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

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:
ORCiD logo [1] ;  [2] ; ORCiD logo [3] ;  [4] ;  [5] ;  [2] ;  [6] ;  [6] ;  [6] ;  [6] ;  [7] ;  [6] ;  [8] ;  [6] ;  [6] ;  [9] ;  [9] ;  [9] ;  [9] ;  [10] more »;  [10] ;  [11] ;  [11] ;  [12] ;  [13] ;  [3] ;  [3] ;  [14] ;  [15] ;  [15] ;  [15] ;  [16] ;  [3] ;  [17] « less
  1. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management
  3. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences
  4. Univ. of California, Berkeley, CA (United States). Dept. of Earth and Planetary Science
  5. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; Aerosol Dynamics Inc., Berkeley, CA (United States)
  6. US Environmental Protection Agency (EPA), Research Triangle Park, NC (United States). National Exposure Research Lab., Office of Research and Development
  7. US Environmental Protection Agency (EPA), Research Triangle Park, NC (United States). National Risk Management Lab., Office of Research and Development
  8. Jacobs Technology, Inc., Research Triangle Park, NC (United States)
  9. Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences
  10. Georgia Inst. of Technology, Atlanta, GA (United States). School of Earth and Atmospheric Sciences
  11. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences; National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Earth System Research Lab.
  12. Atmospheric Research and Analysis, Cary, NC (United States)
  13. Pennsylvania State Univ., University Park, PA (United States). Dept. of Meteorology
  14. Univ. of Gothenberg, Gothenberg (Sweden). Dept. of Chemistry and Molecular Biology
  15. Aerosol Dynamics Inc., Berkeley, CA (United States)
  16. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  17. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; Univ. of California, Berkeley, CA (United States). Dept. of of Civil and Environmental Engineering
Publication Date:
Grant/Contract Number:
AC02-05CH11231; SC0016559; AGS-1250569; AGS-1644406
Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 9; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; aerosol source apportionment; biogenic volatile organic compound oxidation; nitrogen oxides
OSTI Identifier:
1420215
Alternate Identifier(s):
OSTI ID: 1456999

Zhang, Haofei, Yee, Lindsay D., Lee, Ben H., Curtis, Michael P., Worton, David R., Isaacman-VanWertz, Gabriel, Offenberg, John H., Lewandowski, Michael, Kleindienst, Tadeusz E., Beaver, Melinda R., Holder, Amara L., Lonneman, William A., Docherty, Kenneth S., Jaoui, Mohammed, Pye, Havala O. T., Hu, Weiwei, Day, Douglas A., Campuzano-Jost, Pedro, Jimenez, Jose L., Guo, Hongyu, Weber, Rodney J., de Gouw, Joost, Koss, Abigail R., Edgerton, Eric S., Brune, William, Mohr, Claudia, Lopez-Hilfiker, Felipe D., Lutz, Anna, Kreisberg, Nathan M., Spielman, Steve R., Hering, Susanne V., Wilson, Kevin R., Thornton, Joel A., and Goldstein, Allen H.. Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States. United States: N. p., Web. doi:10.1073/pnas.1717513115.
Zhang, Haofei, Yee, Lindsay D., Lee, Ben H., Curtis, Michael P., Worton, David R., Isaacman-VanWertz, Gabriel, Offenberg, John H., Lewandowski, Michael, Kleindienst, Tadeusz E., Beaver, Melinda R., Holder, Amara L., Lonneman, William A., Docherty, Kenneth S., Jaoui, Mohammed, Pye, Havala O. T., Hu, Weiwei, Day, Douglas A., Campuzano-Jost, Pedro, Jimenez, Jose L., Guo, Hongyu, Weber, Rodney J., de Gouw, Joost, Koss, Abigail R., Edgerton, Eric S., Brune, William, Mohr, Claudia, Lopez-Hilfiker, Felipe D., Lutz, Anna, Kreisberg, Nathan M., