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Title: Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

Abstract

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m-3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very agedmore » (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.« less

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [6];  [6];  [2];  [4];  [7];  [8];  [9];  [10];  [10];  [11]
+ Show Author Affiliations
  1. Michigan Technological Univ., Houghton, MI (United States). Department of Chemistry and Atmospheric Science Program
  2. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Science Program and Department of Physics
  3. Azores University, Angra do Heroísmo (Portugal). Department of Agricultural Sciences
  4. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Science Program and Department of Civil and Environmental Engineering
  5. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Science Program
  6. Univ. of Colorado, Boulder, CO (United States). Institute of Arctic and Alpine Research (INSTAAR)
  7. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Science Program and Department of Geological and Mining Engineering and Sciences
  8. Michigan Technological Univ., Houghton, MI (United States). Department of Geological and Mining Engineering and Sciences
  9. Michigan Technological Univ., Houghton, MI (United States). Department of Chemistry
  10. Univ. of Illinois, Urbana Champaign, IL (United States). Department of Atmospheric Science
  11. Michigan Technological Univ., Houghton, MI (United States). Department of Chemistry, Atmospheric Science Program and Department of Geological and Mining Engineering and Sciences
Publication Date:
Research Org.:
Michigan Technological Univ., Houghton, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1454935
Grant/Contract Number:  
SC0006941
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 15; Journal Issue: 9; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dzepina, K., Mazzoleni, C., Fialho, P., China, S., Zhang, B., Owen, R. C., Helmig, D., Hueber, J., Kumar, S., Perlinger, J. A., Kramer, L. J., Dziobak, M. P., Ampadu, M. T., Olsen, S., Wuebbles, D. J., and Mazzoleni, L. R. Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume. United States: N. p., 2015. Web. doi:10.5194/acp-15-5047-2015.
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Dzepina, K., Mazzoleni, C., Fialho, P., China, S., Zhang, B., Owen, R. C., Helmig, D., Hueber, J., Kumar, S., Perlinger, J. A., Kramer, L. J., Dziobak, M. P., Ampadu, M. T., Olsen, S., Wuebbles, D. J., & Mazzoleni, L. R. Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume. United States. https://doi.org/10.5194/acp-15-5047-2015
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Dzepina, K., Mazzoleni, C., Fialho, P., China, S., Zhang, B., Owen, R. C., Helmig, D., Hueber, J., Kumar, S., Perlinger, J. A., Kramer, L. J., Dziobak, M. P., Ampadu, M. T., Olsen, S., Wuebbles, D. J., and Mazzoleni, L. R. Tue . "Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume". United States. https://doi.org/10.5194/acp-15-5047-2015. https://www.osti.gov/servlets/purl/1454935.
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@article{osti_1454935,
title = {Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume},
author = {Dzepina, K. and Mazzoleni, C. and Fialho, P. and China, S. and Zhang, B. and Owen, R. C. and Helmig, D. and Hueber, J. and Kumar, S. and Perlinger, J. A. and Kramer, L. J. and Dziobak, M. P. and Ampadu, M. T. and Olsen, S. and Wuebbles, D. J. and Mazzoleni, L. R.},
abstractNote = {Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m-3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.},
doi = {10.5194/acp-15-5047-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 9,
volume = 15,
place = {United States},
year = {Tue May 05 00:00:00 EDT 2015},
month = {Tue May 05 00:00:00 EDT 2015}
}
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Technical Note: A new method for the Lagrangian tracking of pollution plumes from source to receptor using gridded model output
journal, November 2008

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