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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. 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

  3. 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.

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

    DOE PAGES

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; ...

    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

  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; 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.

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  7. 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.

  8. 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

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  10. Variations in the chemical composition of the submicron aerosol and in the sources of the organic fraction at a regional background site of the Po Valley (Italy)

    NASA Astrophysics Data System (ADS)

    Bressi, Michael; Cavalli, Fabrizia; Belis, Claudio A.; Putaud, Jean-Philippe; Fröhlich, Roman; Martins dos Santos, Sebastiao; Petralia, Ettore; Prévôt, André S. H.; Berico, Massimo; Malaguti, Antonella; Canonaco, Francesco

    2016-10-01

    Fine particulate matter (PM) levels and resulting impacts on human health are in the Po Valley (Italy) among the highest in Europe. To build effective PM abatement strategies, it is necessary to characterize fine PM chemical composition, sources and atmospheric processes on long timescales (> months), with short time resolution (< day), and with particular emphasis on the predominant organic fraction. Although previous studies have been conducted in this region, none of them addressed all these aspects together. For the first time in the Po Valley, we investigate the chemical composition of nonrefractory submicron PM (NR-PM1) with a time resolution of 30 min at the regional background site of Ispra during 1 full year, using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) under the most up-to-date and stringent quality assurance protocol. The identification of the main components of the organic fraction is made using the Multilinear-Engine 2 algorithm implemented within the latest version of the SoFi toolkit. In addition, with the aim of a potential implementation of ACSM measurements in European air quality networks as a replacement of traditional filter-based techniques, parallel multiple offline analyses were carried out to assess the performance of the ACSM in the determination of PM chemical species regulated by air quality directives. The annual NR-PM1 level monitored at the study site (14.2 µg m-3) is among the highest in Europe and is even comparable to levels reported in urban areas like New York City and Tokyo. On the annual basis, submicron particles are primarily composed of organic aerosol (OA, 58 % of NR-PM1). This fraction was apportioned into oxygenated OA (OOA, 66 %), hydrocarbon-like OA (HOA, 11 % of OA) and biomass burning OA (BBOA, 23 %). Among the primary sources of OA, biomass burning (23 %) is thus bigger than fossil fuel combustion (11 %). Significant contributions of aged secondary organic aerosol (OOA) are observed throughout the

  11. 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

  12. 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

  13. 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

  14. 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

  15. 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.

  16. 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.

  17. 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

  18. Aerosol therapy in the equine species.

    PubMed

    Duvivier, D H; Votion, D; Vandenput, S; Lekeux, P

    1997-11-01

    Inhalation therapy plays an increasing role in the management of equine respiratory disorders. This alternative to systematic treatment permits a high concentration of medication to act locally while minimizing side effects and residues. In human medicine, literature in this field is prolific and continuously renewed, whereas in veterinary medicine, applications of aerosol therapy are less extensive. This review considers the principles of action of the different types of devices used for inhalation, i.e., nebulization, metered-dose inhalation and dry powder inhalation, describes the technical and practical requirements for their use in the equine species and considers the advantages and disadvantages of each inhalation device. The pharmacological agents currently administered to horses by inhalation are also discussed. Perspectives of aerosol therapy in the equine species, including aerosols already used in human medicine and their potential applications for horses are described.

  19. 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

  20. Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin at the SW Atlantic coast of Iberia

    NASA Astrophysics Data System (ADS)

    Diesch, J.-M.; Drewnick, F.; Zorn, S. R.; von der Weiden-Reinmüller, S.-L.; Martinez, M.; Borrmann, S.

    2012-04-01

    Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean, a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol (NR-PM1) was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m-3 and 1000 cm-3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition, small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions, could be identified in the particle phase

  1. 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

  2. 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.

  3. 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...

  4. 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

  5. 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

  6. Characterization of Ambient Aerosols in Mexico City during the MCMA-2003 Campaign with Aerosol Mass Spectrometry. Results from the CENICA Supersite

    SciTech Connect

    Salcedo, D; Onasch, Timothy B; Dzepina, K; Canagaratna, M R; Zhang, Q; Huffman, A J; DeCarlo, Peter; Jayne, J T; Mortimer, P; Worsnop, Douglas R; Kolb, C E; Johnson, Kirsten S; Zuberi, Bilal M; Marr, L; Volkamer, Rainer M; Molina, Luisa; Molina, Mario J; Cardenas, B; Bernabe, R; Marquez, C; Gaffney, Jeffrey S; Marley, Nancy A; Laskin, Alexander; Shutthanandan, V; Xie, YuLong; Brune, W H; Lesher, R; Shirley, T; Jiminez, J L

    2006-03-24

    An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed at the CENICA Supersite, while another was deployed in the Aerodyne Mobile Laboratory (AML) during the Mexico City Metropolitan Area field study (MCMA-2003) from March 29-May 4, 2003 to investigate particle concentrations, sources, and processes. This is the first of a series of papers reporting the AMS results from this campaign. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 μm (NR PM1) with high time and size resolution. For the first time, we report field results from a beam width probe, which was used to study the shape and mixing state of the particles and to quantify potential losses of irregular particles due to beam broadening inside the AMS. Data from this probe show that no significant amount of irregular particles was lost due to excessive beam broadening. A comparison of the CENICA and AML AMSs measurements is presented, being the first published intercomparison between two quadrupole AMSs. The speciation, and mass concentrations reported by the two AMSs compared well. In order to account for the refractory material in the aerosol, we also present measurements of Black Carbon (BC) using an aethalometer and an estimate of the aerosol soil component obtained from PIXE analysis of filters. Comparisons of (AMS + BC + soil) mass concentration with other collocated particle instruments (a LASAIR Optical Particle Counter, a Tapered Element Oscillating Microbalance (TEOM) and a DustTrack Aerosol Monitor) are also presented. The comparisons show that the (AMS + BC + soil) mass concentration during MCMC-2003 is a good approximation to the total PM₂.₅ mass concentration.

  7. Chemical characterization of submicron aerosol particles during wintertime in a northwest city of China using an Aerodyne aerosol mass spectrometry.

    PubMed

    Zhang, Xinghua; Zhang, Yangmei; Sun, Junying; Yu, Yangchun; Canonaco, Francesco; Prévôt, Andre S H; Li, Gang

    2017-03-01

    An Aerodyne quadrupole aerosol mass spectrometry (Q-AMS) was utilized to measure the size-resolved chemical composition of non-refractory submicron particles (NR-PM1) from October 27 to December 3, 2014 at an urban site in Lanzhou, northwest China. The average NR-PM1 mass concentration was 37.3 μg m(-3) (ranging from 2.9 to 128.2 μg m(-3)) under an AMS collection efficiency of unity and was composed of organics (48.4%), sulfate (17.8%), nitrate (14.6%), ammonium (13.7%), and chloride (5.7%). Positive matrix factorization (PMF) with the multi-linear engine (ME-2) solver identified six organic aerosol (OA) factors, including hydrocarbon-like OA (HOA), coal combustion OA (CCOA), cooking-related OA (COA), biomass burning OA (BBOA) and two oxygenated OA (OOA1 and OOA2), which accounted for 8.5%, 20.2%, 18.6%, 12.4%, 17.8% and 22.5% of the total organics mass on average, respectively. Primary emissions were the major sources of fine particulate matter (PM) and played an important role in causing high chemically resolved PM pollution during wintertime in Lanzhou. Back trajectory analysis indicated that the long-range regional transport air mass from the westerly was the key factor that led to severe submicron aerosol pollution during wintertime in Lanzhou.

  8. Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

    NASA Astrophysics Data System (ADS)

    Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Flynn, M. J.; Harrison, R. M.; Yin, J.; Gallagher, M. W.; Coe, H.

    2015-06-01

    For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show that secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±1 standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52), and 0.15 (±0.24) μg m-3, contributing 44, 28, 14, 13, and 2 % to the total non-refractory submicron mass (NR-PM1) respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF), in which five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3 respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual

  9. Measurement of mass distribution of chemical species in aerosol particles

    NASA Technical Reports Server (NTRS)

    Sinha, M. P.; Friedlander, S. K.

    1984-01-01

    Aerosols may be generated through the nebulizing of solutions and the evaporation of their solvent, leaving the dry solute particles. Attention is presently given to a method for the direct determination of the masses of chemical species in individual aerosol particles on a continuous, real-time basis, using mass spectrometry. After the aerosol particles are introduced into the ion source of a quadrupole mass spectrometer, the particles impinge on a hot rhenium filament in the mass spectrometer's ion source. The resulting vapor plume is ionized by electron bombardment, and a pulse of ions is generated by each particle. The intensities of different masses in the ion pulses can then be measured by the mass spectrometer.

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

    NASA Astrophysics Data System (ADS)

    Fleury, Benjamin; Gudipati, Murthy; Carrasco, Nathalie

    2016-10-01

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

  11. 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.

  12. Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry Part II: overview of the results at the CENICA supersite and comparison to previous studies

    NASA Astrophysics Data System (ADS)

    Salcedo, D.; Dzepina, K.; Onasch, T. B.; Canagaratna, M. R.; Jayne, J. T.; Worsnop, D. R.; Gaffney, J. S.; Marley, N. A.; Johnson, K. S.; Zuberi, B.; Molina, L. T.; Molina, M. J.; Shutthanandan, V.; Xie, Y.; Jimenez, J. L.

    2005-06-01

    An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed at the CENICA Supersite during the Mexico City Metropolitan Area field study from 31 March-4 May 2003. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 µm (NR-PM1) with high time and size-resolution. Measurements of Black Carbon (BC) using an aethalometer, and estimated soil concentrations from Proton-Induced X-Ray Emission (PIXE) analysis of impactor substrates are also presented and combined with the AMS in order to include refractory material and estimate the total PM2.5 mass concentration at CENICA during this campaign. In Mexico City, the organic fraction of the estimated PM2.5 at CENICA represents 54.6% of the mass, with the rest consisting of inorganic compounds (mainly ammonium nitrate and sulfate/ammonium salts), BC, and soil. Inorganic compounds represent 27.5% of PM2.5; BC mass concentration is about 11%; while soil represents about 6.9%. The NR species and BC have diurnal cycles that can be qualitatively interpreted as the interplay of direct emissions, photochemical production in the atmosphere followed by condensation and gas-to-particle partitioning, boundary layer dynamics, and/or advection. Bi- and trimodal size distributions are observed for the AMS species, with a small combustion (likely traffic) organic particle mode and an accumulation mode that contains mainly organic and secondary inorganic compounds. The AMS and BC mass concentrations, size distributions, and diurnal cycles are found to be qualitatively similar to those from most previous field measurements in Mexico City.

  13. 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.

  14. Combined effects of organic aerosol loading and fog processing on organic aerosols oxidation, composition, and evolution.

    PubMed

    Chakraborty, Abhishek; Gupta, Tarun; Tripathi, S N

    2016-12-15

    Chemical characterization of ambient non-refractory submicron aerosols (NR-PM1) was carried out in real time at Kanpur, India. The measurements were performed during the winter (December 2014 to February 2015), and comprised of two very distinct high and low aerosol loading periods coupled with prevalent foggy conditions. The average non-refractory submicron aerosol loading varied significantly from high (HL, ~240μg/m(3)) to low loading (LL, ~100μg/m(3)) period and was dominated by organic aerosols (OA) which contributed more than half (~60%) of the measured aerosol mass. OA source apportionment via positive matrix factorization (PMF) showed drastic changes in the composition of OA from HL to LL period. Overall, O/C (oxygen to carbon) ratios also varied significantly from HL (=0.59) to LL (=0.69) period. Fog episodes (n=17) studied here seem to be reducing the magnitude of the negative impact of OA loading on O/C ratio (OA loading and O/C ratio are anti-correlated, as higher OA loading allows gas to particle partitioning of relatively less oxidized organics) by 60% via aqueous processing. This study provided new insights into the combined effects of OA loading and fog aqueous processing on the evolution of ambient organic aerosols (OA) for the first time.

  15. 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

  16. Aerosols

    Atmospheric Science Data Center

    2013-04-17

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-06-01

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

  18. Four dimensional variational data assimilation of species-resolved satellite-retrieved aerosol optical thickness

    NASA Astrophysics Data System (ADS)

    Nieradzik, Lars Peter; Elbern, Hendrik

    2010-05-01

    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 only 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 like mineral dust derived from desert storms and sea salt contribute to PMx it is necessary to make aerosol forcasts not only of load, but also type resolved. The source of information chosen for this study is the aerosol retrieval system SYNAER (SYNergetic AErosol Retrieval) from DLR-DFD that retrieves BLAOT (Boundary Layer Aerosol Optical Thickness) 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, sea salt, and mineral dust which are furthermore size resolved in terms of modes. A widely known technique to enhance forecast skills of CTMs (Chemistry-Transport-Models) by ingesting in-situ and, especially, remote-sensing measurements is the method of four dimensional variational data assimilation (4Dvar). 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 and internal aerosol species. Furthermore, its condensation scheme has been bypassed by an HDMR (High-Dimensional-Model-Representation) to ensure differentiability, and a time saving online NMC-module for the generation of the background

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

    NASA Astrophysics Data System (ADS)

    Guo, Liang; Turner, Andrew; Highwood, Eleanor

    2016-04-01

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

  20. Aerosol distributions and radiative forcing over the Asian Pacific region simulated by Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS)

    NASA Astrophysics Data System (ADS)

    Takemura, Toshihiko; Nakajima, Teruyuki; Higurashi, Akiko; Ohta, Sachio; Sugimoto, Nobuo

    2003-12-01

    A three-dimensional aerosol transport-radiation model coupled with a general circulation model, Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS), simulates atmospheric aerosol distributions and optical properties. The simulated results are compared with aerosol sampling and optical observations from ground, aircraft, and satellite acquired by intensive observation campaigns over east Asia in spring 2001. Temporal variations of the aerosol concentrations, optical thickness, and Ångström exponent are in good agreement between the simulation and observations. The midrange values of the Ångström exponent, even at the Asian dust storm events over the outflow regions, suggest that the contribution of the anthropogenic aerosol, such as carbonaceous and sulfate, to the total optical thickness is of an order comparable to that of the Asian dust. The radiative forcing by the aerosol direct and indirect effects is also calculated. The negative direct radiative forcing is simulated to be over -10 W m-2 at the tropopause in the air mass during the large-scale dust storm, to which both anthropogenic aerosols and Asian dust contribute almost equivalently. The direct radiative forcing, however, largely depends on the cloud water content and the vertical profiles of aerosol and cloud. The simulation shows that not only sulfate and sea salt aerosols but also black carbon and soil dust aerosols, which absorb solar and thermal radiation, make strong negative radiative forcing by the direct effect at the surface, which may exceed the positive forcing by anthropogenic greenhouse gases over the east Asian region.

  1. 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.

  2. 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

  3. 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

  4. 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

  5. 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.

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

    SciTech Connect

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

    1992-10-01

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

  7. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  9. Variability of aerosol, gaseous pollutants and meteorological characteristics associated with continental, urban and marine air masses at the SW Atlantic coast of Iberia

    NASA Astrophysics Data System (ADS)

    Diesch, J.-M.; Drewnick, F.; Zorn, S. R.; von der Weiden-Reinmüller, S.-L.; Martinez, M.; Borrmann, S.

    2011-12-01

    air masses passing the continent the organic aerosol fraction dominated the total NR-PM1. For this reason, using Positive Matrix Factorization (PMF) four organic aerosol (OA) classes that can be associated with various aerosol sources and components were identified: a highly-oxygenated OA is the major component contributing an average of 43% of the particulate organic mass while the semi-volatile OA accounts for 23%. A hydrocarbon-like OA mainly resulting from industries, traffic and shipping emissions as well as particles from wood burning emissions also contribute to total OA dependent on the air mass origin. The variability of ozone is not only affected by different types of air masses but also significantly by the diurnal variation as a consequence of the solar radiation as well as local meteorological parameters.

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

    NASA Astrophysics Data System (ADS)

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

    1992-10-01

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

  11. 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

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

    NASA Astrophysics Data System (ADS)

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

    2001-12-01

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

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

    NASA Astrophysics Data System (ADS)

    Sheridan, Patrick J.; Norton, Richard B.

    1998-04-01

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

  14. 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

  15. 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.

  16. 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.

  17. Regional influence of wildfires on aerosol chemistry in the western US and insights into atmospheric aging of biomass burning organic aerosol

    DOE PAGES

    Zhou, Shan; Collier, Sonya; Jaffe, Daniel A.; ...

    2017-02-16

    Biomass burning (BB) is one of the most important contributors to atmospheric aerosols on a global scale, and wildfires are a large source of emissions that impact regional air quality and global climate. As part of the Biomass Burning Observation Project (BBOP) field campaign in summer 2013, we deployed a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) coupled with a thermodenuder at the Mt. Bachelor Observatory (MBO, ∼  2.8 km above sea level) to characterize the impact of wildfire emissions on aerosol loading and properties in the Pacific Northwest region of the United States. MBO represents a remote background site in the western US,more » and it is frequently influenced by transported wildfire plumes during summer. Very clean conditions were observed at this site during periods without BB influence where the 5 min average (±1σ) concentration of non-refractory submicron aerosols (NR-PM1) was 3.7 ± 4.2 µg m−3. Aerosol concentration increased substantially (reaching up to 210 µg m−3 of NR-PM1) for periods impacted by transported BB plumes, and aerosol composition was overwhelmingly organic. Based on positive matrix factorization (PMF) of the HR-AMS data, three types of BB organic aerosol (BBOA) were identified, including a fresh, semivolatile BBOA-1 (O ∕ C  =  0.35; 20 % of OA mass) that correlated well with ammonium nitrate; an intermediately oxidized BBOA-2 (O ∕ C  =  0.60; 17 % of OA mass); and a highly oxidized BBOA-3 (O ∕ C  =  1.06; 31 % of OA mass) that showed very low volatility with only  ∼  40 % mass loss at 200 °C. The remaining 32 % of the OA mass was attributed to a boundary layer (BL) oxygenated OA (BL-OOA; O ∕ C  =  0.69) representing OA influenced by BL dynamics and a low-volatility oxygenated OA (LV-OOA; O ∕ C  =  1.09) representing regional aerosols in the free troposphere. The mass spectrum of BBOA-3

  18. Regional influence of wildfires on aerosol chemistry in the western US and insights into atmospheric aging of biomass burning organic aerosol

    NASA Astrophysics Data System (ADS)

    Zhou, Shan; Collier, Sonya; Jaffe, Daniel A.; Briggs, Nicole L.; Hee, Jonathan; Sedlacek, Arthur J., III; Kleinman, Lawrence; Onasch, Timothy B.; Zhang, Qi

    2017-02-01

    Biomass burning (BB) is one of the most important contributors to atmospheric aerosols on a global scale, and wildfires are a large source of emissions that impact regional air quality and global climate. As part of the Biomass Burning Observation Project (BBOP) field campaign in summer 2013, we deployed a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) coupled with a thermodenuder at the Mt. Bachelor Observatory (MBO, ˜ 2.8 km above sea level) to characterize the impact of wildfire emissions on aerosol loading and properties in the Pacific Northwest region of the United States. MBO represents a remote background site in the western US, and it is frequently influenced by transported wildfire plumes during summer. Very clean conditions were observed at this site during periods without BB influence where the 5 min average (±1σ) concentration of non-refractory submicron aerosols (NR-PM1) was 3.7 ± 4.2 µg m-3. Aerosol concentration increased substantially (reaching up to 210 µg m-3 of NR-PM1) for periods impacted by transported BB plumes, and aerosol composition was overwhelmingly organic. Based on positive matrix factorization (PMF) of the HR-AMS data, three types of BB organic aerosol (BBOA) were identified, including a fresh, semivolatile BBOA-1 (O / C = 0.35; 20 % of OA mass) that correlated well with ammonium nitrate; an intermediately oxidized BBOA-2 (O / C = 0.60; 17 % of OA mass); and a highly oxidized BBOA-3 (O / C = 1.06; 31 % of OA mass) that showed very low volatility with only ˜ 40 % mass loss at 200 °C. The remaining 32 % of the OA mass was attributed to a boundary layer (BL) oxygenated OA (BL-OOA; O / C = 0.69) representing OA influenced by BL dynamics and a low-volatility oxygenated OA (LV-OOA; O / C = 1.09) representing regional aerosols in the free troposphere. The mass spectrum of BBOA-3 resembled that of LV-OOA and had negligible contributions from the HR-AMS BB tracer ions - C2H4O2+ (m/z = 60.021) and C3H5O2+ (m/z = 73

  19. 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

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

    NASA Astrophysics Data System (ADS)

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

    2017-02-01

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

  1. 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

    2015-04-07

    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.

  2. Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Arangio, Andrea M.; Tong, Haijie; Socorro, Joanna; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-10-01

    Fine particulate matter plays a central role in the adverse health effects of air pollution. Inhalation and deposition of aerosol particles in the respiratory tract can lead to the release of reactive oxygen species (ROS), which may cause oxidative stress. In this study, we have detected and quantified a wide range of particle-associated radicals using electron paramagnetic resonance (EPR) spectroscopy. Ambient particle samples were collected using a cascade impactor at a semi-urban site in central Europe, Mainz, Germany, in May-June 2015. Concentrations of environmentally persistent free radicals (EPFR), most likely semiquinone radicals, were found to be in the range of (1-7) × 1011 spins µg-1 for particles in the accumulation mode, whereas coarse particles with a diameter larger than 1 µm did not contain substantial amounts of EPFR. Using a spin trapping technique followed by deconvolution of EPR spectra, we have also characterized and quantified ROS, including OH, superoxide (O2-) and carbon- and oxygen-centered organic radicals, which were formed upon extraction of the particle samples in water. Total ROS amounts of (0.1-3) × 1011 spins µg-1 were released by submicron particle samples and the relative contributions of OH, O2-, C-centered and O-centered organic radicals were ˜ 11-31, ˜ 2-8, ˜ 41-72 and ˜ 0-25 %, respectively, depending on particle sizes. OH was the dominant species for coarse particles. Based on comparisons of the EPR spectra of ambient particulate matter with those of mixtures of organic hydroperoxides, quinones and iron ions followed by chemical analysis using liquid chromatography mass spectrometry (LC-MS), we suggest that the particle-associated ROS were formed by decomposition of organic hydroperoxides interacting with transition metal ions and quinones contained in atmospheric humic-like substances (HULIS).

  3. Efficacy of RNA interference knockdown using aerosolized short interfering RNAs bound to nanoparticles in three diverse aphid species.

    PubMed

    Thairu, M W; Skidmore, I H; Bansal, R; Nováková, E; Hansen, T E; Li-Byarlay, H; Wickline, S A; Hansen, A K

    2017-03-17

    RNA interference (RNAi) has emerged as a promising method for validating gene function; however, its utility in nonmodel insects has proven problematic, with delivery methods being one of the main obstacles. This study investigates a novel method of RNAi delivery in aphids, the aerosolization of short interfering RNA (siRNA)-nanoparticle complexes. By using nanoparticles as a siRNA carrier, the likelihood of cellular uptake is increased, when compared to methods previously used in insects. To determine the efficacy of this RNAi delivery system, siRNAs were aerosolized with and without nanoparticles in three aphid species: Acyrthosiphon pisum, Aphis glycines and Schizaphis graminum. The genes targeted for knockdown were carotene dehydrogenase (tor), which is important for pigmentation in Ac. pisum, and branched chain-amino acid transaminase (bcat), which is essential in the metabolism of branched-chain amino acids in all three aphid species. Overall, we observed modest gene knockdown of tor in Ac. pisum and moderate gene knockdown of bcat in Ap. glycines along with its associated phenotype. We also determined that the nanoparticle emulsion significantly increased the efficacy of gene knockdown. Overall, these results suggest that the aerosolized siRNA-nanoparticle delivery method is a promising new high-throughput and non-invasive RNAi delivery method in some aphid species.

  4. 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.

  5. 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

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

    DOE PAGES

    Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; ...

    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

  7. The use of ambient measurements to identify which precursor species limit aerosol nitrate formation.

    PubMed

    Blanchard, C L; Roth, P M; Tanenbaum, S J; Ziman, S D; Seinfeld, J H

    2000-12-01

    A thermodynamic equilibrium model was used to investigate the response of aerosol NO3 to changes in concentrations of HNO3, NH3, and H2SO4. Over a range of temperatures and relative humidities (RHs), two parameters provided sufficient information for indicating the qualitative response of aerosol NO3. The first was the excess of aerosol NH4+ plus gas-phase NH3 over the sum of HNO3, particulate NO3, and particulate SO4(2-) concentrations. The second was the ratio of particulate to total NO3 concentrations. Computation of these quantities from ambient measurements provides a means to rapidly analyze large numbers of samples and identify cases in which inorganic aerosol NO3 formation is limited by the availability of NH3. Example calculations are presented using data from three field studies. The predictions of the indicator variables and the equilibrium model are compared.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  9. 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.

  10. Hazardous components and health effects of atmospheric aerosol particles: reactive oxygen species, soot, polycyclic aromatic compounds and allergenic proteins.

    PubMed

    Shiraiwa, Manabu; Selzle, Kathrin; Pöschl, Ulrich

    2012-08-01

    This review outlines recent advances in the investigation of the chemical properties, molecular interactions and health effects of hazardous compounds in atmospheric aerosols, in particular reactive oxygen species (ROS), soot, polycyclic aromatic compounds (PACs) and allergenic proteins. Epidemiological studies show correlations between air particulate matter and adverse health effects of air pollution including allergy, asthma, cardiovascular and respiratory diseases, but the causative relations and mechanisms of interaction on the molecular level are still unclear. ROS generated by photochemical and heterogeneous reactions in the atmosphere seem to play a key role in aerosol health effects and provide a direct link between atmospheric and physiological multiphase processes. Soot and PACs can trigger formation of ROS in vivo, leading to inflammation and cellular damage. PACs as well as allergenic proteins are efficiently oxygenated and nitrated upon exposure to ozone and nitrogen dioxide, which leads to an enhancement of their toxicity and allergenicity.

  11. 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.

  12. Formic Sulfuric Anhydride: a New Chemical Species with Possible Implications for Atmospheric Aerosol

    NASA Astrophysics Data System (ADS)

    Mackenzie, Becca; Dewberry, Chris; Leopold, Ken

    2015-06-01

    Aerosols are important players in the Earth's atmosphere, affecting climate, cloud formation, and human health. In this work, we report the discovery of a previously unknown molecule, formic sulfuric anhydride (FSA), that may influence the formation and composition of atmospheric aerosol particles. Five isotopologues of FSA have been observed by microwave spectroscopy and further characterized using DFT calculations. The system has dipole moment components along all three inertial axes, and indeed a, b, and c-type transitions have been observed. A π2 + π2 + σ2 cycloaddition reaction between SO3 and HCOOH is proposed as a possible mechanism for the formation of FSA and calculations indicate that the transformation is effectively barrierless. Facile formation of the anhydride followed by hydrolysis in small water-containing clusters or liquid droplets may provide a mechanism of incorporating volatile organics into atmospheric aerosol. We suggest that FSA and its derivatives be considered in future atmospheric and climate models.

  13. E-Cigarette Aerosol Exposure Induces Reactive Oxygen Species, DNA Damage, and Cell Death in Vascular Endothelial Cells.

    PubMed

    Anderson, Chastain; Majeste, Andrew; Hanus, Jakub; Wang, Shusheng

    2016-12-01

    Cigarette smoking remains one of the leading causes of preventable death worldwide. Vascular cell death and dysfunction is a central or exacerbating component in the majority of cigarette smoking related pathologies. The recent development of the electronic nicotine delivery systems known as e-cigarettes provides an alternative to conventional cigarette smoking; however, the potential vascular health risks of e-cigarette use remain unclear. This study evaluates the effects of e-cigarette aerosol extract (EAE) and conventional cigarette smoke extract (CSE) on human umbilical vein endothelial cells (HUVECs). A laboratory apparatus was designed to produce extracts from e-cigarettes and conventional cigarettes according to established protocols for cigarette smoking. EAE or conventional CSE was applied to human vascular endothelial cells for 4-72 h, dependent on the assay. Treated cells were assayed for reactive oxygen species, DNA damage, cell viability, and markers of programmed cell death pathways. Additionally, the anti-oxidants α-tocopherol and n-acetyl-l-cysteine were used to attempt to rescue e-cigarette induced cell death. Our results indicate that e-cigarette aerosol is capable of inducing reactive oxygen species, causing DNA damage, and significantly reducing cell viability in a concentration dependent fashion. Immunofluorescent and flow cytometry analysis indicate that both the apoptosis and programmed necrosis pathways are triggered by e-cigarette aerosol treatment. Additionally, anti-oxidant treatment provides a partial rescue of the induced cell death, indicating that reactive oxygen species play a causal role in e-cigarette induced cytotoxicity.

  14. Global three-dimensional simulation and radiative forcing of various aerosol species with GCM

    NASA Astrophysics Data System (ADS)

    Takemura, Toshihiko; Okamoto, Hajime; Numaguti, Atusi; Suzuki, Kentaroh; Higurashi, Akiko; Nakajima, Teruyuki

    2001-02-01

    A global three-dimensional transport model that can simultaneously treat main tropospheric aerosols, i.e., carbonaceous (organic and black carbons), sulfate, soil dust, and sea salt, is developed. It is coupled with a Center for Climate System Research (CCSR)/National Institute for Enviormental Studies (NIES) atmospheric general circulation model (AGCM), and the meteorological field of wind, temperature, and specific humidity can be nudged by reanalysis data. Simulated results are compared with not only observations for aerosol concentrations but also the optical thickness and Angstrom exponent retrieved from remote sensing data such as National Oceanic and Atmospheric Administration (NOAA)/Advanced Very High Resolution Radiometer (AVHRR) and Aerosol Robotic Network (AERONET). A general agreement is found between simulated results and observations spatially seasonally, and quantitatively. The present model is also coupled with the radiative process over both the solar and thermal regions. The annual and global mean radiative forcing by anthropogenic aerosols from fossil fuel sources is estimated to be -0.5 W m-2 over the clear sky for the direct effect and -2.0 W m-2 for the indirect effect.

  15. 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

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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.

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

    SciTech Connect

    SAJO, ERNO

    2012-07-31

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

  2. 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

  3. Release of Reactive Halogen Species from Sea-Salt Aerosols under Tropospheric Conditions with/without the Influence of Organic Matter in Smog-Chamber Experiments

    NASA Astrophysics Data System (ADS)

    Balzer, N.; Behnke, W.; Bleicher, S.; Krueger, H.; Ofner, J.; Siekmann, F.; Zetzsch, C.

    2008-12-01

    Experiments to investigate the release of reactive halogen species from sea-salt aerosol and the influence of organic matter were performed in an aerosol smog-chamber (3500 l), made of Teflon film (FEP 200A, Dupont). Smog chamber facilities at lowered temperature (coolable down to -25°C) enable us to simulate these reactions under polar, tropospheric conditions. First experiments were performed to investigate the production of atomic Br and Cl without the impact of organic aerosol. Br and Cl play an important role in atmospheric ozone depletion, particularly regarding ozone depletion events (bromine explosion) during polar spring. In these studies, the aerosol was generated by atomizing salt solutions containing the typical Br/Cl ratio of 1/660 in seawater by an ultrasonic nebulizer and increasing the Br content up to sixfold. To ensure the aqueous surface of the aerosol, the experiments were performed at relative humidities above 76%. We determined the atomic Cl and OH-radical concentrations from the simultaneous consumption of four reference hydrocarbons. The Br-radical concentration was calculated on the basis of ozone depletion. Organic aerosol may take part in these reaction cycles by halogenation and production of volatile organic halogens. Further experiments are planned to add organic aerosol for mechanistic and kinetic studies on the influence of secondary organic aerosols (SOA) and humic-like substances (HULIS) on bromine explosion. The formation of the secondary organic aerosol and the determination of possible halogenated gaseous and solid organic products will be studied using longpath-FTIR, DRIFTS, ATR-FTIR, GC-FID, GC-ECD, GC-MS, TPD-MS and DMA-CNC.

  4. 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.

  5. Detailed mass size distributions of atmospheric aerosol species in the Negev desert, Israel, during ARACHNE-96

    NASA Astrophysics Data System (ADS)

    Maenhaut, Willy; Ptasinski, Jacek; Cafmeyer, Jan

    1999-04-01

    As part of the 1996 summer intensive of the Aerosol, RAdiation and CHemistry Experiment (ARACHNE-96), the mass size distribution of various airborne particulate elements was studied at a remote site in the Negev Desert, Israel. Aerosol collections were made with 8-stage PIXE International cascade impactors (PCIs) and 12-stage small deposit area low pressure impactors (SDIs) and the samples were analyzed by PIXE for about 20 elements. The mineral elements (Al, Si, Ca, Ti, Fe) exhibited a unimodal size distribution which peaked at about 6 μm, but the contribution of particles larger than 10 μm was clearly more pronounced during the day than during night. Sulphur and Br had a tendency to exhibit two modes in the submicrometer size range, with diameters at about 0.3 and 0.6 μm, respectively. The elements V and Ni, which are indicators of residual fuel burning, showed essentially one fine mode (at 0.3 μm) in addition to a coarse mode which represented the mineral dust contribution. Overall, good agreement was observed between the mass size distributions from the PCI and SDI devices. The PCI was superior to the SDI for studying the size distribution in the coarse size range, but the SDI was clearly superior for unravelling the various modes in the submicrometer size range.

  6. 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 ...

  7. 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.

  8. 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.

  9. Analysis of organic and inorganic species on the surface of atmospheric aerosol using time-of-flight secondary ion mass spectrometry (TOF-SIMS)

    NASA Astrophysics Data System (ADS)

    Peterson, Richard E.; Tyler, Bonnie J.

    This work explores the utility of time-of-flight static secondary-ion mass spectrometry (TOF-SIMS) for the analysis of the surface organic layer on individual atmospheric aerosol particles. The surface sensitivity and minimal fragmentation available with TOF-SIMS suggest that it can be a powerful tool for the examination of the organic and inorganic species on the surface of individual particles. Cascade impactors were used to collect aerosol from summer 2000 Montana forest fires, winter snowmobile samples in Yellowstone National Park, Hawaiian lava and sea salt, from an Asian Dust event reaching Salt Lake City, Utah in April 2001 and from Salt Lake Valley summer urban aerosol. TOF-SIMS analysis and multivariate statistical techniques combined gave chemical and morphological information about the particles. Surfaces of the aerosol from forest fires, snowmobile exhaust, and sea salt were all dominated by aliphatic hydrocarbons and their amphiphilic derivatives. Each source showed a different organic chemical signature. The extent and composition of the organics layer which typically covers the surface of atmospheric particles are expected to effect all of the surface related aerosol properties such as health effects, the ability of the particle to activate and form cloud droplets, and the aggregation of particles as well as reactions between the particle and gas phase species.

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

    PubMed

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

    2013-09-01

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

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

    NASA Astrophysics Data System (ADS)

    Pavlovic, Jelica

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

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

    NASA Astrophysics Data System (ADS)

    Zhang, 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

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

    NASA Astrophysics Data System (ADS)

    Zhang, 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

  14. 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

  15. Identification of nitrogenous organic species in Titan aerosols analogs: Nitrogen fixation routes in early atmospheres

    NASA Astrophysics Data System (ADS)

    He, Chao; Smith, Mark A.

    2013-09-01

    Titan, an icy world surrounded by auburn organic haze, is considered as one of the best targets for studying abiotic planetary organic chemistry. In spite of a great many efforts being made, the chemistry in Titan’s atmosphere and its resulting chemical structures are still not fully understood. In our previous work, we have investigated the structure of Titan aerosols analogs (tholin) by NMR and identified hexamethylenetetramine as a dominant small molecule in Titan tholin. Here we report a more complete and definitive structural investigation of the small molecule inventory in Titan tholin. We identified several nitrogenous organic molecules including cyanamide, guanidine, 2-cyanoguanidine, melamine, N‧-cyanoformamidine and 1,2,4-triazole in Titan tholin by using NMR and GC-MS and standard sample comparison. The structural characteristics of these molecules suggest a possible formation pathway from the reaction of HCN and NH3, both of which are known to exist in appreciable density in the atmosphere and were tentatively detected by the Huygens probe.

  16. Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin

    NASA Astrophysics Data System (ADS)

    Trebs, I.; Meixner, F. X.; Slanina, J.; Otjes, R.; Jongejan, P.; Andreae, M. O.

    2004-06-01

    We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2 and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl- and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate: Aerosols from Biomass Burning Perturb Global and Regional Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder (WAD) in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015ppb for acidic trace gases and aerosol anions and ≤0.118ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative

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

    PubMed

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

    2013-11-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  20. Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin

    NASA Astrophysics Data System (ADS)

    Trebs, I.; Meixner, F. X.; Slanina, J.; Otjes, R.; Jongejan, P.; Andreae, M. O.

    2004-02-01

    We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2) and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl-) and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia Smoke Aerosols, Clouds, Rainfall and Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015 ppb for acidic trace gases and aerosol anions and ≤0.118 ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative humidity and temperature variations between day and night as well as to

  1. Analysis of inorganic mercury species associated with airborne particulate matter/aerosols: method development.

    PubMed

    Feng, Xinbin; Lu, Julia Y; Grègoire, D Conrad; Hao, Yingjie; Banic, Catharine M; Schroeder, William H

    2004-10-01

    This paper describes a method for speciation of Hg associated with airborne particulate matter. This method uses a mini-sampler for sample collection and analysis, thermal desorption for separating Hg species, and inductively coupled plasma mass spectrometry (ICP-MS) for identification and quantification of Hg. Coal fly ash spiked with different Hg compounds (e.g. Hg0, HgCl2, HgO, and HgS) was used for qualitative calibration. A standard reference material with a certified value for Hg concentration was used to evaluate the method. When the temperature of the furnace was programmed at a linear rate of increase of 50 degrees min(-1), different Hg compounds could clearly be separated. Three airborne particulate matter samples were collected in parallel in Toronto, ON, Canada and analyzed using this method. Reproducible results were obtained and Hg0, HgCl2, HgO, and HgS species from these samples were detected.

  2. 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.

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

    PubMed

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

    2013-01-01

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

  4. Seasonal changes in Fe species and soluble Fe concentration in the atmosphere in the Northwest Pacific region based on the analysis of aerosols collected in Tsukuba, Japan

    NASA Astrophysics Data System (ADS)

    Takahashi, Y.; Furukawa, T.; Kanai, Y.; Uematsu, M.; Zheng, G.; Marcus, M. A.

    2013-03-01

    Atmospheric iron (Fe) can be a significant source of nutrition for phytoplankton inhabiting remote oceans, which in turn has a large influence on the Earth's climate. The bioavailability of Fe in aerosols depends mainly on the fraction of soluble Fe (= [FeSol]/[FeTotal], where [FeSol] and [FeTotal] are the atmospheric concentrations of soluble and total Fe, respectively). However, the numerous factors affecting the soluble Fe fraction have not been fully understood. In this study, the Fe species, chemical composition, and soluble Fe concentrations in aerosols collected in Tsukuba, Japan were investigated over a year (nine samples from December 2002 to October 2003) to identify the factors affecting the amount of soluble Fe supplied into the ocean. The soluble Fe concentration in aerosols is correlated with those of sulfate and oxalate originated from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. Moreover, the soluble Fe concentration is also correlated with the enrichment factors of vanadium and nickel emitted by fossil fuel combustion. These results suggest that the degree of Fe dissolution is influenced by the magnitude of anthropogenic activity, such as fossil fuel combustion. X-ray absorption fine structure (XAFS) spectroscopy was performed in this study to identify the Fe species in aerosols. The fitting of XAFS spectra coupled with micro X-ray fluorescence analysis (XRF) determined the main Fe species in aerosols in Tsukuba to be illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, the soluble Fe fraction in each sample measured by leaching experiments is closely correlated with the Fe(III) sulfate fraction determined by the XAFS spectrum fitting, suggesting that Fe(III) sulfate is the main soluble Fe in the ocean. Another possible factor that can control the amount of soluble Fe supplied into the ocean is the total Fe(III) concentration in the atmosphere, which was high in spring due to the high

  5. Seasonal changes in Fe species and soluble Fe concentration in the atmosphere in the Northwest Pacific region based on the analysis of aerosols collected in Tsukuba, Japan

    NASA Astrophysics Data System (ADS)

    Takahashi, Y.; Furukawa, T.; Kanai, Y.; Uematsu, M.; Zheng, G.; Marcus, M. A.

    2013-08-01

    Atmospheric iron (Fe) can be a significant source of nutrition for phytoplankton inhabiting remote oceans, which in turn has a large influence on the Earth's climate. The bioavailability of Fe in aerosols depends mainly on the fraction of soluble Fe (= [FeSol]/[FeTotal], where [FeSol] and [FeTotal] are the atmospheric concentrations of soluble and total Fe, respectively). However, the numerous factors affecting the soluble Fe fraction have not been fully understood. In this study, the Fe species, chemical composition, and soluble Fe concentrations in aerosols collected in Tsukuba, Japan were investigated over a year (nine samples from December 2002 to October 2003) to identify the factors affecting the amount of soluble Fe supplied into the ocean. The soluble Fe concentration in aerosols is correlated with those of sulfate and oxalate originated from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. Moreover, the soluble Fe concentration is also correlated with the enrichment factors of vanadium and nickel emitted by fossil fuel combustion. These results suggest that the degree of Fe dissolution is influenced by the magnitude of anthropogenic activity, such as fossil fuel combustion. X-ray absorption fine structure (XAFS) spectroscopy was performed in order to identify the Fe species in aerosols. Fitting of XAFS spectra coupled with micro X-ray fluorescence analysis (μ-XRF) showed the main Fe species in aerosols in Tsukuba to be illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, the soluble Fe fraction in each sample measured by leaching experiments is closely correlated with the Fe(III) sulfate fraction determined by the XAFS spectrum fitting, suggesting that Fe(III) sulfate is the main soluble Fe in the ocean. Another possible factor that can control the amount of soluble Fe supplied into the ocean is the total Fe(III) concentration in the atmosphere, which was high in spring due to the high mineral

  6. Some environmental considerations relating to the interaction of the solid rocket motor exhaust with the atmosphere: Predicted chemical composition of exhaust species and predicted conditions for the formation of HCl aerosol

    NASA Technical Reports Server (NTRS)

    Rhein, R. A.

    1973-01-01

    The exhaust products of a solid rocket motor using as propellant 14% binder, 16% aluminum, and 70% (wt) ammonium perchlorate consist of hydrogen chloride, water, alumina, and other compounds. The equilibrium and some frozen compositions of the chemical species upon interaction with the atmosphere were computed. The conditions under which hydrogen chloride interacts with the water vapor in humid air to form an aerosol containing hydrochloric acid were computed for various weight ratios of air/exhaust products. These computations were also performed for the case of a combined SRM and hydrogen-oxygen rocket engine. Regimes of temperature and relative humidity where this aerosol is expected were identified. Within these regimes, the concentration of HCL in the aerosol and weight fraction of aerosol to gas phase were plotted. Hydrochloric acid aerosol formation was found to be particularly likely in cool humid weather.

  7. Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

    NASA Astrophysics Data System (ADS)

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

    2015-07-01

    We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

  8. 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

  9. 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

  10. 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

  11. 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

  12. 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.

  13. 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.

  14. 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

  15. Contribution of water-soluble and insoluble components and their hydrophobic/hydrophilic subfractions to the reactive oxygen species-generating potential of fine ambient aerosols.

    PubMed

    Verma, Vishal; Rico-Martinez, Roberto; Kotra, Neel; King, Laura; Liu, Jiumeng; Snell, Terry W; Weber, Rodney J

    2012-10-16

    Relative contributions of water- and methanol-soluble compounds and their hydrophobic/hydrophilic subfractions to the ROS (reactive oxygen species)-generating potential of ambient fine aerosols (D(p) < 2.5 μm) are assessed. ROS-generating (or oxidative) potential of the particulate matter (PM) was measured by the dithiothreitol (DTT) assay. Particles were collected on quartz filters (N = 8) at an urban site near central Atlanta during January-February 2012 using a PM(2.5) high-volume sampler. Filter punches were extracted separately in both water and methanol. Hydrophobic and hydrophilic fractions were then subsequently segregated via a C-18 solid phase extraction column. The DTT assay response was significantly higher for the methanol extract, and for both extracts a substantial fraction of PM oxidative potential was associated with the hydrophobic compounds as evident from a substantial attenuation in DTT response after passing PM extracts through the C-18 column (64% for water and 83% for methanol extract; both median values). The DTT activities of water and methanol extracts were correlated with the water-soluble (R = 0.86) and water-insoluble organic carbon (R = 0.94) contents of the PM, respectively. Brown carbon (BrC), which predominantly represents the hydrophobic organic fraction (referred to as humic-like substances, HULIS), was also correlated with DTT activity in both the water (R = 0.78) and methanol extracts (R = 0.83). Oxidative potential was not correlated with any metals measured in the extracts. These findings suggest that the hydrophobic components of both water-soluble and insoluble organic aerosols substantially contribute to the oxidative properties of ambient PM. Further investigation of these hydrophobic organic compounds could help identify sources of a significant fraction of ambient aerosol toxicity.

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

    NASA Astrophysics Data System (ADS)

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

    2016-11-01

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

  17. 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.

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

    DOE PAGES

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

    2015-04-01

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

  19. 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.

  20. 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.

  1. Unified Aerosol Microphysics for NWP

    DTIC Science & Technology

    2011-09-30

    Specifically, the goal is to develop a COAMPS that is capable of simulating the full range of interactions between aerosol particles, clouds , and radiative...aerosol species that are responsible for degradation of Electro- Optical (EO) propagation or that modify cloud behavior and lifetime. Report...enabling new development of more complex cloud -aerosol interactions. The work on this project has been divided into two phases, an investigation phase

  2. 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.

  3. 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.

  4. Infrared spectroscopy of aerosols

    NASA Astrophysics Data System (ADS)

    Mentel, Th.; Sebald, H.

    2003-04-01

    In our large Aerosol Chamber at the FZ Jülich we apply HR FTIR absorption spectroscopy for the determination of trace gases. In the FTIR spectra we also observe broad absorptions of several 10 to a few 100 cm-1 widths that arise from species in the condensed aerosol phase: liquid H_2O, NO_3^-, SO_42-, HSO_4^-, or dicarboxylic acids. Moreover, the aerosol droplets caused extinctions over several 1000 cm-1 by IR scattering. This allows for in-situ observation of changes in the condensed aerosol phase e.g. on HNO_3 uptake, like the shift of the sulfate/bisulfate equilibrium or the growth by water condensation. The IR absorptions of the condensed aerosol phase provide useful extra information in process studies, if they can be quantified. Therefore the absorption cross section, respective, the absorption index which is the imaginary part of the complex refractive index is needed. We set up an aerosol flow tube in which IR spectroscopy on a 8 m light path and aerosol size distribution measurements in the range from 20 nm - 10 μm can be performed simultaneously. We measured sulfate aerosols at several relative humidities (dry, metastable, deliquescent). We will demonstrate an iterative procedure based on Mie calculations and Kramers Kronig transformation to retrieve the absorption index from the observed IR spectra and the corresponding size distribution (for dry ammonium sulfate). We will compare resulting absorption indices for aqueous sodium bisulfate aerosols at several relative humidties with thermodynamic model calculations for the Na^+/H^+/HSO_4^-/SO_42-/H_2O system.

  5. Determination of aerosol ammonium using an aerodyne aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Delia, A. E.; Toohey, D. W.; Worsnop, D. R.

    2003-04-01

    The chemical composition of fine aerosols is a significant issue both because it influences the chemical and radiative properties of the aerosols, which in turn impact the regional and global climate and human health, and because it is difficult to measure accurately. The Aerosol Mass Spectrometer (AMS) developed by Aerodyne Research measures both chemical composition and aerodynamic size of submicron aerosols quantitatively. However, the measurement of aerosol ammonium is more difficult than that of the other major inorganic species, nitrate and sulfate, because of interferences in the mass spectrum from air and water. This presentation will describe the successful procedure developed for dealing with these interferences and accurately determining the ammonium mass. In addition, the application of this procedure to aerosols from a range of ambient conditions will be demonstrated using data from several field studies.

  6. Effect of aerosol subgrid variability on aerosol optical depth and cloud condensation nuclei: implications for global aerosol modelling

    NASA Astrophysics Data System (ADS)

    Weigum, Natalie; Schutgens, Nick; Stier, Philip

    2016-11-01

    A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid boxes, which can lead to discrepancies in simulated aerosol climate effects between high- and low-resolution models. This study investigates the impact of neglecting subgrid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem (Weather and Research Forecast model) runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. The processes most affected by neglecting aerosol subgrid variability are gas-phase chemistry and aerosol uptake of water through aerosol-gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol properties when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of subgrid variability on these

  7. Sources of chemical species in rainwater during monsoon and non-monsoonal periods over two mega cities in India and dominant source region of secondary aerosols

    NASA Astrophysics Data System (ADS)

    Rao, P. S. P.; Tiwari, S.; Matwale, J. L.; Pervez, S.; Tunved, P.; Safai, P. D.; Srivastava, A. K.; Bisht, D. S.; Singh, S.; Hopke, P. K.

    2016-12-01

    Samples of rainwater (RW) were collected to characterize the chemistry and sources in two representative megacities at Pune (Southwest) and Delhi (Northern) India from 2011 to 2014 across two seasons: monsoon (MN) and non-monsoon (NMN). Collected RW samples were analyzed for major chemical constituents (F-, Cl-, SO42-, NO3-, NH4+, Na+, K+, Ca2+, and Mg2+), pH and conductivity. In addition, bicarbonate (HCO3-) was also estimated. The mean pH values of the RW were >6 at Pune and <6 at Delhi and 4% and 26% were acidic, respectively. The mean sum of all measured ionic species in Pune and Delhi was 304.7 and 536.4 μeq/l, respectively, indicating that significant atmospheric pollution effects in these Indian mega cities. Both the Ca2+ and SO42- were the dominant ions, accounting for 43% (Pune) and 54% (Delhi) of the total ions. The sum of measured ions during the NMN period was greater than the NM period by a factor of 1.5 for Pune (278.4: NM and 412.1: NMN μeq/l) and a factor of about 2.5 for Delhi (406 and 1037.7 μeq/l). The contributions of SO42- and NO3- to the RW acidity were ∼40% and 60%, respectively, at Pune and correspondingly, 36% and 64% at Delhi. The concentrations of secondary aerosols (SO42-and NO3-) were higher by a factor of two and three when the air masses were transported to Pune from the continental side. At Delhi, the concentrations of SO42-, NO3-, Ca2+, and Mg2+ were significantly higher when the air masses arrive from Punjab, Haryana, and Pakistan indicating the greater atmospheric pollution over the Indo-Gangetic Plain. Positive matrix factorization was applied to the source apportionment of the deposition fluxes of these ions. Three factors were obtained for Pune and four for Delhi. The sources at Pune were secondary aerosols from fossil fuel combustion, soil dust, and marine, whereas, at Delhi, the sources were soil, fossil fuel combustion, biomass burning, and industrial chlorine.

  8. 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

  9. 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.

  10. Aerosol and monsoon climate interactions over Asia: AEROSOL AND MONSOON CLIMATE INTERACTIONS

    SciTech Connect

    Li, Zhanqing; Lau, W. K. -M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S. -S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

    2016-11-15

    Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. The atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.

  11. 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.

  12. ENCAPSULATED AEROSOLS

    DTIC Science & Technology

    acetate, polymerized rapidly and produced some polymer film encapsulation of the aerosol droplets. A two-stage microcapsule generator was designed...encapsulating material, the generator also produced microcapsules of dibutyl phosphite in polyethylene, nitrocellulose, and natural rubber.

  13. Aerosol Microphysics and Radiation Integration

    DTIC Science & Technology

    2016-06-13

    storm activity, and 4) surface and airborne measurements on the west coast of the U.S. indicate the presence of aerosols and dust on the predicted...observables (in situ and satellites) and model quantities such as mass. Aerosol species currently included in the analyses are dust , pollution, biomass...Prediction System ( COAMPS ®). Over the next several years it is the goal of this project to maintain these systems as the world leaders in EO prediction

  14. 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

  15. Water absorption by secondary organic aerosol and its effect on inorganic aerosol behavior

    SciTech Connect

    Ansari, A.S.; Pandis, S.N.

    2000-01-01

    The hygroscopic nature of atmospheric aerosol has generally been associated with its inorganic fraction. In this study, a group contribution method is used to predict the water absorption of secondary organic aerosol (SOA). Compared against growth measurements of mixed inorganic-organic particles, this method appears to provide a first-order approximation in predicting SOA water absorption. The growth of common SOA species is predicted to be significantly less than common atmospheric inorganic salts such as (NH{sub 4}){sub 2}SO{sub 4} and NaCl. Using this group contribution method as a tool in predicting SOA water absorption, an integrated modeling approach is developed combining available SOA and inorganic aerosol models to predict overall aerosol behavior. The effect of SOA on water absorption and nitrate partitioning between the gas and aerosol phases is determined. On average, it appears that SOA accounts for approximately 7% of total aerosol water and increases aerosol nitrate concentrations by approximately 10%. At high relative humidity and low SOA mass fractions, the role of SOA in nitrate partitioning and its contribution to total aerosol water is negligible. However, the water absorption of SOA appears to be less sensitive to changes in relative humidity than that of inorganic species, and thus at low relative humidity and high SOA mass fraction concentrations, SOA is predicted to account for approximately 20% of total aerosol water and a 50% increase in aerosol nitrate concentrations. These findings could improve the results of modeling studies where aerosol nitrate has often been underpredicted.

  16. 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.

  17. 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

  18. 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.

  19. Influence of local and regional sources on the observed spatial and temporal variability of size resolved atmospheric aerosol mass concentrations and water-soluble species in the Athens metropolitan area

    NASA Astrophysics Data System (ADS)

    Eleftheriadis, Konstantinos; Ochsenkuhn, Klaus M.; Lymperopoulou, Theopisti; Karanasiou, Angeliki; Razos, Panayiotis; Ochsenkuhn-Petropoulou, Maria

    2014-11-01

    The variability of common aerosol species in large Metropolitan urban areas is a major air quality issue with strong health impacts of large populations. PM10 and PM2.5 particulate matter samples were obtained at three sites characteristic of industrial, urban traffic and sub-urban residential areas in the Athens basin. Samples were analysed for anions (Cl-, NO3-, SO42-) and cations (K+, Na+, Ca2+, Mg2+, NH4+) using ion chromatography. The spatial and temporal variability for the particulate matter (PM) concentration mass and water-soluble ionic species concentrations for the investigated sites were studied. Mean PM fine concentration levels were 20% higher at the industrial and the central urban areas compared to those in the suburban area (24.2 μg/m3). The mean values for the coarse fraction at those two sites were two to three times higher compared to those at the suburban site (12.4 μg/m3). Comparable concentration levels of most species were observed in all areas, while SO42- and NO3- differ at a significant level. Furthermore, the average size distributions of the mass and individual ions at the suburban site (NCSR Demokritos) showed a bimodal size distribution. SO42- and NH4+ have their main peak in the fine fraction while NO3- showed equal distribution on the fine and coarse mode.. Good correlation was found for SO42- and NO3- with Ca2+ and Na+ with Cl- for the coarse fraction in the industrial area. NH4+ was closely correlated with SO42- in the fine particles and in all areas. For the urban site the best correlations in coarse particulates were reported between Na+/Mg2+-Cl-, Ca2+/Mg2+-SO42-, explained by neutralization of acidic aerosol by soil dust and sea salt in the coarse fraction. Moreover, time weighted concentrations roses at the industrial and urban sites, showed no significant directional dependence, indicating either uniform generation of mainly the coarse species within the metropolitan area or major influence of the regional background for

  20. Aerosol and monsoon climate interactions over Asia

    NASA Astrophysics Data System (ADS)

    Li, Zhanqing; Lau, W. K.-M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S.-S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

    2016-12-01

    The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from

  1. ENCAPSULATED AEROSOLS

    DTIC Science & Technology

    materials determine the range of applicability of each method. A useful microencapsulation method, based on coagulation by inertial force was developed...The generation apparatus, consisting of two aerosol generators in series, was utilized to produce many kinds of microcapsules . A fluid energy mill...was found useful for the production of some microcapsules . The permeability of microcapsule films and the effect of exposure time and humidity were

  2. Absorbing aerosols over Asia: A Geophysical Fluid Dynamics Laboratory general circulation model sensitivity study of model response to aerosol optical depth and aerosol absorption

    NASA Astrophysics Data System (ADS)

    Randles, C. A.; Ramaswamy, V.

    2008-11-01

    Forcing by absorbing atmospheric black carbon (BC) tends to heat the atmosphere, cool the surface, and reduce the surface latent and sensible heat fluxes. BC aerosol can have a large impact on regional climates and the hydrologic cycle. However, significant uncertainties remain concerning the increases in (1) the total amount of all aerosol species and (2) the amount of aerosol absorption that may have occurred over the 1950-1990 period. Focusing on south and east Asia, the sensitivity of a general circulation model's climate response (with prescribed sea surface temperatures and aerosol distributions) to such changes is investigated by considering a range of both aerosol absorption and aerosol extinction optical depth increases. We include direct and semidirect aerosol effects only. Precipitation changes are less sensitive to changes in aerosol absorption optical depth at lower aerosol loadings. At higher-extinction optical depths, low-level convergence and increases in vertical velocity overcome the stabilizing effects of absorbing aerosols and enhance the monsoonal circulation and precipitation in northwestern India. In contrast, the presence of increases in only scattering aerosols weakens the monsoonal circulation and inhibits precipitation here. Cloud amount changes can enhance or counteract surface solar flux reduction depending on the aerosol loading and absorption, with the changes also influencing the surface temperature and the surface energy balance. The results have implications for aerosol reduction strategies in the future that seek to mitigate air pollution concerns. At higher optical depths, if absorbing aerosol is present, reduction of scattering aerosol alone has a reduced effect on precipitation changes, implying that reductions in BC aerosols should be undertaken at the same time as reductions in sulfate aerosols.

  3. Photothermal spectroscopy of aerosols

    SciTech Connect

    Campillo, A.J.; Lin, H.B.

    1981-04-01

    In situ aerosol absorption spectroscopy was performed using two novel photothermal detection schemes. The first, based on a photorefractive effect and coherent detection, called phase fluctuation optical heterodyne (PFLOH) spectroscopy, could, depending on the geometry employed, yield particle specific or particle and gas absorption data. Single particles of graphite as small as 1 ..mu..m were detected in the particle specific mode. In another geometrical configuration, the total absorption (both gas and particle) of submicron sized aerosols of ammonium sulfate particles in equilibrium with gaseous ammonia and water vapor were measured at varying CO/sub 2/ laser frequencies. The specific absorption coefficient for the sulfate ion was measured to be 0.5 m/sup 2//g at 1087 cm/sup -1/. The absorption coefficient sensitivity of this scheme was less than or equal to 10/sup -8/ cm/sup -1/. The second scheme is a hybrid visible Mie scattering scheme incorporating photothermal modulation. Particle specific data on ammonium sulfate droplets were obtained. For chemically identical species, the relative absorption spectrum versus laser frequency can be obtained for polydisperse aerosol distributions directly from the data without the need for complex inverse scattering calculations.

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

    DOE PAGES

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; ...

    2015-09-25

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

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. 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

  10. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2013-03-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This

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

    SciTech Connect

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

    2009-07-10

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

  12. A review of atmospheric aerosol measurements

    NASA Astrophysics Data System (ADS)

    McMurry, Peter H.

    Recent developments in atmospheric aerosol measurements are reviewed. The topics included complement those covered in the recent review by Chow (JAWMA 45: 320-382, 1995) which focuses on regulatory compliance measurements and filter measurements of particulate composition. This review focuses on measurements of aerosol integral properties (total number concentration, CCN concentration, optical coefficients, etc.), aerosol physical chemical properties (density, refractive index, equilibrium water content, etc.), measurements of aerosol size distributions, and measurements of size-resolved aerosol composition. Such measurements play an essential role in studies of secondary aerosol formation by atmospheric chemical transformations and enable one to quantify the contributions of various species to effects including light scattering/absorption, health effects, dry deposition, etc. Aerosol measurement evolved from an art to a science in the 1970s following the development of instrumentation to generate monodisperse calibration aerosols of known size, composition, and concentration. While such calibration tools permit precise assessments of instrument responses to known laboratory-generated aerosols, unquantifiable uncertainties remain even when carefully calibrated instruments are used for atmospheric measurements. This is because instrument responses typically depend on aerosol properties including composition, shape, density, etc., which, for atmospheric aerosols, may vary from particle-to-particle and are often unknown. More effort needs to be made to quantify measurement accuracies that can be achieved for realistic atmospheric sampling scenarios. The measurement of organic species in atmospheric particles requires substantial development. Atmospheric aerosols typically include hundreds of organic compounds, and only a small fraction (˜10%) of these can be identified by state-of-the-art analytical methodologies. Even the measurement of the total particulate organic

  13. 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

  14. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2012-08-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and cloud susceptibilities, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of -1.17 W m-2

  15. 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.

  16. Thermodynamic characterization of Mexico City aerosol during MILAGRO 2006

    NASA Astrophysics Data System (ADS)

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

    2007-06-01

    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. PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. Semi-volatile partitioning equilibrates on a timescale between 6 and 20 min. When the aerosol sulfate-to-nitrate molar ratio is less than 1, 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 are required to accurately predict the partitioning and phase state of aerosols.

  17. 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.

  18. Analysis of Ambient Aerosol Measurements During PROPHET 2001

    NASA Astrophysics Data System (ADS)

    Delia, A. E.; Garland, R.; Toohey, D. W.; Worsnop, D. R.; Allen, J. O.; Carroll, M. A.; Fortner, E.; Hengel, S.; Lilly, M.; Moody, J.; Huey, G.; Tanner, D.

    2002-12-01

    Aerosol size and composition were measured using an aerosol mass spectrometer, developed by Aerodyne Research, Inc., during PROPHET 2001 (Program for Research on Oxidants: PHotochemistry, Emissions and Transport). Our purpose in this study was to characterize chemical composition and size of ambient aerosols, investigate the effects of transport, and study aerosol microphysics. The site is located in a remote forested area of northern Michigan at the University of Michigan Biological Station, far from any large urban areas and surrounded primarily by deciduous forests. The aerosols at this site can be cataloged into four classes. The two principal classes are distinguished by meteorological conditions. Clean, northerly airflow produced low aerosol mass loadings dominated by organic species. More polluted southerly airflow brought higher aerosol mass loadings dominated by sulfate with an organic contribution. Under both of these conditions, aerosol existed almost entirely in the accumulation size mode of 300-600 nm. In addition to these principal aerosol types, small particle growth was observed on several occasions. It appears that these events occurred primarily during periods of low aerosol mass loading (i.e., northerly airflow) when the low aerosol number provided an opportunity for new particle formation and rapid growth. On at least one occasion, it appears that a large plume of sulfur dioxide that was converted to sulfuric acid near the site may be responsible for new particle formation. The fourth type of aerosol consisted of short events dominated by organic species, apparently diesel exhaust caused by local truck traffic. In addition to the overall aerosol characterization, comparisons with other measurements that affected the aerosol composition or characterized the air masses will be presented and the implications of these results for regional transport of aerosols will be discussed.

  19. Light Absorbing Aerosols in Mexico City

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  20. 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.

  1. Asian Aerosols: A Geophysical Fluid Dynamics Laboratory general circulation model sensitivity study of model response to aerosol optical depth and aerosol absorption

    NASA Astrophysics Data System (ADS)

    Randles, C. A.; Ramaswamy, V.

    2007-12-01

    Atmospheric absorption by black carbon (BC) aerosol heats the atmosphere while simultaneously cooling the surface and reducing latent and sensible heat fluxes from the land. Recent studies have shown that absorbing BC aerosol can have a large impact on regional climates, including modification of the hydrological cycle. However, significant uncertainties remain with regards to (a) the total amount of all aerosol species and (b) the amount of aerosol absorption. Here we present a GCM sensitivity study focusing on the influences due to total aerosol amount and aerosol absorption in the south and east Asian regions. Six experiments are conducted to test the equilibrium response of the GFDL AM2 GCM (under conditions of prescribed, observed sea surface temperatures) to (i) changes in aerosol absorption caused by changes in BC aerosol amount, and (ii) aerosol extinction optical depth increases corresponding to the year 1990 relative to a control case of 1950. In order to systematically explore the uncertainties in aerosol loading and absorption, the sensitivity experiments are classified into four regimes: low extinction optical depth, low absorption; low extinction optical depth, high absorption; high extinction optical depth, low absorption; and high extinction optical depth, high absorption. Changes in surface temperature and changes in the hydrological cycle are generally insignificant when lower aerosol extinction optical depths are considered. For higher extinction optical depths, the change in the modeled regional circulation relative to the control circulation over south and east Asia is affected by the amount of aerosol absorption and contrasts sharply to the regional circulation change associated with increasing only scattering aerosols. When increasing absorbing aerosols over the region, low-level convergence and increases in vertical velocity overcome the stabilizing effects of the absorbing aerosol and enhance the monsoonal circulation and precipitation rate

  2. 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

  3. Change in global aerosol composition since preindustrial times

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Krol, M.; Dentener, F. J.; Balkanski, Y.; Lathière, J.; Metzger, S.; Hauglustaine, D. A.; Kanakidou, M.

    2006-06-01

    To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. This is the first 3-d modeling study that focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3-, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34-42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has

  4. Change in global aerosol composition since preindustrial times

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Krol, M.; Dentener, F. J.; Balkanski, Y.; Lathière, J.; Metzger, S.; Hauglustaine, D. A.; Kanakidou, M.

    2006-11-01

    To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3aerosol loading is dampened by a 34-42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased

  5. Differentiation of hydrophobic from hydrophilic submicrometer aerosol particles

    SciTech Connect

    Juozaitis, A.; Ulevicius, V.; Girgzdys, A. ); Willeke, K. )

    1993-02-01

    A method has been developed that differentiates hydrophobic from hydrophilic submicrometer aerosol particles in air environments containing polydisperse aerosols composed of different chemical species. First, a narrow particle size range is extracted from the polydisperse aerosol by an electrostatic aerosol classifier. Then the monodisperse aerosols of different origins are exposed to preselected supersaturation levels and are size-classified again by a second electrostatic classifier. Hydrophobic aerosol particles pass through the second classifier when its size window matches that of the first classifier. Hydrophilic aerosol particles grow to a larger size and are removed by the second classifier. The method has been applied in the field by measuring the fraction of hydrophobic atmospheric particles in a suburb of Vilnius, Lithuania, during a period of high emission of hydrophobic soot particles from residential coal and industrial oil burning in winter. 33 refs., 4 figs.

  6. Atmospheric responses to stratospheric aerosol geoengineering

    NASA Astrophysics Data System (ADS)

    Ferraro, Angus; Highwood, Eleanor; Charlton-Perez, Andrew

    2013-04-01

    Stratospheric aerosol geoengineering, also called solar radiation management (SRM), involves the injection of aerosol into the stratosphere to increase the planetary albedo. It has been conceieved as a policy option in response to human-induced global warming. It is well-established from modelling studies and observations following volcanic eruptions that stratospheric sulphate aerosols cause global cooling. Some aspects of the climate response, especially those involving large-scale dynamical changes, are more uncertain. This work attempts to identify the physical mechanisms operating in the climate response to stratospheric aerosol geoengineering using idealised model experiments. The radiative forcing produced by the aerosol depends on its type (species) and size. Aerosols absorb terrestrial and solar radiation, which drives stratospheric temperature change. The stratospheric temperature change also depends on aerosol type and size. We calculate the stratospheric temperature change due to geoengineering with sulphate, titania, limestone and soot in a fixed-dynamical-heating radiative model. Sulphate produces tropical heating of up to ~6 K. Titania produces much less heating, whereas soot produces much more. Most aerosols increase the meridional temperature gradient in the lower stratosphere which, by thermal wind balance, would be expected to intensify the zonal winds in the polar vortex. An intermediate-complexity general circulation model is used to investigate the dynamical response to geoengineering aerosols. Atmospheric carbon dioxide concentrations are quadrupled. The carbon dioxide forcing is then balanced using stratospheric sulphate aerosol. We assess dynamical changes in the stratosphere, for example, the frequency of stratospheric sudden warmings and the strength of the Brewer-Dobson overturning circulation. We also assess changes in the strength and position of the tropospheric jets. We compare results for sulphate with those for titania.

  7. 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

  8. 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...

  9. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  10. 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.

  11. On the implications of aerosol liquid water and phase separation for organic aerosol mass

    NASA Astrophysics Data System (ADS)

    Pye, Havala O. T.; Murphy, Benjamin N.; Xu, Lu; Ng, Nga L.; Carlton, Annmarie G.; Guo, Hongyu; Weber, Rodney; Vasilakos, Petros; Wyat Appel, K.; Hapsari Budisulistiorini, Sri; Surratt, Jason D.; Nenes, Athanasios; Hu, Weiwei; Jimenez, Jose L.; Isaacman-VanWertz, Gabriel; Misztal, Pawel K.; Goldstein, Allen H.

    2017-01-01

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM / OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM / OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM / OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model-measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. Aerosol Radiative Forcing and Weather Forecasts in the ECMWF Model

    NASA Astrophysics Data System (ADS)

    Bozzo, A.; Benedetti, A.; Rodwell, M. J.; Bechtold, P.; Remy, S.

    2015-12-01

    Aerosols play an important role in the energy balance of the Earth system via direct scattering and absorpiton of short-wave and long-wave radiation and indirect interaction with clouds. Diabatic heating or cooling by aerosols can also modify the vertical stability of the atmosphere and influence weather pattern with potential impact on the skill of global weather prediction models. The Copernicus Atmosphere Monitoring Service (CAMS) provides operational daily analysis and forecast of aerosol optical depth (AOD) for five aerosol species using a prognostic model which is part of the Integrated Forecasting System of the European Centre for Medium-Range Weather Forecasts (ECMWF-IFS). The aerosol component was developed during the research project Monitoring Atmospheric Composition and Climate (MACC). Aerosols can have a large impact on the weather forecasts in case of large aerosol concentrations as found during dust storms or strong pollution events. However, due to its computational burden, prognostic aerosols are not yet feasible in the ECMWF operational weather forecasts, and monthly-mean climatological fields are used instead. We revised the aerosol climatology used in the operational ECMWF IFS with one derived from the MACC reanalysis. We analyse the impact of changes in the aerosol radiative effect on the mean model climate and in medium-range weather forecasts, also in comparison with prognostic aerosol fields. The new climatology differs from the previous one by Tegen et al 1997, both in the spatial distribution of the total AOD and the optical properties of each aerosol species. The radiative impact of these changes affects the model mean bias at various spatial and temporal scales. On one hand we report small impacts on measures of large-scale forecast skill but on the other hand details of the regional distribution of aerosol concentration have a large local impact. This is the case for the northern Indian Ocean where the radiative impact of the mineral

  17. Aerosol algorithm evaluation within aerosol-CCI

    NASA Astrophysics Data System (ADS)

    Kinne, Stefan; Schulz, Michael; Griesfeller, Jan

    Properties of aerosol retrievals from space are difficult. Even data from dedicated satellite sensors face contaminations which limit the accuracy of aerosol retrieval products. Issues are the identification of complete cloud-free scenes, the need to assume aerosol compositional features in an underdetermined solution space and the requirement to characterize the background at high accuracy. Usually the development of aerosol is a slow process, requiring continuous feedback from evaluations. To demonstrate maturity, these evaluations need to cover different regions and seasons and many different aerosol properties, because aerosol composition is quite diverse and highly variable in space and time, as atmospheric aerosol lifetimes are only a few days. Three years ago the ESA Climate Change Initiative started to support aerosol retrieval efforts in order to develop aerosol retrieval products for the climate community from underutilized ESA satellite sensors. The initial focus was on retrievals of AOD (a measure for the atmospheric column amount) and of Angstrom (a proxy for aerosol size) from the ATSR and MERIS sensors on ENVISAT. The goal was to offer retrieval products that are comparable or better in accuracy than commonly used NASA products of MODIS or MISR. Fortunately, accurate reference data of ground based sun-/sky-photometry networks exist. Thus, retrieval assessments could and were conducted independently by different evaluation groups. Here, results of these evaluations for the year 2008 are summarized. The capability of these newly developed retrievals is analyzed and quantified in scores. These scores allowed a ranking of competing efforts and also allow skill comparisons of these new retrievals against existing and commonly used retrievals.

  18. Aerosol optical depths and their contributing sources in Taiwan

    NASA Astrophysics Data System (ADS)

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

    2017-01-01

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

  19. 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...

  20. Global modeling of nitrate and ammonium aerosols using EQSAM3

    NASA Astrophysics Data System (ADS)

    Xu, L.; Penner, J. E.

    2009-12-01

    Atmospheric aerosols, particles suspending in air, are important as they affect human health, air quality, and visibility as well as climate. Sulfate, nitrate, ammonium, chloride and sodium are among the most important inorganic aerosol species in the atmosphere. These compounds are hygroscopic and absorb water under almost all ambient environmental conditions. The uptake of water alters the aerosol size, and causes water to become the constituent with the largest atmospheric aerosol mass, especially when the aerosols grow into fog, haze or clouds. Furthermore, several global model studies have demonstrated that rapid increases in nitrogen emissions could produce enough nitrate in aerosols to offset the expected decline in sulfate forcing by 2100 for the extreme IPCC A2 scenario (Bauer et al., 2007). Although nitrate and ammonium were identified as significant anthropogenic sources of aerosols by a number of modeling studies, most global aerosol models still exclude ammonium-nitrate when the direct aerosol forcing is studied. In this study, the computationally efficient equilibrium model, EQSAM3, is incorporated into the UMICH-IMPACT-nitrate model using the hybrid dynamical solution method (Feng and Penner, 2007). The partitioning of nitrate and ammonium along with the corresponding water uptake is evaluated by comparing the model to the EQUISOLVE II method used in Feng and Penner (2007). The model is also evaluated by comparison with the AERONET data base and satellite-based aerosol optical depths.

  1. Phase transition behaviour of sodium oleate aerosol particles

    NASA Astrophysics Data System (ADS)

    Nájera, Juan J.

    Field measurements have shown that organic surfactants are significant components of atmospheric aerosols. While fatty acids, among other surfactants, are prevalent in the atmosphere, the influence of these species on the chemical and physical properties of atmospheric aerosols remains not fully characterized. In order to assess the phase in which particles may exist, a detailed study of the deliquescence of a model surfactant aerosol has been carried out. Sodium oleate was chosen as a surfactant proxy relevant in atmospheric aerosol. Sodium oleate micelle aerosol particles were generated nebulizing a sodium oleate aqueous solution. In this study, the water uptake and phase transition of sodium oleate aerosol particles have been studied in a room temperature aerosol flow tube system (AFT) using Fourier transform infrared (FTIR) spectroscopy. Aerosol morphology and elemental composition were also analysed using scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDX) techniques. The particles are homogeneously distributed as ellipsoidal-shape aggregates of micelles particles with an average size of ˜1.1 μm. The deliquescence by the sodium oleate aerosol particles was monitored by infrared extinction spectroscopy, where the dried aerosol particles were exposed to increasing relative humidity as they passed through the AFT. Observations of the infrared absorption features of condensed phase liquid water enable to determine the sodium oleate deliquescence phase transition at 88±2%.

  2. Anthropogenic Aerosols in Asia, Radiative Forcing, and Climate Change

    NASA Astrophysics Data System (ADS)

    Ramaswamy, V.; Bollasina, M. A.; Ming, Y.; Ocko, I.; Persad, G.

    2014-12-01

    Aerosols arising as a result of human-induced emissions in Asia form a key 'driver' in causing pollution and in the forcing of anthropogenic climate change. The manner of the forced climate change is sensitive to the scattering and absorption properties of the aerosols and the aerosol-cloud microphysical interactions. Using the NOAA/ GFDL global climate models and observations from multiple platforms, we investigate the radiative perturbations due to the 20th Century sulfate and carbonaceous aerosol emissions and the resultant impacts on surface temperature, tropical precipitation, Indian monsoon, hemispheric circulation, and atmospheric and oceanic heat transports. The influence of the aerosol species has many contrasts with that due to the anthropogenic well-mixed greenhouse gas emissions e.g., the asymmetry in the hemispheric climate response, but is subject to larger uncertainties. The aerosol forcing expected in the future indicates a significant control on the 21st Century anthropogenic climate change in Asia.

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

    PubMed

    Zimmer, Anthony T

    2002-10-01

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

  4. Introducing GMXe: A new global aerosol dynamics and thermodynamics model for climate and air quality studies

    NASA Astrophysics Data System (ADS)

    Pringle, K.; Metzger, S.; Tost, H.; Steil, B.; Lelieveld, J.

    2009-04-01

    The treatment of aerosols in global atmospheric models has advanced significantly in the past decade, but the global aerosol distribution is very complex and simplifications must be made in order to treat aerosols in global models. One common simplification is in the treatment of the partitioning of semi-volatile species (e.g. NH3, HNO3 and H2O) between the gas and the aerosol phases, which is often neglected in models or treated in a simplified manner. The treatment of partitioning is, however, important as it controls the aerosol composition (including the aerosol water concentration) as well as affecting the concentration of both aerosol and gas phase pollutants. This paper introduces the newly developed GMXe aerosol model, which has been developed to investigate gas / aerosol partitioning on a global scale. The model (implemented within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model) combines an extended version of an established aerosol microphysics model (the M7, Stier et al ACP 2005) with a thermodynamic equilibrium model (EQSAM3, Metzger et al ACP 2008). The resulting model is capable of calculating gas / aerosol partitioning with relatively little additional computational overhead. In this paper we give an overview of the modelling approach used and show various model inter-comparisons, including a detailed comparison of the results of the GMXe and M7 models. We show the effect of including additional aerosol components - such as nitrate aerosol - on the global aerosol distribution and on the behaviour of other aerosol species (e.g. sulphate). The water uptake behaviour of the aerosol is examined, a factor that is important for the aerosol lifetime and also for the aerosol radiative forcing. We examine our results in the context of future emissions scenarios and air quality standards.

  5. 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.

  6. 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

  7. Thermodynamic characterization of Mexico City aerosol during MILAGRO 2006

    NASA Astrophysics Data System (ADS)

    Fountoukis, C.; Nenes, A.; Sullivan, A.; Weber, R.; van Reken, T.; Fischer, M.; Matías, E.; Moya, M.; Farmer, D.; Cohen, R. C.

    2009-03-01

    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. PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. For particle sizes up to 1μm diameter, semi-volatile partitioning requires 15-30 min to equilibrate; longer time is typically required during the night and early morning hours. Aerosol and gas-phase speciation always exhibits substantial temporal variability, so that aerosol composition measurements (bulk or size-resolved) obtained over large integration periods are not reflective of its true state. 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.

  8. 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%.

  9. 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%.

  10. Operational aerosol and dust storm forecasting

    NASA Astrophysics Data System (ADS)

    Westphal, D. L.; Curtis, C. A.; Liu, M.; Walker, A. L.

    2009-03-01

    The U. S. Navy now conducts operational forecasting of aerosols and dust storms on global and regional scales. The Navy Aerosol Analysis and Prediction System (NAAPS) is run four times per day and produces 6-day forecasts of sulfate, smoke, dust and sea salt aerosol concentrations and visibility for the entire globe. The Coupled Ocean Atmosphere Mesoscale Prediction System (COAMPS®) is run twice daily for Southwest Asia and produces 3-day forecasts of dust, smoke, and visibility. The graphical output from these models is available on the Internet (www.nrlmry.navy.mil/aerosol/). The aerosol optical properties are calculated for each specie for each forecast output time and used for sea surface temperature (SST) retrieval corrections, regional electro-optical (EO) propagation assessments, and the development of satellite algorithms. NAAPS daily aerosol optical depth (AOD) values are compared with the Advanced Very High Resolution Radiometer (AVHRR) and Moderate Resolution Imaging Spectroradiometer (MODIS) AOD values. Visibility forecasts are compared quantitatively with surface synoptic reports.

  11. 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

  12. Overview of Aerosol Distribution

    NASA Technical Reports Server (NTRS)

    Kaufman, Yoram

    2005-01-01

    Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with clouds and precipitation is still lacking despite decades of research. Understanding the global aerosol system is fundamental for progress in climate change and hydrological cycle research. While a single instrument was used to demonstrate 50 years ago that the global CO2 levels are rising, posing threat of global warming, we need an array of satellites and field measurements coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week) and variable chemical composition. A new generation of satellites provides exciting opportunities to measure the global distribution of aerosols, distinguishing natural from anthropogenic aerosol and measuring their interaction with clouds and climate. I shall discuss these topics and application of the data to air quality monitoring.

