BC had a diurnal pattern similar to traffic volume, while OM was higher in the evening compared to the morning. OM was a mixture of fresh HOA, urban- and regional-scale OOA, and BBOA; in the evening, SV-OOA and BBOA peaked, while HOA concentrations were on average the same in the morning and evening, similar to BC. OM/OC ratios were low (1.52 +/-0.14 on average) during the morning rush hour (average OM = 2.4 mug/m3) when vehicular emissions dominate this near-road measurement site, and

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

    NASA Astrophysics Data System (ADS)

    Hodzic, A.; Vautard, R.; Chazette, P.; Menut, L.; Bessagnet, B.

    2006-01-01

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