Title: Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States

Abstract

The chemical complexity of atmospheric organic aerosol (OA) has caused substantial uncertainties in understanding its origins and environmental impacts. Here, we provide constraints on OA origins through compositional characterization with molecular-level details. Our results suggest that secondary OA (SOA) from monoterpene oxidation accounts for approximately half of summertime fine OA in Centreville, AL, a forested area in the southeastern United States influenced by anthropogenic pollution. We find that different chemical processes involving nitrogen oxides, during days and nights, play a central role in determining the mass of monoterpene SOA produced. These findings elucidate the strong anthropogenic–biogenic interaction affecting ambient aerosol in the southeastern United States and point out the importance of reducing anthropogenic emissions, especially under a changing climate, where biogenic emissions will likely keep increasing.

Authors:

Zhang, Haofei  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-7936-4493"

Yee, Lindsay D. ^[2]; Lee, Ben H.  ^[3];

• Search DOE PAGES for author "Lee, Ben H."
• Search DOE PAGES for ORCID "0000-0002-5057-2168"

Curtis, Michael P. ^[4]; Worton, David R. ^[5]; Isaacman-VanWertz, Gabriel ^[2]; Offenberg, John H. ^[6]; Lewandowski, Michael ^[6]; Kleindienst, Tadeusz E. ^[6]; Beaver, Melinda R. ^[6]; Holder, Amara L. ^[7]; Lonneman, William A. ^[6]; Docherty, Kenneth S. ^[8]; Jaoui, Mohammed ^[6]; Pye, Havala O. T. ^[6]; Hu, Weiwei ^[9]; Day, Douglas A. ^[9]; Campuzano-Jost, Pedro ^[9]; Jimenez, Jose L. ^[9]; Guo, Hongyu ^[10] more »; Weber, Rodney J. ^[10]; de Gouw, Joost ^[11]; Koss, Abigail R. ^[11]; Edgerton, Eric S. ^[12]; Brune, William ^[13]; Mohr, Claudia ^[3]; Lopez-Hilfiker, Felipe D. ^[3]; Lutz, Anna ^[14]; Kreisberg, Nathan M. ^[15]; Spielman, Steve R. ^[15]; Hering, Susanne V. ^[15]; Wilson, Kevin R. ^[16]; Thornton, Joel A. ^[3]; Goldstein, Allen H. ^[17] « less

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+ Show Author Affiliations

1. Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA 94720,, Department of Chemistry, University of California, Riverside, CA 92521,
2. Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA 94720,
3. Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195,
4. Department of Earth and Planetary Science, University of California, Berkeley, CA 94720,
5. Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA 94720,, Aerosol Dynamics Inc., Berkeley, CA 94710,
6. National Exposure Research Laboratory, Office of Research and Development, US Environmental Protection Agency, Research Triangle Park, NC 27711,
7. National Risk Management Laboratory, Office of Research and Development, US Environmental Protection, Agency, Research Triangle Park, NC 27711,
8. Jacobs Technology, Inc., Research Triangle Park, NC 27711,
9. Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO 80309,, Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309,
10. School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332,
11. Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309,, National Oceanic and Atmospheric Administration Earth System Research Laboratory, Boulder, CO 80305,
12. Atmospheric Research and Analysis, Cary, NC 27513,
13. Department of Meteorology, Pennsylvania State University, University Park, PA 16802,
14. Department of Chemistry and Molecular Biology, University of Gothenberg, SE-41296 Gothenberg, Sweden,
15. Aerosol Dynamics Inc., Berkeley, CA 94710,
16. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
17. Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA 94720,, Department of Civil and Environmental Engineering, University of California, Berkeley, CA 94720

Publication Date:

Mon Feb 12 00:00:00 EST 2018

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1420215

Alternate Identifier(s):

OSTI ID: 1456999

Grant/Contract Number:  

AC02-05CH11231; SC0016559; AGS-1250569; AGS-1644406

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 9; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

54 ENVIRONMENTAL SCIENCES; aerosol source apportionment; biogenic volatile organic compound oxidation; nitrogen oxides