  13. 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.

  14. 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.

  15. Aerosol, radiation, and climate

    NASA Technical Reports Server (NTRS)

    Pollack, J. B.

    1983-01-01

    Airborne, spaceborne, and ground-based measurements are used to study the radiative and climatic effects of aerosols. The data, which are modelled with a hierarchy of radiation and climate models, and their implications are summarized. Consideration is given to volcanic aerosols, polar stratospheric clouds, and the Arctic haze. It is shown that several types of aerosols (volcanic particles and the Arctic haze) cause significant alterations to the radiation budget of the regions where they are located.

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. On the implications of aerosol liquid water and phase ...

    EPA Pesticide Factsheets

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were hig

  2. 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.

  3. 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

  4. Global observations of cloud-sensitive aerosol loadings in low-level marine clouds

    NASA Astrophysics Data System (ADS)

    Andersen, H.; Cermak, J.; Fuchs, J.; Schwarz, K.

    2016-11-01

    Aerosol-cloud interaction is a key component of the Earth's radiative budget and hydrological cycle, but many facets of its mechanisms are not yet fully understood. In this study, global satellite-derived aerosol and cloud products are used to identify at what aerosol loading cloud droplet size shows the greatest sensitivity to changes in aerosol loading (ACSmax). While, on average, cloud droplet size is most sensitive at relatively low aerosol loadings, distinct spatial and temporal patterns exist. Possible determinants for these are identified with reanalysis data. The magnitude of ACSmax is found to be constrained by the total columnar water vapor. Seasonal patterns of water vapor are reflected in the seasonal patterns of ACSmax. Also, situations with enhanced turbulent mixing are connected to higher ACSmax, possibly due to intensified aerosol activation. Of the analyzed aerosol species, dust seems to impact ACSmax the most, as dust particles increase the retrieved aerosol loading without substantially increasing the concentration of cloud condensation nuclei.

  5. Technical Note: Simulation of detailed aerosol chemistry on the global scale using MECCA-AERO

    NASA Astrophysics Data System (ADS)

    Kerkweg, A.; Sander, R.; Tost, H.; Jöckel, P.; Lelieveld, J.

    2007-06-01

    We present the MESSy submodel MECCA-AERO, which simulates both aerosol and gas phase chemistry within one comprehensive mechanism. Including the aerosol phase into the chemistry mechanism increases the stiffness of the resulting set of differential equations. The numerical aspects of the approach followed in MECCA-AERO are presented. MECCA-AERO requires input of an aerosol dynamical/microphysical model to provide the aerosol size and particle number information of the modes/bins for which the chemistry is explicitly calculated. Additional precautions are required to avoid the double counting of processes, especially for sulphate in the aerosol dynamical and the chemistry model. This coupling is explained in detail. To illustrate the capabilities of the new aerosol submodel, examples for species usually treated in aerosol dynamical models are shown. The aerosol chemistry as provided by MECCA-AERO is very sumptuous and not readily applicable for long-term simulations, though it provides a reference to evaluate simplified approaches.

  6. Technical Note: simulation of detailed aerosol chemistry on the global scale using MECCA-AERO

    NASA Astrophysics Data System (ADS)

    Kerkweg, A.; Sander, R.; Tost, H.; Jöckel, P.; Lelieveld, J.

    2007-03-01

    We present the MESSy submodel MECCA-AERO, which simulates both aerosol and gas phase chemistry with the same mechanism. Including the aerosol phase into the chemistry mechanism increases the stiffness of the resulting set of differential equations. The numerical aspects of the approach followed in MECCA-AERO are presented. MECCA-AERO requires input of an aerosol dynamical/microphysical model to provide the aerosol size and particle number information of the modes/bins for which the chemistry is explicitly calculated. Additional precautions are required to avoid the double counting of processes, especially for sulphate in the aerosol dynamical and the chemistry model. This coupling is explained in detail. To illustrate the capabilities of the new aerosol submodel, examples for species usually treated in aerosol dynamical models are shown. The aerosol chemistry as provided by MECCA-AERO is very sumptuous and not readily applicable for long-term simulations, though it provides a reference to evaluate simplified approaches.

  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. 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.

  9. 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, ...

  10. 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.

  11. Ganges valley aerosol experiment.

    SciTech Connect

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

    2011-08-01

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

  12. 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

  13. 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.

  14. 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.

  15. 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.

  16. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

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

    2003-02-01

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

  17. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

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

    2002-02-01

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

  18. 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.

  19. 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.

  20. ModelE2-TOMAS development and evaluation using aerosol optical depths, mass and number concentrations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2014-09-01

    The TwO-Moment Aerosol Sectional microphysics model (TOMAS) has been integrated into the state-of-the-art general circulation model, GISS ModelE2. TOMAS has the flexibility to select a size resolution as well as the lower size cutoff. A computationally efficient version of TOMAS is used here, which has 15 size bins covering 3 nm to 10 μm aerosol dry diameter. For each bin, it simulates the total aerosol number concentration and mass concentrations of sulphate, pure elementary carbon (hydrophobic), mixed elemental carbon (hydrophilic), hydrophobic organic matter, hydrophilic organic matter, sea salt, mineral dust, ammonium, and aerosol-associated water. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the TOMAS model is compared to the default aerosol model in ModelE2, which is a bulk aerosol model. Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of sulphur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as the bulk aerosol model) cannot capture the observed vertical distribution of sulphur dioxide over the Pacific Ocean possibly due to overly strong convective transport. The TOMAS model successfully captures observed aerosol number concentrations and cloud condensation nuclei concentrations. Anthropogenic aerosol burdens in the bulk aerosol model running in the same host model as TOMAS (ModelE2) differ by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. Larger differences are found for naturally

  1. Airborne studies of aerosol emissions from savanna fires in southern Africa: 2. Aerosol chemical composition

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Andreae, T. W.; Annegarn, H.; Beer, J.; Cachier, H.; Le Canut, P.; Elbert, W.; Maenhaut, W.; Salma, I.; Wienhold, F. G.; Zenker, T.

    1998-12-01

    We investigated smoke emissions from fires in savanna, forest, and agricultural ecosystems by airborne sampling of plumes close to prescribed burns and incidental fires in southern Africa. Aerosol samples were collected on glass fiber filters and on stacked filter units, consisting of a Nuclepore prefilter for particles larger than ˜1-2 μm and a Teflon second filter stage for the submicron fraction. The samples were analyzed for soluble ionic components, organic carbon, and black carbon. Onboard the research aircraft, particle number and volume distributions as a function of size were determined with a laser-optical particle counter and the black carbon content of the aerosol with an aethalometer. We determined the emission ratios (relative to CO2 and CO) and emission factors (relative to the amount of biomass burnt) for the various aerosol constituents. The smoke aerosols were rich in organic and black carbon, the latter representing 10-30% of the aerosol mass. K+ and NH4+ were the dominant cationic species in the smoke of most fires, while Cl- and SO42- were the most important anions. The aerosols were unusually rich in Cl-, probably due to the high Cl content of the semiarid vegetation. Comparison of the element budget of the fuel before and after the fires shows that the fraction of the elements released during combustion is highly variable between elements. In the case of the halogen elements, almost the entire amount released during the fire is present in the aerosol phase, while in the case of C, N, and S, only a small proportion ends up as particulate matter. This suggests that the latter elements are present predominantly as gaseous species in the fresh fire plumes studied here.

  2. MATRIX-VBS (v1.0): implementing an evolving organic aerosol volatility in an aerosol microphysics model

    NASA Astrophysics Data System (ADS)

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

    2017-02-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  3. MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

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

    2017-01-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  4. 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.

  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. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    SciTech Connect

    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 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

  7. 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

  8. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGES

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-03-02

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

  9. 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

  10. Deposition and retention of radioactive aerosols on desert vegetation

    SciTech Connect

    Millard, G.E.

    1986-01-01

    Deposition velocities and retention times were obtained for submicron aerosols of /sup 134/Cs and /sup 141/Ce on a shrub species (Artemisia tridentata) and a grass (Elymus elimoides) in a natural desert environment. Submicron aerosols of these two nuclides were artificially generated and released over a sagebrush community in southeast Idaho during each of three seasons: spring, summer and winter, to determine the effects of weathering and plant development on aerosol deposition and retention. Information on friction velocities, roughness lengths, and particle size was also obtained.

  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. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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

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

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

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

  20. 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.

  1. 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.

  2. 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.

  3. 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

  4. Large-Scale Aerosol Modeling and Analysis

    DTIC Science & Technology

    2008-09-30

    aerosol species up to six days in advance anywhere on the globe. NAAPS and COAMPS are particularly useful for forecasts of dust storms in areas...impact cloud processes globally. With increasing dust storms due to climate change and land use changes in desert regions, the impact of the...bacteria in large-scale dust storms is expected to significantly impact warm ice cloud formation, human health, and ecosystems globally. In Niemi et al

  5. 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

  6. 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

  7. 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.

  8. 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.

  9. Palaeoclimate: Aerosols shift lake ecosystem

    NASA Astrophysics Data System (ADS)

    Dowsett, Harry J.

    2017-02-01

    Anthropogenic aerosols over the Chinese Loess Plateau have diminished monsoon precipitation and concomitant soil erosion that plagues the region. Now, a reconstruction documents the differences between historical warming events and the present, highlighting the paradoxical implications of decreasing atmospheric aerosols.

  10. 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.

  11. Generation of aerosolized drugs.

    PubMed

    Wolff, R K; Niven, R W

    1994-01-01

    The expanding use of inhalation therapy has placed demands on current aerosol generation systems that are difficult to meet with current inhalers. The desire to deliver novel drug entities such as proteins and peptides, as well as complex formulations including liposomes and microspheres, requires delivery systems of improved efficiency that will target the lung in a reproducible manner. These efforts have also been spurred by the phase out of chlorofluorocarbons (CFCs) and this has included a directed search for alternative propellants. Consequently, a variety of new aerosol devices and methods of generating aerosols are being studied. This includes the use of freon replacement propellants, dry powder generation systems, aqueous unit spray systems and microprocessor controlled technologies. Each approach has advantages and disadvantages depending upon each principle of action and set of design variables. In addition, specific drugs may be better suited for one type of inhaler device vs. another. The extent to which aerosol generation systems achieve their goals is discussed together with a summary of selected papers presented at the recent International Congress of Aerosols in Medicine.

  12. 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).

  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. 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.

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

    SciTech Connect

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

    2015-09-25

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

  17. 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.

  18. Chemical aerosol Raman detector

    NASA Astrophysics Data System (ADS)

    Aggarwal, R. L.; Farrar, L. W.; Di Cecca, S.; Amin, M.; Perkins, B. G.; Clark, M. L.; Jeys, T. H.; Sickenberger, D. W.; D'Amico, F. M.; Emmons, E. D.; Christesen, S. D.; Kreis, R. J.; Kilper, G. K.

    2017-03-01

    A sensitive chemical aerosol Raman detector (CARD) has been developed for the trace detection and identification of chemical particles in the ambient atmosphere. CARD includes an improved aerosol concentrator with a concentration factor of about 40 and a CCD camera for improved detection sensitivity. Aerosolized isovanillin, which is relatively safe, has been used to characterize the performance of the CARD. The limit of detection (SNR = 10) for isovanillin in 15 s has been determined to be 1.6 pg/cm3, which corresponds to 6.3 × 109 molecules/cm3 or 0.26 ppb. While less sensitive, CARD can also detect gases. This paper provides a more detailed description of the CARD hardware and detection algorithm than has previously been published.

  19. 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

  20. 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.

  1. Dry season aerosol iron solubility in tropical northern Australia

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  2. 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.

  3. 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.

  4. Stratospheric Aerosol Measurements

    NASA Technical Reports Server (NTRS)

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

    1998-01-01

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

  5. Highly stable aerosol generator

    SciTech Connect

    DeFord, Henry S.; Clark, Mark L.

    1981-01-01

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

  6. 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.

  7. 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

  8. 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.

  9. 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 ...

  10. 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

  11. 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.

  12. 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

  13. 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

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

    SciTech Connect

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

    1990-10-01

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

  15. 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.

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

    NASA Astrophysics Data System (ADS)

    Rao, R. R.

    2015-12-01

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

  17. 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.

  18. Aerosol contributions to speleothem geochemistry

    NASA Astrophysics Data System (ADS)

    Dredge, J. A.; Fairchild, I. J.; Harrison, R.; Woodhead, J. D.; Hellstrom, J.

    2011-12-01

    The term "aerosols" encompasses the suspension of both fine solid or liquid particles within a gaseous medium. Aerosols become suspended into the earth's atmosphere through a multitude of processes both natural and anthropogenic. Atmospheric aerosols enter cave networks as a result of cave ventilation processes and are either deposited, or cycled and removed from the system. Speleothem offer a multiproxy palaeoclimate resource; many of the available proxies have been extensively investigated and utilised for palaeoclimatic reconstructions in a range of studies. The potential contribution of aerosols to speleothem chemistry and their applicability for palaeoenvironmental reconstructions remains untested and the extent of their value as an addition to palaeoclimate sciences unknown. Aerosols through incorporation into speleothem may provide a novel palaeoenvironmental resource. The aerosol component of interest is that which is transported into the cave atmosphere and deposited and are available for incorporation into precipitated calcite. Aerosol deposition and therefore distribution in the cave has shown to be a complex function of ventilation and changing environmental factors. Through detailed monitoring aerosols have been detected, identified, characterised and quantified to determine their prominence in the cave system. Investigations are on a case study basis, searching for suitable aerosol proxies of environmentally significant emission processes. Case studies include: Palaeofires at Yarrangobilly Caves, Australia; anthropogenic emissions at St Michaels Cave, Gibraltar and Cheddar gorge, UK; and drip water aerosol production and geochemical addition in Obir cave, Austria. Monitoring has allowed for the temporal and spatial determination of aerosols in karst networks. Speleothem samples will be analysed in combination with in-situ monitoring to determine incorporation factors and record preservation. By understanding how aerosols are transmitted within the

  19. 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.

  20. Secondary organic aerosol formation from reaction of tertiary amines with nitrate radical

    NASA Astrophysics Data System (ADS)

    Erupe, M. E.; Price, D. J.; Silva, P. J.; Malloy, Q. G. J.; Qi, L.; Warren, B.; Cocker, D. R., III

    2008-09-01

    Secondary organic aerosol formation from the reaction of tertiary amines with nitrate radical was investigated in an indoor environmental chamber. Particle chemistry was monitored using a high resolution aerosol mass spectrometer while gas-phase species were detected using a proton transfer reaction mass spectrometer. Trimethylamine, triethylamine and tributylamine were studied. Results indicate that tributylamine forms the most aerosol mass followed by trimethylamine and triethylamine respectively. Spectra from the aerosol mass spectrometer indicate the formation of complex non-salt aerosol products. We propose a reaction mechanism that proceeds via abstraction of a proton by nitrate radical followed by RO2 chemistry. Rearrangement of the aminyl alkoxy radical through hydrogen shift leads to the formation of hydroxylated amides, which explain most of the higher mass ions in the mass spectra. These experiments show that oxidation of tertiary amines by nitrate radical may be an important night-time source of secondary organic aerosol.

  1. 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

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  3. American Association for Aerosol Research (AAAR) `95

    SciTech Connect

    1995-12-31

    The Fourteenth annual meeting of the American Association for Aerosol Research was held October 9-13, 1995 at Westin William Penn Hotel in Pittsburgh, PA. This volume contains the abstracts of the papers and poster sessions presented at this meeting, grouped by the session in which they were presented as follows: Radiation Effects; Aerosol Deposition; Collision Simulations and Microphysical Behavior; Filtration Theory and Measurements; Materials Synthesis; Radioactive and Nuclear Aerosols; Aerosol Formation, Thermodynamic Properties, and Behavior; Particle Contamination Issues in the Computer Industry; Pharmaceutical Aerosol Technology; Modeling Global/Regional Aerosols; Visibility; Respiratory Deposition; Biomass and Biogenic Aerosols; Aerosol Dynamics; Atmospheric Aerosols.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  5. 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.

  6. 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).

  7. Characteristics of microbial aerosols released from chicken and swine feces.

    PubMed

    Chien, Yeh-Chung; Chen, Chiou-Jong; Lin, Tzu-Hsien; Chen, Shih-Hsun; Chien, Yu-Ching

    2011-08-01

    Bioaerosols generated during livestock and poultry production are significant occupational hazards. This study investigates the characteristics of bioaerosols released from animal feces. Fresh feces from pigs and chickens were obtained and tested in a controlled-environment facility. Airborne viable (culturable) bacteria and fungi were sampled hourly for 48 hr. The predominant species were identified via polymerase chain reaction analysis. The number of bacterial colonies released from chicken feces increased gradually, peaked at approximately 20 hr, and remained relatively constant to test end; however, the bacterial colonies released from swine feces did not increase significantly. The chicken feces released significantly (P < 0.05) more bacterial aerosols than swine feces over 40 hr, by approximately 1 order of magnitude. However, the difference in total fungal aerosols released from the two feces types was relatively small (30-40%) and insignificant (P > 0.05). Aerosols sized between approximately 0.65 and 1.1 microm were predominant for bacteria, whereas aerosols sized between approximately 2.1 and 3.3 microm prevailed for fungi. Genera Stenotrophomonas were the predominant bacterial aerosols, whereas Cladosporium and Acremonium accounted for the greatest amounts of fungi from chicken and swine feces, respectively. More than 1000 culturable bacterial colonies can be released from 1 g of chicken feces per hour, and approximately 80% of these bioaerosols are respirable. Most bacterial aerosols released from swine and chicken feces were opportunistic human pathogens; thus, the significance of their presence warrants further investigations.

  8. 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

  9. Charicteristics of Aerosol indices distribution followed by Aerosol types

    NASA Astrophysics Data System (ADS)

    Park, S.; Kim, J.; Lee, J.; Kim, M.; Lee, S.; Song, C.

    2010-12-01

    Transboundary transport of aerosol has been a hot issue in East Asia and with various aerosol types from different source region. To detect signals from aerosols, OMI provides aerosol indices. Aerosol Indices (AI) represent the change of spectral contrast between two wavelengths and these indices are derived in UV and Visible regions. These indices also can get not only in ocean but also in land region so that AI is good to observe the source region and transport of aerosols. In UV region, AI (UV-AI) can classify the absorbing and non-absorbing aerosols (Torres et al., 1998) so that this value is frequently used for dust detection. Additionally, visible AI (VIS-AI) uses to differentiate the absorbing and non-absorbing aerosol types. If we combine two types of indices at the coordinate system of two types of AI, distribution of indices contains different signals if aerosol types change theoretically. In this study, we want to find out classification results based by the observation data to see the theoretical distribution in two AI values. For the observation data, aerosol types are obtained from the results of MODIS-OMI algorithm and 4-channel algorithm classify four types of aerosols, i.e. dust, carbonaceous, sea-salt and Non-Absorbing (NA). These algorithms classify aerosol by using the characteristics of aerosol optical properties in visible and near IR regions. MODIS-OMI algorithm uses the MODIS AOD and UV-AI in OMI values. For UV-AI case, dust and carbonaceous types have larger UV-AI values than non-absorbing aerosols because of absorbing characteristics. However, dust and carbonaceous types cannot classify if UV-AI values use only. For VIS-AI case, dust has larger proportion, but carbonaceous aerosol has smaller proportion in high AI value. However, VIS-AI cannot clearly classify between dust and carbonaceous types except for the case of extremely high AI cases. In NA type, VIS-AI has almost positive values, but the distribution has smaller than the absorbing

  10. Aerosol Dynamics Laboratory

    SciTech Connect

    Rader, D.J.; Mondy, L.A.

    1990-04-01

    In past five years, Department 1510 has developed a state-of-the-art Aerosol Dynamics Laboratory (ADL). This report documents the current instrumentation and capabilities that exist in this laboratory. The ADL was developed from a variety of sources, with a primary contribution from Department 1510's Independent Research and Development program in aerosol dynamics. Current capabilities of the ADL include: (1) generation of calibration-quality monodisperse particles with diameters between 0.005 to 100 {mu}m, (2) real-time measurement of particle size distributions for particle diameters between 0.01 and 100 {mu}m, (3) in situ, real-time measurement of particle size distributions for particle diameters between 0.3 and 100 {mu}m, and (4) real-time measurement of particle charge distributions for particle diameters between 0.01 and 1.0 {mu}m. 14 refs., 5 figs.

