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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Discussion papers | Copyright
https://doi.org/10.5194/acp-2018-255
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 21 Mar 2018

Research article | 21 Mar 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Secondary Organic Aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects

Juliane L. Fry1, Steven S. Brown2,5, Ann M. Middlebrook2, Peter M. Edwards2,3,4, Pedro Campuzano-Jost3,5, Douglas A. Day3,5, José L. Jimenez3,5, Hannah M. Allen6, Thomas B. Ryerson2, Ilana Pollack2,3,a, Martin Graus3,b, Carsten Warneke2,3, Joost A. de Gouw3,5, Charles A. Brock2, Jessica Gilman2,3, Brian M. Lerner2,3,c, William P. Dubé2,3, Jin Liao2,3,d, and André Welti2,3,e Juliane L. Fry et al.
  • 1Chemistry Department, Reed College, Portland, OR, USA
  • 2Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
  • 3Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 4Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
  • 5Department of Chemistry, University of Colorado, Boulder, CO, USA
  • 6Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
  • anow at: Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
  • bnow at: Institute of Atmospheric and Cryospheric Sciences, University of Innsbruck, Austria
  • cnow at: Aerodyne Research, Inc., Billerica, MA, USA
  • dnow at: Universities Space Research Association, Columbia, MD, USA and NASA Goddard Space Flight Center, Atmospheric Chemistry and Dynamic Laboratory, Greenbelt, MD, USA
  • enow at: Leibniz Institute for Tropospheric Research, Department of Physics, Leipzig, Germany

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 southeast 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 9 plumes is 9%. Corresponding mass yields depend on the assumed molecular formula for isoprene-NO3-SOA, but the average over 9 plumes is 27%, larger than those previously measured in chamber studies (12–14% 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 ambient peroxy radical lifetimes and heterogeneous reactions of NO3-isoprene gas phase products. Future studies of aerosol composition from NO3 radical + isoprene are needed to better understand the oxidation chemistry producing this potentially important coupled anthropogenic – biogenic source of SOA.

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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory-in-the-field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced pollutant emissions (the smokestack plumes) with natural background molecules emitted by trees in the southeastern United States. We did this analysis because in the real atmosphere we observe different behavior than in the lab.
This paper uses measurements made during research aircraft flights through power plant...
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