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Title: Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects

Abstract

Nighttime reaction of nitrate radicals (NO3) with biogenic volatile organic compounds (BVOC) has been proposed as a potentially important but also highly uncertain source of secondary organic aerosol (SOA). The southeastern United States has both high BVOC and nitrogen oxide (NOx) emissions, resulting in a large model-predicted NO3-BVOC source of SOA. Coal-fired power plants in this region constitute substantial NOx emissions point sources into a nighttime atmosphere characterized by high regionally widespread concentrations of isoprene. In this paper, we exploit nighttime aircraft observations of these power plant plumes, in which NO3 radicals rapidly remove isoprene, to obtain field-based estimates of the secondary organic aerosol yield from NO3 + isoprene. Observed in-plume increases in nitrate aerosol are consistent with organic nitrate aerosol production from NO3 + isoprene, and these are used to determine molar SOA yields, for which the average over nine plumes is 9 % (±5 %). Corresponding mass yields depend on the assumed molecular formula for isoprene-NO3-SOA, but the average over nine plumes is 27 %(±14 %), on average larger than those previously measured in chamber studies (12 %–14 % mass yield as ΔOA / ΔVOC after oxidation of both double bonds). Yields are larger for longer plume ages.Thismore » suggests that ambient aging processes lead more effectively to condensable material than typical chamber conditions allow. We discuss potential mechanistic explanations for this difference, including longer ambient peroxy radical lifetimes and heterogeneous reactions of NO3-isoprene gas phase products. As a result more in-depth studies are needed to better understand the aerosol yield and oxidation mechanism of NO3 radical + isoprene, a coupled anthropogenic–biogenic source of SOA that may be regionally significant.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [5];  [6];  [3];  [7];  [8];  [2]; ORCiD logo [5];  [3];  [2];  [9];  [2];  [10]; ORCiD logo [11]
+ Show Author Affiliations
  1. Reed College, Portland, OR (United States)
  2. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  3. National Oceanic and Atmospheric Administration, Boulder, CO (United States)
  4. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States); Univ. of York, York (United Kingdom)
  5. Univ. of Colorado, Boulder, CO (United States)
  6. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  7. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Colorado State Univ., Fort Collins, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  8. Univ. of Colorado, Boulder, CO (United States); Univ. of Innsbruck, Innsbruck (Austria)
  9. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States); Aerodyne Research, Inc., Billerica, MA (United States)
  10. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States); Univ. Space Research Assoc., Columbia, MD (United States); NASA Goddard Space Flight Center (GSFC), Greenbelt, MD (United States)
  11. National Oceanic and Atmospheric Administration, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States); Leibniz Institute for Tropospheric Research, Leipzig (Germany)
Publication Date:
Research Org.:
Univ. of Colorado, Denver, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1502876
Grant/Contract Number:  
SC0016559
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 16; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fry, Juliane L., Brown, Steven S., Middlebrook, Ann M., Edwards, Peter M., Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, José L., Allen, Hannah M., Ryerson, Thomas B., Pollack, Ilana, Graus, Martin, Warneke, Carsten, de Gouw, Joost A., Brock, Charles A., Gilman, Jessica, Lerner, Brian M., Dubé, William P., Liao, Jin, and Welti, André. Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects. United States: N. p., 2018. Web. doi:10.5194/acp-18-11663-2018.
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Fry, Juliane L., Brown, Steven S., Middlebrook, Ann M., Edwards, Peter M., Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, José L., Allen, Hannah M., Ryerson, Thomas B., Pollack, Ilana, Graus, Martin, Warneke, Carsten, de Gouw, Joost A., Brock, Charles A., Gilman, Jessica, Lerner, Brian M., Dubé, William P., Liao, Jin, & Welti, André. Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects. United States. https://doi.org/10.5194/acp-18-11663-2018
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Fry, Juliane L., Brown, Steven S., Middlebrook, Ann M., Edwards, Peter M., Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, José L., Allen, Hannah M., Ryerson, Thomas B., Pollack, Ilana, Graus, Martin, Warneke, Carsten, de Gouw, Joost A., Brock, Charles A., Gilman, Jessica, Lerner, Brian M., Dubé, William P., Liao, Jin, and Welti, André. Thu . "Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects". United States. https://doi.org/10.5194/acp-18-11663-2018. https://www.osti.gov/servlets/purl/1502876.
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@article{osti_1502876,
title = {Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects},
author = {Fry, Juliane L. and Brown, Steven S. and Middlebrook, Ann M. and Edwards, Peter M. and Campuzano-Jost, Pedro and Day, Douglas A. and Jimenez, José L. and Allen, Hannah M. and Ryerson, Thomas B. and Pollack, Ilana and Graus, Martin and Warneke, Carsten and de Gouw, Joost A. and Brock, Charles A. and Gilman, Jessica and Lerner, Brian M. and Dubé, William P. and Liao, Jin and Welti, André},
abstractNote = {Nighttime reaction of nitrate radicals (NO3) with biogenic volatile organic compounds (BVOC) has been proposed as a potentially important but also highly uncertain source of secondary organic aerosol (SOA). The southeastern United States has both high BVOC and nitrogen oxide (NOx) emissions, resulting in a large model-predicted NO3-BVOC source of SOA. Coal-fired power plants in this region constitute substantial NOx emissions point sources into a nighttime atmosphere characterized by high regionally widespread concentrations of isoprene. In this paper, we exploit nighttime aircraft observations of these power plant plumes, in which NO3 radicals rapidly remove isoprene, to obtain field-based estimates of the secondary organic aerosol yield from NO3 + isoprene. Observed in-plume increases in nitrate aerosol are consistent with organic nitrate aerosol production from NO3 + isoprene, and these are used to determine molar SOA yields, for which the average over nine plumes is 9 % (±5 %). Corresponding mass yields depend on the assumed molecular formula for isoprene-NO3-SOA, but the average over nine plumes is 27 %(±14 %), on average larger than those previously measured in chamber studies (12 %–14 % mass yield as ΔOA / ΔVOC after oxidation of both double bonds). Yields are larger for longer plume ages.This suggests that ambient aging processes lead more effectively to condensable material than typical chamber conditions allow. We discuss potential mechanistic explanations for this difference, including longer ambient peroxy radical lifetimes and heterogeneous reactions of NO3-isoprene gas phase products. As a result more in-depth studies are needed to better understand the aerosol yield and oxidation mechanism of NO3 radical + isoprene, a coupled anthropogenic–biogenic source of SOA that may be regionally significant.},
doi = {10.5194/acp-18-11663-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 16,
volume = 18,
place = {United States},
year = {2018},
month = {8}
}
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journal, September 2015

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  • DOI: 10.5194/acpd-11-5699-2011

Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature)
journal, January 2006

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The formation, properties and impact of secondary organic aerosol: current and emerging issues
text, January 2009

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  • DOI: 10.17615/k22s-ek71

A review of the anthropogenic influence on biogenic secondary organic aerosol
text, January 2011

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