  11. 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.

  12. 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

  13. Optical Properties of Polymers Relevant to Secondary Organic Aerosols

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2007-05-01

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

  15. 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.

  16. Improvement of Aerosol Prediction Capability

    DTIC Science & Technology

    2001-09-30

    by dust storms in the past.) The operational aerosol products will be used for initialization or specification of aerosols in COAMPS when new cloud...Figure 2. SeaWiFS visible imagery for May 18, 2001, showing a dust storm originating at dry lakes along the Iran-Afghanistan border and then...versions of the Navy Aerosol Analysis and Prediction System (NAAPS) for analysis of airborne dust loads (Westphal/NRL). B: Modify existing radiative

  17. 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

  18. Development towards a global operational aerosol consensus: basic climatological characteristics of the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME)

    NASA Astrophysics Data System (ADS)

    Sessions, W. R.; Reid, J. S.; Benedetti, A.; Colarco, P. R.; da Silva, A.; Lu, S.; Sekiyama, T.; Tanaka, T. Y.; Baldasano, J. M.; Basart, S.; Brooks, M. E.; Eck, T. F.; Iredell, M.; Hansen, J. A.; Jorba, O. C.; Juang, H.-M. H.; Lynch, P.; Morcrette, J.-J.; Moorthi, S.; Mulcahy, J.; Pradhan, Y.; Razinger, M.; Sampson, C. B.; Wang, J.; Westphal, D. L.

    2014-06-01

    Over the past several years, there has been a rapid development in the number and quality of global aerosol models intended for operational forecasting use. Indeed, most centers with global numerical weather prediction (NWP) capabilities have some program for aerosol prediction. These aerosol models typically have differences in their underlying meteorology as well as aerosol sources, sinks, microphysics and transformations. However, like similar diversity in aerosol climate models, the aerosol forecast models have fairly similar overall bulk error statistics for aerosol optical thickness (AOT)-one of the few aerosol metrics that is globally available. Experience in climate and weather prediction has shown that in situations such as this where there are several independent models, a multi-model ensemble or consensus will be top performing in many key error metrics. Further, multi-model ensembles provide a highly valuable tool for forecasters attempting to predict severe aerosol events. Here we present the first steps in developing a global multi-model aerosol forecasting ensemble intended for eventual operational and basic research use. Drawing from members of the International Cooperative for Aerosol Prediction (ICAP) latest generation of quasi-operational aerosol models, five day AOT forecasts are analyzed for December 2011 through November 2012 from four institutions: ECMWF, JMA, NASA GSFC, and NRL/FNMOC. For dust, we also include the NOAA NGAC product in our analysis. The Barcelona Supercomputing Centre (NMMC) and UK Met office dust product have also recent become available with ICAP, but have insufficient data to be included in this analysis period. A simple consensus ensemble of member and mean AOT fields for modal species (e.g., fine and coarse mode, and a separate dust ensemble) is used to create the ICAP Multi-Model Ensemble (ICAP-MME). The ICAP-MME is run daily at 0Z for 6 hourly forecasts out to 120 h. Basing metrics on comparisons to 21 regionally

  19. Subarctic atmospheric aerosol composition: 2. Hygroscopic growth properties

    SciTech Connect

    Herich, Hanna; Kammermann, Lukas; Friedman, Beth; Gross, Deborah S.; Weingartner, E.; Lohmann, U.; Spichtinger, Peter; Gysel, Martin; Baltensperger, Urs; Cziczo, Daniel J.

    2009-07-10

    Sub-arctic aerosols were sampled during July 2007 at the Abisko Scientific Research Station Stordalen site in northern Sweden with an instrument setup consisting of a custom-built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) connected in series to a single particle mass spectrometer. Aerosol chemical composition in the form of bipolar single particle mass spectra was determined as a function of hygroscopic growth both in situ and in real time. The HTDMA was deployed at a relative humidity of 82% and particles with a dry mobility diameter of 260 nm were selected. Aerosols from two distinct airmasses were analyzed during the sampling period. Sea salt aerosols were found to be the dominant particle group with the highest hygroscopicity. High intensities of sodium and related peaks in the mass spectra were identified as exclusive markers for large hygroscopic growth. Particles from biomass combustion were found to be the least hygroscopic aerosol category. Species normally considered soluble (e.g., sulfates and nitrates) were found in particles ranging from high to low hygroscopicity. Furthermore, the signal intensities of the peaks related to these species did not correlate with hygroscopicity.

  20. Electro-Optical Aerosol Phase Function Database PFNDAT2005

    DTIC Science & Technology

    2005-11-01

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

  1. 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

  2. Volcanic aerosols and lunar eclipses.

    PubMed

    Keen, R A

    1983-12-02

    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.

  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. 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

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

    NASA Astrophysics Data System (ADS)

    Curci, G.; Hogrefe, C.; Bianconi, R.; Im, U.; Balzarini, A.; Baró, R.; Brunner, D.; Forkel, R.; Giordano, L.; Hirtl, M.; Honzak, L.; Jiménez-Guerrero, P.; Knote, C.; Langer, M.; Makar, P. A.; Pirovano, G.; Pérez, J. L.; San José, R.; Syrakov, D.; Tuccella, P.; Werhahn, J.; Wolke, R.; Žabkar, R.; Zhang, J.; Galmarini, S.

    2015-08-01

    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 intercomparison, we used the bulk mass profiles of aerosol chemical species sampled over the locations of AERONET stations across Europe and North America to calculate the aerosol optical properties under a range of common assumptions for all models. Several simulations with parameters perturbed within a range of observed values are carried out for July 2010 and compared in order to infer the assumptions that have the largest impact on the calculated aerosol optical properties. We calculate that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. The uncertainty introduced by the choice of mixing state choice on the calculation of the asymmetry parameter is the order of 10%. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. It is thus recommended to focus further research on a more accurate representation of the aerosol mixing state in models, in order to have a less uncertain simulation of the related optical properties.

  6. The uptake of HO2 radicals to organic aerosols

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  7. Evaluation of the global aerosol microphysical ModelE2-TOMAS model against satellite and ground-based observations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2015-03-01

    The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the-art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and overpredicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

  8. Modeling global organic aerosol formation and growth

    NASA Astrophysics Data System (ADS)

    Tsimpidi, Alexandra; Karydis, Vlasios; Pandis, Spyros; Lelieveld, Jos

    2014-05-01

    A computationally efficient framework for the description of organic aerosol (OA)-gas partitioning and chemical aging has been developed and implemented into the EMAC atmospheric chemistry-climate model. This model simulates the formation of primary (POA) and secondary organic aerosols (SOA) from semi-volatile (SVOC), intermediate-volatile (IVOC) and volatile organic compounds (VOC). POA are divided in two groups with saturation concentrations at 298 K 0.1, 10, 1000, 100000 µg m-3: OA from fossil fuel combustion and biomass burning. The first 2 surrogate species from each group represent the SVOC while the other surrogate species represent the IVOC. Photochemical reactions that change the volatility of the organics in the gas phase are taken into account. The oxidation products from each group of precursors (SVOC, IVOC, and VOC) are lumped into an additional set of oxidized surrogate species (S-SOA, I-SOA, and V-SOA, respectively) in order to track their source of origin. This model is used to i) estimate the relative contributions of SOA and POA to total OA, ii) determine how SOA concentrations are affected by biogenic and anthropogenic emissions, and iii) evaluate the effect of photochemical aging and long-range transport on OA budget over specific regions.

  9. 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

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

    PubMed

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

    2014-02-01

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

  11. 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

  12. 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

  13. Calculation of aerosol optical properties under different assumptions on mixing state, refractive index, density and hygroscopicity: uncertainties and importance of representation of aerosol mixing state

    NASA Astrophysics Data System (ADS)

    Curci, Gabriele

    2015-04-01

    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. We used the FlexAOD post-processing tool to calculate the optical properties (aerosol optical depth (AOD), single scattering albedo (SSA) and asymmetry parameter (g)) from chemistry-transport model aerosol profiles, using a wide range of assumptions on aerosol chemical and physical properties. We calculated that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. We then tested simple parameterizations of the aerosol mixing state, expressed as a function of the aerosol aging, and verified that they may be helpful in reducing the uncertainty when comparing simulations with AERONET retrievals.

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

    NASA Technical Reports Server (NTRS)

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

    2005-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2005-01-01

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

  16. Size-resolved aerosol composition and its link to hygroscopicity at a forested site in Colorado

    NASA Astrophysics Data System (ADS)

    Levin, E. J. T.; Prenni, A. J.; Palm, B. B.; Day, D. A.; Campuzano-Jost, P.; Winkler, P. M.; Kreidenweis, S. M.; DeMott, P. J.; Jimenez, J. L.; Smith, J. N.

    2014-03-01

    Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen-Rocky Mountain Biogenic Aerosol Study) campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions were between 70 and 90%. Corresponding aerosol hygroscopicity was observed to be in the range κ = 0.15-0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an aerosol mass spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study, with an assumed value of κorg = 0.13 resulting in the best agreement.

  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. 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.

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

    NASA Astrophysics Data System (ADS)

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

    1986-03-01

    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.

  20. Mount Saint Helens aerosol evolution

    NASA Technical Reports Server (NTRS)

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

    1982-01-01

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

  1. 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...

  2. Aerosol Variability Observed with Rpas

    NASA Astrophysics Data System (ADS)

    Altstädter, B.; Lampert, A.; Scholtz, A.; Bange, J.; Platis, A.; Hermann, M.; Wehner, B.

    2013-08-01

    To observe the origin, vertical and horizontal distribution and variability of aerosol particles, and especially ultrafine particles recently formed, we plan to employ the remotely piloted aircraft system (RPAS) Carolo-P360 "ALADINA" of TU Braunschweig. The goal of the presented project is to investigate the vertical and horizontal distribution, transport and small-scale variability of aerosol particles in the atmospheric boundary layer using RPAS. Two additional RPAS of type MASC of Tübingen University equipped with turbulence instrumentation add the opportunity to study the interaction of the aerosol concentration with turbulent transport and exchange processes of the surface and the atmosphere. The combination of different flight patterns of the three RPAS allows new insights in atmospheric boundary layer processes. Currently, the different aerosol sensors are miniaturized at the Leibniz Institute for Tropospheric Research, Leipzig and together with the TU Braunschweig adapted to fit into the RPAS. Moreover, an additional meteorological payload for measuring temperature, humidity and turbulence properties is constructed by Tübingen University. Two condensation particle counters determine the total aerosol number with a different lower detection threshold in order to investigate the horizontal and vertical aerosol variability and new particle formation (aerosol particles of some nm diameter). Further the aerosol size distribution in the range from about 0.300 to ~5 μm is given by an optical particle counter.

  3. 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.

  4. 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.

  5. Sampling stratospheric aerosols with impactors

    NASA Technical Reports Server (NTRS)

    Oberbeck, Verne R.

    1989-01-01

    Derivation of statistically significant size distributions from impactor samples of rarefield stratospheric aerosols imposes difficult sampling constraints on collector design. It is shown that it is necessary to design impactors of different size for each range of aerosol size collected so as to obtain acceptable levels of uncertainty with a reasonable amount of data reduction.

  6. Aerosol forcing in the Climate Model Intercomparison Project (CMIP5) simulations by HadGEM2-ES and the role of ammonium nitrate

    NASA Astrophysics Data System (ADS)

    Bellouin, Nicolas; Rae, Jamie; Jones, Andy; Johnson, Colin; Haywood, Jim; Boucher, Olivier

    2011-10-01

    The latest Hadley Centre climate model, HadGEM2-ES, includes Earth system components such as interactive chemistry and eight species of tropospheric aerosols. It has been run for the period 1860-2100 in support of the fifth phase of the Climate Model Intercomparison Project (CMIP5). Anthropogenic aerosol emissions peak between 1980 and 2020, resulting in a present-day all-sky top of the atmosphere aerosol forcing of -1.6 and -1.4 W m-2 with and without ammonium nitrate aerosols, respectively, for the sum of direct and first indirect aerosol forcings. Aerosol forcing becomes significantly weaker in the 21st century, being weaker than -0.5 W m-2 in 2100 without nitrate. However, nitrate aerosols become the dominant species in Europe and Asia and decelerate the decrease in global mean aerosol forcing. Considering nitrate aerosols makes aerosol radiative forcing 2-4 times stronger by 2100 depending on the representative concentration pathway, although this impact is lessened when changes in the oxidation properties of the atmosphere are accounted for. Anthropogenic aerosol residence times increase in the future in spite of increased precipitation, as cloud cover and aerosol-cloud interactions decrease in tropical and midlatitude regions. Deposition of fossil fuel black carbon onto snow and ice surfaces peaks during the 20th century in the Arctic and Europe but keeps increasing in the Himalayas until the middle of the 21st century. Results presented here confirm the importance of aerosols in influencing the Earth's climate, albeit with a reduced impact in the future, and suggest that nitrate aerosols will partially replace sulphate aerosols to become an important anthropogenic species in the remainder of the 21st century.

  7. 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.

  8. A novel ultrasonic aerosol generator.

    PubMed

    Davies, A; Hudson, N; Pirie, L

    1995-07-01

    An ultrasonic aerosol generator constructed from a domestic humidifier is described which has been used to produce liquid aerosols for physiological investigations. The instrument was constructed from a Pifco domestic humidifier modified to include an energy guide to direct the oscillations of the transducer through the coupling water, which would normally be aerosolized, onto a small membrane based sample chamber containing the liquid to be aerosolized. The size distribution of the aerosol produced was found to be between 2 and 6 mm, optimum for diffuse intrapulmonary deposition. Up to 4 ml/min of aqueous liquid was used; however the sample chamber could be made small enough to contain economic amounts of expensive material to administer by inhalation. The instrument has proved to be reliable over a period of three years.

  9. 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

  10. 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

  11. Improved and new balloon-borne instruments for the measurements of stratospheric aerosols

    NASA Astrophysics Data System (ADS)

    Renard, Jean-Baptiste; Berthet, Gwenael; Gaubicher, Bertrand; Chartier, Michel; Brogniez, Colette; Verwaerde, Christian; Balois, Jean-Yves; Auriol, Frédérique; Palumbo, Pasquale

    The aerosols in the stratosphere play an important role in the ozone chemistry. Liquid sulphate aerosols are involved in the heterogeneous chemistry of nitrogen and bromine species. The key parameters for modelling calculations of stratospheric species are the amount of these aerosols and their size distribution. In fact, the aerosol content in the stratosphere is more complex than previously assumed, since different natures of solid particles are present: soot from various origins and interplanetary dust intercepted by the Earth atmosphere. Since no major volcanic eruption has occurred since 15 years, it is possible to study at present the content of stratospheric background aerosols and to detect the different natures of particles. There is no unique technique of measurements in order to fully describe the physical properties of liquid and solid aerosols. Then different instruments must be used: SALOMON-N2, which is a night-time UV-visible spectrometer (from 350 to 950 nm) allowing the retrieval of the extinction coefficient of aerosols, the STAC particle counter (giving 14 size classes of aerosols), and MicroRADIBAL, which is a polarimeter allowing the retrieval of the aerosol phase function from the radiance and the polarisation measurements in the near infrared. Analysis of measurements performed during previous flights shows that significant amount of solid aerosols were detected in the middle stratosphere, up to about 30 km, with strong spatial and temporal variability. Combined aerosols measurements are necessary in order to be able to distinguish between the various natures of aerosols. Then, STAC is now implanted in the SALOMON-N2 and MicroRADIBAL gondolas. STAC can be also implanted on other gondolas flying in the stratosphere a few days apart, in order to study the variability of the total aerosol content. A new instrument, DUSTER, will be implanted soon in the SALOMON gondola. This instrument will collect solid particles in the middle stratosphere, in

  12. 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

  13. Relationship between CCN activation properties and oxidation level of aerosol organics observed during recent field studies

    NASA Astrophysics Data System (ADS)

    Mei, F.; Zhang, Q.; Xu, J.; Setyan, A.; Hayes, P. L.; Ortega, A. M.; Allan, J. D.; Taylor, J.; Jimenez, J.; Wang, J.

    2011-12-01

    Organic compounds are an important component of atmospheric aerosol, and can contribute upward of ~90% of total fine aerosol mass. Atmospheric aerosols often consist of hundreds of organic species, and their hygroscopicities are not well understood. This incomplete understanding limits our ability to accurately simulate aerosol cloud condensation nuclei (CCN) spectrum and therefore the aerosol indirect effects, which remain the most uncertain components in forcing of climate change over the industrial period. In this study, the hygroscopicity of aerosol organics characterized during three recent field campaigns, CalNex-LA (Pasadena, California), CARES (Cool, CA), and Aerosol lifecycle IOP (Upton, NY), is presented. Hygroscopicity of aerosol particles, which were mixtures of both inorganic and organic species, is first determined from the size-resolved activation efficiency spectrum. Based on measured aerosol chemical composition, the hygroscopicity of organics is then derived from the particle hygroscopicity by subtracting the contribution of inorganic species, whose hygroscopicities are well understood. During the three field studies, organic aerosols were characterized within a number of representative air masses, including urban plumes and those dominated by biogenic emissions. Aerosol organics measured by HR-ToF-AMS exhibit various degrees of photochemical aging, with the atomic O:C ratio ranges from ~0.35 to ~0.65. The hygroscopicity of organics is well correlated with its O:C ratio, increasing from 0.07 at the O:C ratio of 0.35 to 0.16 at the O:C ratio of 0.65. This suggests that to the first order, a simple, semi-empirical parameterization of organic aerosol hygroscopicity based on oxidation level can be developed for global models. While the measurements show that aerosol organics can substantially influence the droplet growth kinetics by modifying particle critical supersaturation, size-classified organic particles exhibit essentially identical growth

  14. 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

  15. 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.

  16. Speciation of Fe in ambient aerosol and cloudwater

    SciTech Connect

    Siefert, Ronald Lyn

    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.

  17. 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

  18. Uncertainty associated with convective wet removal of entrained aerosols in a global climate model

    NASA Astrophysics Data System (ADS)

    Croft, B.; Pierce, J. R.; Martin, R. V.; Hoose, C.; Lohmann, U.

    2012-11-01

    The uncertainties associated with the wet removal of aerosols entrained above convective cloud bases are investigated in a global aerosol-climate model (ECHAM5-HAM) under a set of limiting assumptions for the wet removal of the entrained aerosols. The limiting assumptions for the wet removal of entrained aerosols are negligible scavenging and vigorous scavenging (either through activation, with size-dependent impaction scavenging, or with the prescribed fractions of the standard model). To facilitate this process-based study, an explicit representation of cloud-droplet-borne and ice-crystal-borne aerosol mass and number, for the purpose of wet removal, is introduced into the ECHAM5-HAM model. This replaces and is compared with the prescribed cloud-droplet-borne and ice-crystal-borne aerosol fraction scavenging scheme of the standard model. A 20% to 35% uncertainty in simulated global, annual mean aerosol mass burdens and optical depth (AOD) is attributed to different assumptions for the wet removal of aerosols entrained above convective cloud bases. Assumptions about the removal of aerosols entrained above convective cloud bases control modeled upper tropospheric aerosol concentrations by as much as one order of magnitude. Simulated aerosols entrained above convective cloud bases contribute 20% to 50% of modeled global, annual mean aerosol mass convective wet deposition (about 5% to 10% of the total dry and wet deposition), depending on the aerosol species, when including wet scavenging of those entrained aerosols (either by activation, size-dependent impaction, or with the prescribed fraction scheme). Among the simulations, the prescribed fraction and size-dependent impaction schemes yield the largest global, annual mean aerosol mass convective wet deposition (by about two-fold). However, the prescribed fraction scheme has more vigorous convective mixed-phase wet removal (by two to five-fold relative to the size-dependent impaction scheme) since nearly all

  19. 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 ...

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

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

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

  1. 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

  2. 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.

  3. 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

  4. 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.

  5. Evaluating Simulations of Primary Anthropogenic and Biomass Burning Organic Aerosols using Aerosol Mass Spectrometer Data and Positive Matrix Factorization Analysis

    NASA Astrophysics Data System (ADS)

    Fast, J.; Aiken, A.; Alexander, L.; Canagaratna, M.; Decarlo, P.; Herndon, S.; Jimenez, J.; Kleinman, L.; Ochoa, C.; Onasch, T.; Song, C.; Wiedinmyer, C.; Yu, X.; Zaveri, R.

