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Published August 16, 2018 | Supplemental Material + Published
Journal Article Open

Secondary organic aerosol (SOA) yields from NO_3 radical + isoprene based on nighttime aircraft power plant plume transects

Abstract

Nighttime reaction of nitrate radicals (NO_3) 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 (NO_x) emissions, resulting in a large model-predicted NO_3-BVOC source of SOA. Coal-fired power plants in this region constitute substantial NO_x 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 NO_3 radicals rapidly remove isoprene, to obtain field-based estimates of the secondary organic aerosol yield from NO_3+isoprene. Observed in-plume increases in nitrate aerosol are consistent with organic nitrate aerosol production from NO_3+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-NO_3-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 NO_3-isoprene gas phase products. More in-depth studies are needed to better understand the aerosol yield and oxidation mechanism of NO_3 radical+isoprene, a coupled anthropogenic–biogenic source of SOA that may be regionally significant.

Additional Information

© 2018 Author(s). This work is distributed under the Creative Commons Attribution 4.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 9 March 2018 – Discussion started: 21 March 2018. Revised: 31 July 2018 – Accepted: 1 August 2018 – Published: 16 August 2018. Juliane L. Fry gratefully acknowledges funding from the EPA STAR Program (no. RD-83539901) and from the Fulbright US Scholars Program in the Netherlands. Pedro Campuzano-Jost, Douglas A. Day and José L. Jimenez were partially supported by EPA STAR 83587701-0 and DOE (BER/ASR) DE-SC0016559. This paper has not been formally reviewed by the EPA. The views expressed in this document are solely those of the authors, and do not necessarily reflect those of the EPA. The EPA does not endorse any products or commercial services mentioned in this publication. Data availability: All data is available at: https://esrl.noaa.gov/ csd/groups/csd7/measurements/2013senex/P3/DataDownload/ (National Oceanic and Atmospheric Administration, 2018). Author contributions: JLF, SSB, and AMM conducted data analysis and wrote the paper. PME contributed modeling and writing. DAD, PCJ, and JLJ contributed data analysis and writing. Other coauthors contributed data. The authors declare that they have no conflict of interest.

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Published - acp-18-11663-2018.pdf

Supplemental Material - acp-18-11663-2018-supplement.pdf

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