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Title: Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties

Abstract

The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. In this paper, we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of ≤2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. Lastly, the forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.

Authors:
 [1];  [2];  [3];  [4];  [5];  [1];  [6]; ORCiD logo [4];  [7];  [8];  [9];  [9];  [10];  [1]
  1. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences Program and Department of Physics
  2. Naval Postgraduate School, Monterey, CA (United States). Dept. of Meteorology
  3. U.S. EPA, Research Triangle Park, NC (United States)
  4. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences Program
  5. Michigan Technological Univ., Houghton, MI (United States). Department of Chemistry
  6. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences Program and Department of Chemistry; University of Rijeka (Croatia). Department of Biotechnology
  7. University of Azores, Angra do Heroísmo (Portugal). Department of Agricultural Sciences
  8. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences Program and Department of Civil and Environmental Engineering
  9. Univ. of Colorado, Boulder, CO (United States). Institute of Alpine and Arctic Research
  10. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences Program and Department of Chemistry
Publication Date:
Research Org.:
Michigan Technological Univ., Houghton, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1454934
Alternate Identifier(s):
OSTI ID: 1402214
Grant/Contract Number:  
SC0006941
Resource Type:
Accepted Manuscript
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 42; Journal Issue: 4; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; soot; morphology; free troposphere; long-range transport

Citation Formats

China, Swarup, Scarnato, Barbara, Owen, Robert C., Zhang, Bo, Ampadu, Marian T., Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Fialho, Paulo, Perlinger, Judith A., Hueber, Jacques, Helmig, Detlev, Mazzoleni, Lynn R., and Mazzoleni, Claudio. Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties. United States: N. p., 2015. Web. doi:10.1002/2014GL062404.
China, Swarup, Scarnato, Barbara, Owen, Robert C., Zhang, Bo, Ampadu, Marian T., Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Fialho, Paulo, Perlinger, Judith A., Hueber, Jacques, Helmig, Detlev, Mazzoleni, Lynn R., & Mazzoleni, Claudio. Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties. United States. doi:10.1002/2014GL062404.
China, Swarup, Scarnato, Barbara, Owen, Robert C., Zhang, Bo, Ampadu, Marian T., Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Fialho, Paulo, Perlinger, Judith A., Hueber, Jacques, Helmig, Detlev, Mazzoleni, Lynn R., and Mazzoleni, Claudio. Wed . "Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties". United States. doi:10.1002/2014GL062404. https://www.osti.gov/servlets/purl/1454934.
@article{osti_1454934,
title = {Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties},
author = {China, Swarup and Scarnato, Barbara and Owen, Robert C. and Zhang, Bo and Ampadu, Marian T. and Kumar, Sumit and Dzepina, Katja and Dziobak, Michael P. and Fialho, Paulo and Perlinger, Judith A. and Hueber, Jacques and Helmig, Detlev and Mazzoleni, Lynn R. and Mazzoleni, Claudio},
abstractNote = {The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. In this paper, we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of ≤2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. Lastly, the forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.},
doi = {10.1002/2014GL062404},
journal = {Geophysical Research Letters},
number = 4,
volume = 42,
place = {United States},
year = {2015},
month = {1}
}

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