    2008-12-01

    Most model predictions of organic matter are currently underestimated because the processes contributing to secondary organic aerosol (SOA) formation and transformation are not well understood. Since research associated with developing a better framework to improve the representation of specific gas-to-particle partitioning processes controlling SOA based on new measurements and theoretical relationships is on- going, this study seeks to determine whether 3-D models can adequately predict concentrations of primary organic aerosols (POA). If one assumes POA is non-volatile, then errors in POA predictions will results from uncertainties in the emission inventories and errors in transport and mixing processes. The WRF-chem model is used to predict POA in the vicinity of Mexico City during the 2006 MILAGRO field campaign. Particulate matter emission rates were obtained from urban and regional Mexican emission inventories and from biomass burning estimates derived from MODIS "hotspot" and vegetation databases. Organic aerosol predictions are evaluated using data from Aerodyne Aerosol Mass Spectrometer (AMS) instruments deployed at four ground sites and on two research aircraft and from Sunset Laboratory OCEC instruments deployed at two ground sites. Positive Matrix Factorization (PMF) has recently been applied to derive components of organic aerosols including: hydrocarbon-like organic aerosol (HOA), oxidized organic aerosol (OOA), and biomass burning organic aerosols (BBOA). The temporal variation of HOA is often similar to primary emissions of other species in urban areas. PMF analysis is currently available for three of the ground sites and for some of the aircraft flights. We found that the predicted POA was consistently lower than the measured organic matter at the ground sites, which is consistent with the expectation that SOA should be a large fraction of the total organic aerosol mass. A much better agreement was found when predicted POA was compared with HOA

  6. 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.

  7. 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.

  8. 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.

  9. On the mixing and evaporation of secondary organic aerosol components.

    PubMed

    Loza, Christine L; Coggon, Matthew M; Nguyen, Tran B; Zuend, Andreas; Flagan, Richard C; Seinfeld, John H

    2013-06-18

    The physical state and chemical composition of an organic aerosol affect its degree of mixing and its interactions with condensing species. We present here a laboratory chamber procedure for studying the effect of the mixing of organic aerosol components on particle evaporation. The procedure is applied to the formation of secondary organic aerosol (SOA) from α-pinene and toluene photooxidation. SOA evaporation is induced by heating the chamber aerosol from room temperature (25 °C) to 42 °C over 7 h and detected by a shift in the peak diameter of the SOA size distribution. With this protocol, α-pinene SOA is found to be more volatile than toluene SOA. When SOA is formed from the two precursors sequentially, the evaporation behavior of the SOA most closely resembles that of SOA from the second parent hydrocarbon, suggesting that the structure of the mixed SOA resembles a core of SOA from the initial precursor coated by a layer of SOA from the second precursor. Such a core-and-shell configuration of the organic aerosol phases implies limited mixing of the SOA from the two precursors on the time scale of the experiments, consistent with a high viscosity of at least one of the phases.

  10. Characterization of aerosols containing Legionella generated upon nebulization.

    PubMed

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

    2016-09-27

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

  11. 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

  12. Characterization of aerosols containing Legionella generated upon nebulization

    PubMed Central

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

    2016-01-01

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

  13. Characterization of aerosols containing Legionella generated upon nebulization

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

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

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

    PubMed Central

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

    1970-01-01

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

  15. Aerosols, light, and water: Measurements of aerosol optical properties at different relative humidities

    NASA Astrophysics Data System (ADS)

    Orozco, Daniel

    (RH) at a certain RH divided by sp at a dry value, was used to evaluate the aerosol hygroscopicity. Different empirical fits were evaluated using the f(RH) data. The widely used gamma model was found inappropriate, as it overestimates f(RH) for RH<75%. Abetter empirical fit with two power-law curve-fitting parameters c and k was found to replicate f(RH) accurately from the three sites. The relationship between the organic carbon mass (OMC) and the species that are affected by RH and f(RH) was also studied and categorized between the sites. A second experiment is reported where the first two elements of the scattering matrix of laboratory generated particles were studied under different humidity conditions. The non-spherical particles generated were ammonium sulfate, sodium chloride, and ammonium nitrate. The optical measurements were performed with a polarized imaging nephelometer (PI-Neph) installed in series with the humidifier dryer apparatus. The inorganic salts experienced low (80%) RH levels so that the observations could contrast the differences when the salts were crystallized (low RH) and when the particles turned to aqueous solutions after deliquesence (high RH). The measurements with the PI-Neph produce the aerosol phase function and the polarized phase function in a range of angles that go from 3 to 177. The results showed significant changes in the phase function and polarized phase function due to the hygroscopic growth. Although the inorganic salts used inthe experiments were non-spherical, the dry measurements were successfully reproduced with the Mie theory using literature values for the dry index of refraction. Moreover, the changes in the particle size distribution and index of refraction were evaluated through classic thermodynamic equilibrium theory producing comparable results with the simulations performed with Mie formalism. The final experiment consisted in the measurements of phase function and degree of linear polarization of ambient aerosols

  16. 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

  17. 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.

  18. 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

  19. Direct radiative effects of aerosols over South Asia from observations and modeling

    NASA Astrophysics Data System (ADS)

    Nair, Vijayakumar S.; Babu, S. Suresh; Manoj, M. R.; Moorthy, K. Krishna; Chin, Mian

    2016-10-01

    Quantitative assessment of the seasonal variations in the direct radiative effect (DRE) of composite aerosols as well as the constituent species over the Indian sub continent has been carried out using a synergy of observations from a dense network of ground based aerosol observatories and modeling based on chemical transport model simulations. Seasonal variation of aerosol constituents depict significant influence of anthropogenic aerosol sources in winter and the dominance of natural sources in spring, even though the aerosol optical depth doesn't change significantly between these two seasons. A significant increase in the surface cooling and atmospheric warming has been observed as season changes from winter (DRESUR = -28 ± 12 W m-2 and DREATM = +19.6 ± 9 W m-2) to spring (DRESUR = -33.7 ± 12 W m-2 and DREATM = +27 ± 9 W m-2). Interestingly, springtime aerosols are more absorptive in nature compared to winter and consequently the aerosol induced diabatic heating of the atmosphere goes as high as 1 K day-1 during spring, especially over eastern India. The atmospheric DRE due to dust aerosols (+14 ± 7 W m-2) during spring overwhelms that of black carbon DRE (+11.8 ± 6 W m-2) during winter. The DRE at the top of the atmosphere is mostly governed by the anthropogenic aerosols during all the seasons. The columnar aerosol loading, its anthropogenic fraction and radiative effects shows a steady increase with latitude across Indian mainland leading to a larger aerosol-induced atmospheric warming during spring than in winter.

  20. Influences from soluble and insoluble aerosols on precipitation and lightning in deep convection

    NASA Astrophysics Data System (ADS)

    Phillips, Vaughan; Formenton, Marco; Lienert, Barry

    2013-04-01

    Observations reported in past studies in the literature have revealed correlations between measures of aerosol loading and lightning occurrence. Recent advances in simulating cloud-microphysical processes have highlighted their control by aerosol conditions. New hypotheses about aerosol-precipitation-lightning interactions have emerged. Most deep convective clouds globally have warm bases with precipitation controlled by coalescence and by loadings of soluble aerosols, which form droplets. However, those over mountainous continental regions often have cooler bases and can generate much hail that reaches the ground. Cold-base convective clouds were observed to produce lightning over the High Plains of the USA during the Severe Thunderstorms Electrification and Precipitation Study (STEPS) in the summer of 2000. Cold-base thunderstorms can be without an active coalescence process, due to the low adiabatic liquid water content limiting droplet sizes. There is then the potential for a greater influence from ice-nucleating insoluble aerosols on ice-precipitation production, charge separation and lightning, relative to soluble aerosols. In the presentation, an aerosol-cloud model (hybrid bin/2-moment bulk microphysics, prognostic aerosol component with 6 aerosol species) with a new electrification component is described. The model treats non-inductive charge separation and has a lightning discharge scheme. A simulation of a STEPS case of a cold-base thunderstorm is validated against aircraft, radar and electrical observations. Sensitivity tests are presented to show the roles of ice multiplication and ice-nucleating aerosols, such as dust and soot from biomass-burning plumes, in controlling ice-precipitation production and lightning frequencies for the cold-base thunderstorm. Their influence is compared with that from soluble aerosol loadings. The roles of cloud-base temperature and wet growth of hail and graupel are discussed.

  1. 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

  2. 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

  3. Representation and evaluation of aerosol mixing state in a climate model

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Prather, K. A.; Ault, A. P.

    2011-12-01

    Aerosol particles in the atmosphere are composed out of multiple chemical species. The aerosol mixing state is an important aerosol property that will determine the interaction of aerosols with the climate system via radiative forcings and cloud activation. Through the introduction of aerosol microphysics into climate models, aerosol mixing state is by now taken into account to a certain extend in climate models, and evaluation of mixing state is the next challenge. Here we use data from the Aerosol Time of Flight Mass Spectrometer (ATOFMS) and compare the results to the GISS-modelE-MATRIX model, a global climate model including a detailed aerosol micro-physical scheme. We use data from various field campaigns probing, urban, rural and maritime air masses and compare those to climatological and nudged simulations for the years 2005 to 2009. ATOFMS provides information about the size distributions of several mixing state classes, including the chemical components of black and organic carbon, sulfates, dust and salts. MATRIX simulates 16 aerosol populations, which definitions are based on mixing state. We have grouped ATOFMS and MATRIX data into similar mixing state classes and compare the size resolved number concentrations against each other. As a first result we find that climatological simulations are rather difficult to evaluate with field data, and that nudged simulations give a much better agreement. However this is not just caused by the better fit of natural - meteorological driven - aerosol components, but also due to the interaction between meteorology and aerosol formation. The model seems to get the right amount of mixing state of black carbon material with sulfate and organic components, but seems to always overestimate the fraction of black carbon that is externally mixed. In order to understand this bias between model and the ATOFMS data, we will look into microphysical processes near emission sources and investigate the climate relevance of these sub

  4. Characterization of fine mode atmospheric aerosols by Raman microscopy and diffuse reflectance FTIR.

    PubMed

    Gaffney, Jeffrey S; Marley, Nancy A; Smith, Kenneth J

    2015-05-14

    A combination of Raman microscopy and diffuse reflectance Fourier transform infrared spectroscopy (FTIR) has been used for the characterization of fine mode (<1 μm) tropospheric aerosols. Peak fitting was used to identify five overlapping bands in the Raman spectra. These bands have been identified as due to combustion generated carbon soot as well as large molecular organic carbon species. The fwhm of the D band at 1400 cm(-1) as well as the ratio of intensities of the D3 band at 1550 cm(-1) to the G band at 1580 cm(-1) can serve as a measure of the aerosol organic carbon content. Raman microscopy combined with spectral mapping capabilities was used to investigate the composition of the fine mode aerosols at the particle level, allowing for the direct determination of aerosol mixing state. Results showed that the fine aerosols were predominately internally mixed particles composed of carbon soot coated with molecular organic carbon species. Characterization of the aerosols by diffuse reflectance FTIR showed that the major organic carbon species were polycarboxylates and polysaccharide-like species typical of humic-like substances (HULIS).

  5. 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.

  6. 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.

  7. 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.

  8. Aerosol measurement program strategy for global aerosol backscatter model development

    NASA Technical Reports Server (NTRS)

    Bowdle, David A.

    1985-01-01

    The purpose was to propose a balanced program of aerosol backscatter research leading to the development of a global model of aerosol backscatter. Such a model is needed for feasibility studies and systems simulation studies for NASA's prospective satellite-based Doppler lidar wind measurement system. Systems of this kind measure the Doppler shift in the backscatter return from small atmospheric aerosol wind tracers (of order 1 micrometer diameter). The accuracy of the derived local wind estimates and the degree of global wind coverage for such a system are limited by the local availability and by the global scale distribution of natural aerosol particles. The discussions here refer primarily to backscatter model requirements at CO2 wavelengths, which have been selected for most of the Doppler lidar systems studies to date. Model requirements for other potential wavelengths would be similar.

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

    NASA Astrophysics Data System (ADS)

    Grivicke, Rasa

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

  10. Processing of Ambient Aerosols During Fog Events: Role of Acidity

    NASA Astrophysics Data System (ADS)

    Chakraborty, A.; Gupta, T.; Tripathi, S. N.; Bhattu, D.

    2013-12-01

    Fog is a major processing and removal agent of ambient aerosols. Enhanced secondary organic aerosol (SOA) production has been reported during fog events indicating major role of aqueous processing. Present study was carried out in a heavily polluted city of Kanpur situated in Indo-Gangetic plain of India,from 02- 18 Nov, 2012 and then from 22 Dec, 2012 to 10 January, 2013. 12 fog events were identified from 22 Dec to 10 January based on low visibility (< 300 m) with high liquid water content (~ 0.04 g/m3) and termed as foggy period while remaining as non-foggy period. Foggy period typically showed very high RH (~95%), low temperatures (~2-6°C) compared to non-foggy period. An array of instruments were deployed during this campaign for real time measurement of aerosol physico-chemical properties - High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS), Scanning Mobility Particle Sizer (SMPS), Cloud Combination Probe (CCP), Cloud Condensation Nuclei counter (CCN), fog water collector and Vaisala RH & T sensor. Average aerosol loading during foggy period was 104×44 μg/m3, much higher than 73×49 μg/m3of non-foggy period, but during actual fog events the loading reduced to 85×23 μg/m3 indicating overall aerosol removal by fog. Overall aerosol composition during both the period was dominated by organics which constitutes about 60-70% of the total AMS mass followed by nitrate, but during foggy period sulfate was found to be increased many fold.HR analysis of AMS data revealed noticeable differences in the diurnal average values of O:C ratio between foggy and non -foggy period. Although diurnal O:C ratio was highest around noontime for both period but during fog events, night to early morning O:C ratio was 0.51×0.04, higher than that of non-foggy period 0.44×0.07, clearly indicating enhanced oxidation. AMS data also showed that mode size of all the species specially of organics and sulphate had shifted to a higher diameter during foggy period, an

  11. On the contribution of organics to the North East Atlantic aerosol number concentration

    NASA Astrophysics Data System (ADS)

    Bialek, Jakub; Dall'Osto, Manuel; Monahan, Ciaran; Beddows, David; O'Dowd, Colin

    2012-12-01

    k-means statistical-cluster analysis of submicron aerosol size distributions is combined with coincident humidity tandem differential mobility analyser data, leading to five unique aerosol categories for hygroscopic growth factors (HGFs): low sea-salt background marine, high sea-salt background marine, coastal nucleation, open ocean nucleation and anthropogenically influenced scenarios. When considering only marine conditions, and generic aerosol species associated with this environment (e.g. non-sea-salt sulfate, sea-salt, partly soluble organic matter and water insoluble organic matter), the two-year annual average contribution to aerosol number concentration from the different generic species was made up as follows: 46% (30-54%) of partially modified ammonium sulfate particles; 23% (11-40%) of partially modified sea-salt; and the remaining 31% (25-35%) contribution attributed to two distinct organic species as evidenced by different, but low, HGFs. The analysis reveals that on annual timescales, ˜30% of the submicron marine aerosol number concentration is sourced from predominantly organic aerosol while 60% of the anthropogenic aerosol number is predominantly organic. Coastal nucleation events show the highest contribution of the lowest HGF mode (1.19), although this contribution is more likely to be influenced by inorganic iodine oxides. While organic mass internally mixed with inorganic salts will lower the activation potential of these mixed aerosol types, thereby potentially reducing the concentration of cloud condensation nuclei (CCN), pure organic water soluble particles are still likely to be activated into cloud droplets, thereby increasing the concentration of CCN. A combination of dynamics and aerosol concentrations will determine which effect will prevail under given conditions.

  12. 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

  13. Local environmental pollution strongly influences culturable bacterial aerosols at an urban aquatic superfund site.

    PubMed

    Dueker, M Elias; O'Mullan, Gregory D; Juhl, Andrew R; Weathers, Kathleen C; Uriarte, Maria

    2012-10-16

    In polluted environments, when microbial aerosols originate locally, species composition of the aerosols should reflect the polluted source. To test the connection between local environmental pollution and microbial aerosols near an urban waterfront, we characterized bacterial aerosols at Newtown Creek (NTC), a public waterway and Superfund site in a densely populated area of New York, NY, USA. Culturable bacterial aerosol fallout rate and surface water bacterial concentrations were at least an order of magnitude greater at NTC than at a neighboring, less polluted waterfront and a nonurban coastal site in Maine. The NTC culturable bacterial aerosol community was significantly different in taxonomic structure from previous urban and coastal aerosol studies, particularly in relative abundances of Actinobacteria and Proteobacteria. Twenty-four percent of the operational taxonomic units in the NTC overall (air + water) bacterial isolate library were most similar to bacterial 16S rRNA gene sequences previously described in terrestrial or aquatic environments contaminated with sewage, hydrocarbons, heavy metals, and other industrial waste. This study is the first to examine the community composition and local deposition of bacterial aerosols from an aquatic Superfund site. The findings have important implications for the use of aeration remediation in polluted aquatic environments and suggest a novel pathway of microbial exposure in densely populated urban communities containing contaminated soil and water.

  14. 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.

  15. Remote Sensing of Aerosol and Non-Aerosol Absorption

    NASA Technical Reports Server (NTRS)

    Kaufman, Y. J.; Dubovik, O.; Holben, B. N.; Remer, L. A.; Tanre, D.; Lau, William K. M. (Technical Monitor)

    2001-01-01

    Remote sensing of aerosol from the new satellite instruments (e.g. MODIS from Terra) and ground based radiometers (e.g. the AERONET) provides the opportunity to measure the absorption characteristics of the ambient undisturbed aerosol in the entire atmospheric column. For example Landsat and AERONET data are used to measure spectral absorption of sunlight by dust from West Africa. Both Application of the Landsat and AERONET data demonstrate that Saharan dust absorption of solar radiation is several times smaller than the current international standards. This is due to difficulties of measuring dust absorption in situ, and due to the often contamination of dust properties by the presence of air pollution or smoke. We use the remotely sensed aerosol absorption properties described by the spectral sin le scattering albedo, together with statistics of the monthly optical thickness for the fine and coarse aerosol derived from the MODIS data. The result is an estimate of the flux of solar radiation absorbed by the aerosol layer in different regions around the globe where aerosol is prevalent. If this aerosol forcing through absorption is not included in global circulation models, it may be interpreted as anomalous absorption in these regions. In a preliminary exercise we also use the absorption measurements by AERONET, to derive the non-aerosol absorption of the atmosphere in cloud free conditions. The results are obtained for the atmospheric windows: 0.44 microns, 0.66 microns, 0.86 microns and 1.05 microns. In all the locations over the land and ocean that were tested no anomalous absorption in these wavelengths, was found within absorption optical thickness of +/- 0.005.

  16. Aerosol Climate Time Series Evaluation In ESA Aerosol_cci

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  17. 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

  18. 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.

  19. 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.

  20. 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

  1. Maritime Aerosol Network as a component of Aerosol Robotic Network

    NASA Astrophysics Data System (ADS)

    Smirnov, A.; Holben, B. N.; Slutsker, I.; Giles, D. M.; McClain, C. R.; Eck, T. F.; Sakerin, S. M.; Macke, A.; Croot, P.; Zibordi, G.; Quinn, P. K.; Sciare, J.; Kinne, S.; Harvey, M.; Smyth, T. J.; Piketh, S.; Zielinski, T.; Proshutinsky, A.; Goes, J. I.; Nelson, N. B.; Larouche, P.; Radionov, V. F.; Goloub, P.; Krishna Moorthy, K.; Matarrese, R.; Robertson, E. J.; Jourdin, F.

    2009-03-01

    The paper presents the current status of the Maritime Aerosol Network (MAN), which has been developed as a component of the Aerosol Robotic Network (AERONET). MAN deploys Microtops handheld Sun photometers and utilizes the calibration procedure and data processing (Version 2) traceable to AERONET. A web site dedicated to the MAN activity is described. A brief historical perspective is given to aerosol optical depth (AOD) measurements over the oceans. A short summary of the existing data, collected on board ships of opportunity during the NASA Sensor Intercomparison and Merger for Biological and Interdisciplinary Oceanic Studies (SIMBIOS) Project is presented. Globally averaged oceanic aerosol optical depth (derived from island-based AERONET measurements) at 500 nm is ˜0.11 and Angstrom parameter (computed within spectral range 440-870 nm) is calculated to be ˜0.6. First results from the cruises contributing to the Maritime Aerosol Network are shown. MAN ship-based aerosol optical depth compares well to simultaneous island and near-coastal AERONET site AOD.

  2. Soft Ionization of Thermally Evaporated Hypergolic Ionic Liquid Aerosols

    SciTech Connect

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

    2011-04-20

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

  3. 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.

  4. Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

    SciTech Connect

    Ching, Ping Pui; Riemer, Nicole; West, Matthew

    2016-05-27

    Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcel cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.

  5. 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

  6. 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.

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

    PubMed

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

    2007-09-20

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  9. Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

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

  10. 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.

  11. Uptake of HO2 Radicals Onto Dust Aerosols

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  12. Multi-year Cluster Analyses of CALIPSO Aerosol Layer Data

    NASA Astrophysics Data System (ADS)

    Omar, A. H.; Sumner, A. J.; Vaughan, M.

    2013-12-01

    points within each cluster along with geographical map overlays shows that the clusters formed contained combinations or mixtures of the six types in CALIPSO Level 2 data. These results suggest a larger number of aerosol types, possibly involving combinations of the six types in the current CALIPSO subtyping algorithms, or a smaller number of base species, e.g., sulfate, black carbon, seasalt and dust.

  13. Aerosol studies during the ESCOMPTE experiment: an overview

    NASA Astrophysics Data System (ADS)

    Cachier, Hélène; Aulagnier, Fabien; Sarda, Roland; Gautier, François; Masclet, Pierre; Besombes, Jean-Luc; Marchand, Nicolas; Despiau, Serge; Croci, Delphine; Mallet, Marc; Laj, Paolo; Marinoni, Angela; Deveau, Pierre-Alexandre; Roger, Jean-Claude; Putaud, Jean-Philippe; Van Dingenen, Rita; Dell'Acqua, Alessandro; Viidanoja, Jyrkki; Martins-Dos Santos, Sebastiao; Liousse, Cathy; Cousin, Frédéric; Rosset, Robert; Gardrat, Eric; Galy-Lacaux, Corinne

    2005-03-01

    satisfactorily for the measured aerosol concentrations. The formation of secondary particles in the model is currently underway; initial encouraging results show that the model accounts for the formation of secondary species, such as sulphate and organic particles. Finally, radiative calculations suggest that the role of the fine aerosol fraction is predominant mostly due to the presence of black carbon (BC) particles, which could induce a regional atmospheric heating.

  14. Stratospheric aerosols and climatic change

    NASA Technical Reports Server (NTRS)

    Baldwin, B.; Pollack, J. B.; Summers, A.; Toon, O. B.; Sagan, C.; Van Camp, W.

    1976-01-01

    Generated primarily by volcanic explosions, a layer of submicron silicate particles and particles made of concentrated sulfuric acids solution is present in the stratosphere. Flights through the stratosphere may be a future source of stratospheric aerosols, since the effluent from supersonic transports contains sulfurous gases (which will be converted to H2SO4) while the exhaust from Space Shuttles contains tiny aluminum oxide particles. Global heat balance calculations have shown that the stratospheric aerosols have made important contributions to some climatic changes. In the present paper, accurate radiative transfer calculations of the globally-averaged surface temperature (T) are carried out to estimate the sensitivity of the climate to changes in the number of stratospheric aerosols. The results obtained for a specified model atmosphere, including a vertical profile of the aerosols, indicate that the climate is unlikely to be affected by supersonic transports and Space Shuttles, during the next decades.

  15. Satellite measurements of tropospheric aerosols

    NASA Technical Reports Server (NTRS)

    Griggs, M.

    1981-01-01

    This investigation uses LANDSAT 2 radiance data and ground-truth measurements of the aerosol optical thickness, obtained previously from five inland sites, to study the usefulness and limitations of the near infrared radiance over inland bodies of water. The linear relationship between LANDSAT 2 MSS7 and aerosol content found in this study can be used to estimate the aerosol content with a standard deviation of 0.42N. Analysis of the data for MSS6 and MSS7 suggest that the larger uncertainty is mostly due to water turbidity, with little contribution from the adjacency effect. The relationship found is best applied to determine an average aerosol content over a period of time at a given target, or an area average at a given time over several targets close together.

  16. Wind Power Charged Aerosol Generator

    SciTech Connect

    Marks, A.M.

    1980-07-01

    This describes experimental results on a Charged Aerosol Wind/Electric Power Generator, using Induction Electric Charging with a water jet issuing under water pressure from a small diameter (25-100 ..mu..m) orifice.

  17. 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

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

    PubMed

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

    2008-11-13

    We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changes in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of 'acid rain' that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy

  19. Method for producing monodisperse aerosols

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

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

  20. Aerosol Microphysics and Radiation Integration

    DTIC Science & Technology

    2016-06-07

    for dust storm forecasting and analysis, AGU Fall Meeting, San Francisco, CA. Dec. 11-15, 2002 [Published]. Reid, J.S., J.R. Cook, D.L. Westphal...Persian Gulf/Arabian Sea, East Asia, and some parts of the Mediterranean Sea. Along coastal regions, dust , pollution and smoke can be present and...transitioned from the combined Marine Aerosol and Dust Aerosol programs from SPAWAR Systems Center San Diego (SSC-SD) to the Naval Research Laboratory

  1. AEROSOL, CLOUDS, AND CLIMATE CHANGE

    SciTech Connect

    SCHWARTZ, S.E.

    2005-09-01

    Earth's climate is thought to be quite sensitive to changes in radiative fluxes that are quite small in absolute magnitude, a few watts per square meter, and in relation to these fluxes in the natural climate. Atmospheric aerosol particles exert influence on climate directly, by scattering and absorbing radiation, and indirectly by modifying the microphysical properties of clouds and in turn their radiative effects and hydrology. The forcing of climate change by these indirect effects is thought to be quite substantial relative to forcing by incremental concentrations of greenhouse gases, but highly uncertain. Quantification of aerosol indirect forcing by satellite- or ground-based remote sensing has proved quite difficult in view of inherent large variation in the pertinent observables such as cloud optical depth, which is controlled mainly by liquid water path and only secondarily by aerosols. Limited work has shown instances of large magnitude of aerosol indirect forcing, with local instantaneous forcing upwards of 50 W m{sup 66}-2. Ultimately it will be necessary to represent aerosol indirect effects in climate models to accurately identify the anthropogenic forcing at present and over secular time and to assess the influence of this forcing in the context of other forcings of climate change. While the elements of aerosol processes that must be represented in models describing the evolution and properties of aerosol particles that serve as cloud condensation particles are known, many important components of these processes remain to be understood and to be represented in models, and the models evaluated against observation, before such model-based representations can confidently be used to represent aerosol indirect effects in climate models.

  2. 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.

  3. 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.

  4. Formation and Processing of Organic Aerosols Measured by a Time of Flight Aerosol Mass Spectrometer during TexAQS/GoMACCS 2006

    NASA Astrophysics Data System (ADS)

    Bahreini, R.; Middlebrook, A. M.; Decarlo, P. F.; Denlea, E.; Jimenez, J. L.; Brock, C. A.; Degouw, J. A.; Flocke, F.; Gallar, C.; Holloway, J. S.; Neuman, J. A.; Ryerson, T. B.; Schwarz, J. P.; Spackman, J. R.; Trainer, M. K.; Warneke, C.; Wollny, A. G.; Zhang, W.; Fehsenfeld, F. C.

    2007-12-01

    Formation of particulate matter is common in areas with high emissions of volatile organic compounds (VOCs), NOx, and SO2. These particles have lifetimes of days to weeks, and thus can have both local and regional effects on visibility, air quality, and human health as well as direct and indirect effects on climate. During TexAQS 2006, mass concentrations of non-refractory inorganic species (sulfate, ammonium, and nitrate) and total organics in submicron aerosols were measured by a Compact Time of Flight Aerosol Mass Spectrometer (C-ToF-AMS) onboard the NOAA WP-3D aircraft. In this presentation, we analyze composition changes of organic aerosols in different air masses. We examine organic mass spectra along with simultaneous measurements of VOCs and their oxidation products in order to determine the contribution of anthropogenic and biogenic sources to the aerosol organic mass. These measurements were performed in plumes intercepted during the daytime north of Houston where large isoprene emissions were observed. Furthermore, the fresh hydrocarbon-like (HOA) and processed oxygenated-like organics (OOA) fractions of the total organic aerosol mass in several plumes transected during daytime and nighttime are presented and compared. We will also discuss differences in correlations between organic aerosol composition markers and primary or secondary gas-phase species in different plumes.

  5. CALIPSO Observations of Aerosol Properties Near Clouds

    NASA Technical Reports Server (NTRS)

    Marshak, Alexander; Varnai, Tamas; Yang, Weidong

    2010-01-01

    Clouds are surrounded by a transition zone of rapidly changing aerosol properties. Characterizing this zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects as well as for improving satellite measurements of aerosol properties. We present a statistical analysis of a global dataset of CALIPSO (Cloud-Aerosol Lidar and infrared Pathfinder Satellite Observation) Lidar observations over oceans. The results show that the transition zone extends as far as 15 km away from clouds and it is ubiquitous over all oceans. The use of only high confidence level cloud-aerosol discrimination (CAD) data confirms the findings. However, the results underline the need for caution to avoid biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

  6. Satellite Remote Sensing: Aerosol Measurements

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2013-01-01

    Aerosols are solid or liquid particles suspended in the air, and those observed by satellite remote sensing are typically between about 0.05 and 10 microns in size. (Note that in traditional aerosol science, the term "aerosol" refers to both the particles and the medium in which they reside, whereas for remote sensing, the term commonly refers to the particles only. In this article, we adopt the remote-sensing definition.) They originate from a great diversity of sources, such as wildfires, volcanoes, soils and desert sands, breaking waves, natural biological activity, agricultural burning, cement production, and fossil fuel combustion. They typically remain in the atmosphere from several days to a week or more, and some travel great distances before returning to Earth's surface via gravitational settling or washout by precipitation. Many aerosol sources exhibit strong seasonal variability, and most experience inter-annual fluctuations. As such, the frequent, global coverage that space-based aerosol remote-sensing instruments can provide is making increasingly important contributions to regional and larger-scale aerosol studies.

  7. Climate forcing by anthropogenic aerosols

    NASA Technical Reports Server (NTRS)

    Charlson, R. J.; Schwartz, S. E.; Hales, J. M.; Cess, R. D.; Coakley, J. A., Jr.; Hansen, J. E.; Hofmann, D. J.

    1992-01-01

    Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol, in particular, has imposed a major perturbation to this forcing. Both the direct scattering of short-wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

  8. Modeling aerosol-water interactions in subsaturated and supersaturated environments

    NASA Astrophysics Data System (ADS)

    Fountoukis, Christos

    conditions. Based on its computational rigor and performance, ISORROPIA-II appears to be a highly attractive alternative for use in large scale air quality and atmospheric transport models. The new equilibrium model was also used to thermodynamically characterize aerosols measured at a Megacity. In the ammonia-rich environment of Mexico City, nitrate and chloride primarily partition in the aerosol phase with a 20-min equilibrium timescale; PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. When RH is below 50%, predictions improve substantially if the aerosol follows a deliquescent behavior. The impact of including crustal species (Ca2+, K +, M2+) in equilibrium calculations within a three dimensional air quality model was also studied. A significant change in aerosol water (20%) and ammonium (-27.5%) concentrations was predicted when crustals are explicitly included in the calculations even though they contributed, on average, only a few percent of the total PM2.5 mass, highlighting the need for comprehensive thermodynamic calculations in the presence of dust.

  9. Assessment of the Aerosol Distribution Over Indian Subcontinent in CMIP5 Models

    NASA Astrophysics Data System (ADS)

    Sanap, S. D.; Pandithurai, G.

    2014-12-01

    This paper examines the aerosol distribution over Indian subcontinent as represented in 21 models from Coupled Model Inter-comparison Project Phase 5 (CMIP5) simulations, wherein model simulated aerosol optical depth (AOD) is compared with Moderate Resolution Imaging Spectro-radiometer (MODIS) satellite observations. The objective of the study is to provide an assessment of the capability of various global models, participating in CMIP5 project, in capturing the realistic spatial and temporal distribution of aerosol species over the Indian subcontinent. Results from our analysis show that majority of the CMIP5 models seriously underestimates the spatio-temporal variability of aerosol species over the Indian subcontinent, in particular over Indo-Gangetic Plains(IGP). Though the representation of black carbon (BC) loading in many models is fairly good, the dust loading is observed to be significantly low in majority of the models. The presence of pronounced dust activity over northern India and dust being one of the major constituent of aerosol species, the biases in dust loading has a great impact on the AOD of that region. We found that considerable biases in simulating the 850 hPa wind field (which plays important role in transport of dust from adjacent deserts) would be the possible reason for poor representation of dust AOD and in turn total AOD over Indian region in CMIP5 models. In addition, aerosol radiative forcing (ARF) underestimated/overestimated in most of the models. However, spatial distribution of ARF in multi-model ensemble mean is comparable reasonably well with observations with bias in magnitudes. This analysis emphasizes the fundamental need to improve the representation of aerosol species in current state of the art climate models. As reported in Intergovernmental Panel on Climate Change (IPCC) fourth assessment report (AR4), the level of scientific understanding (LOSU) of climatic impact of aerosols is medium-low. For better understanding of

  10. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouch, N.; Pichon, J.-M.; Prévôt, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2013-09-01

    The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA

  11. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouche, N.; Pichon, J.-M.; Bourianne, T.; Gomes, L.; Prevot, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2014-02-01

    The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation

  12. Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

    NASA Astrophysics Data System (ADS)

    Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

    2014-11-01

    The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

  13. Test-Aerosol Generator For Calibrating Particle Counters

    NASA Technical Reports Server (NTRS)

    Mogan, Paul A.; Adams, Alois J.; Schwindt, Christian J.; Hodge, Timothy R.; Mallow, Tim J.; Duong, Anh A.; Bukauskas, Vyto V.

    1996-01-01

    Apparatus generates clean, stable aerosol stream for use in testing and calibrating laser-based aerosol-particle counter. Size and concentration of aerosol particles controlled to ensure accurate calibration. Cheap, widely available medical nebulizers used to generate aerosols.

  14. Analysis of anions in ambient aerosols by microchip capillary electrophoresis.

    PubMed

    Liu, Yan; MacDonald, David A; Yu, Xiao-Ying; Hering, Susanne V; Collett, Jeffrey L; Henry, Charles S

    2006-11-01

    We describe a microchip capillary electrophoresis method for the analysis of nitrate and sulfate in ambient aerosols. Investigating the chemical composition of ambient aerosol particles is essential for understanding their sources and effects. Significant progress has been made towards developing mass spectrometry-based instrumentation for rapid qualitative analysis of aerosols. Alternative methods for rapid quantification of selected high abundance compounds are needed to augment the capacity for widespread routine analysis. Such methods could provide much higher temporal and spatial resolution than can be achieved currently. Inorganic anions comprise a large percentage of particulate mass, with nitrate and sulfate among the most abundant species. While ion chromatography has proven very useful for analyzing extracts of time-integrated ambient aerosol samples collected on filters and for semi-continuous, on-line particle composition measurements, there is a growing need for development of new compact, inexpensive approaches to routine on-line aerosol ion analysis for deployment in spatially dense, atmospheric measurement networks. Microchip capillary electrophoresis provides the necessary speed and portability to address this need. In this report, on-column contact conductivity detection is used with hydrodynamic injection to create a simple microchip instrument for analysis of nitrate and sulfate. On-column contact conductivity detection was achieved using a Pd decoupler placed upstream from the working electrodes. Microchips containing two Au or Pd working electrodes showed a good linear range (5-500 microM) and low limits-of-detection for sulfate and nitrate, with Au providing the lowest detection limits (1 microM) for both ions. The completed microchip system was used to analyze ambient aerosol filter samples. Nitrate and sulfate concentrations measured by the microchip matched the concentrations measured by ion chromatography.

  15. Reactions and mass spectra of complex particles using Aerosol CIMS

    NASA Astrophysics Data System (ADS)

    Hearn, John D.; Smith, Geoffrey D.

    2006-12-01

    Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

  16. Aerosol size distribution and aerosol water content measurements during Atlantic Stratocumulus Transition Experiment/Marine Aerosol and Gas Exchange

    NASA Astrophysics Data System (ADS)

    Kim, Y.; Sievering, H.; Boatman, J.; Wellman, D.; Pszenny, A.

    1995-11-01

    Aerosol size distribution data measured during the June 1992 Marine Aerosol and Gas Exchange experiment are analyzed to investigate the characteristics of fine marine aerosol particles measured over the North Atlantic near the Azores Islands. Measured aerosol size distribution data were corrected using the corrected size calibration data based on the optical properties of particles being measured. The corrected size distribution data were then approximated with either one or two lognormal size distributions, depending on air mass conditions. Under clean air mass conditions <3 μm diameter aerosol size distributions typically exhibited two modes, consisting of an accumulation mode and the small end of the sea-salt particle mode. However, under the influence of continental polluted air masses, the aerosol size distribution was dominated by <1 μm diameter particles in a single mode with an increased aerosol concentration. Aerosol water content of accumulation mode marine aerosols was estimated from differences between several series of ambient and dried aerosol size distributions. The average aerosol water fraction was 0.31, which is in good agreement with an empirical aerosol growth model estimate. The average rate of SO4= production in the accumulation mode aerosol water by H2O2 oxidation was estimated to be <7×10-10 mol L-1 s-1, which is an insignificant contributor to the observed non-sea-salt SO4= in the accumulation mode.

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

    NASA Astrophysics Data System (ADS)

    Andersson, Emma; Kahnert, Michael

    2016-05-01

    A new aerosol-optics model is implemented in which realistic morphologies and mixing states are assumed, especially for black carbon particles. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey-shell" model. Simulated results of aerosol optical properties, such as aerosol optical depth, backscattering coefficients and the Ångström exponent, as well as radiative fluxes are computed with the new optics model and compared with results from an older optics-model version that treats all particles as externally mixed homogeneous spheres. The results show that using a more detailed description of particle morphology and mixing state impacts the aerosol optical properties to a degree of the same order of magnitude as the effects of aerosol-microphysical processes. For instance, the aerosol optical depth computed for two cases in 2007 shows a relative difference between the two optics models that varies over the European region between -28 and 18 %, while the differences caused by the inclusion or omission of the aerosol-microphysical processes range from -50 to 37 %. This is an important finding, suggesting that a simple optics model coupled to a chemical transport model can introduce considerable errors affecting radiative fluxes in chemistry-climate models, compromising comparisons of model results with remote sensing observations of aerosols, and impeding the assimilation of satellite products for aerosols into chemical-transport models.

  18. Toward new techniques to measure heterogeneous oxidation of aerosol: Electrodynamic Balance-Mass Spectrometry (EDB-MS) and Aerosol X-ray Photoelectron Spectroscopy

    NASA Astrophysics Data System (ADS)

    Jacobs, M. I.; Heine, N.; Xu, B.; Davies, J. F.; Kirk, B. B.; Kostko, O.; Alayoglu, S.; Wilson, K. R.; Ahmed, M.

    2015-12-01

    The chemical composition and physical properties of aerosol can be changed via heterogeneous oxidation with the OH radical. However, the physical state of the aerosol influences the kinetics of this reaction; liquid particles with a high diffusion coefficient are expected to be well mixed and homogenously oxidized, while oxidation of solid, diffusion-limited aerosol is expected to occur primarily on the surface, creating steep chemical gradients within the particle. We are working to develop several new techniques to study the heterogeneous oxidation of different types of aerosol. We are developing a "modular" electrodynamic balance (EDB) that will enable us to study heterogeneous oxidation at aqueous interfaces using a mass-spectrometer (and potentially other detection techniques). Using a direct analysis in real time (DART) interface, preliminary droplet train measurements have demonstrated single-droplet mass spectrometry to be possible. With long reaction times in our EDB, we will be able to study heterogeneous oxidation of a wide variety of organic species in aqueous droplets. Additionally, we are working to use aerosol photoemission and velocity map imaging (VMI) to study the surface of aerosol particles as they undergo heterogeneous oxidation. With VMI, we're able to collect electrons with a 4π collection efficiency over conventional electron energy analyzers. Prelimina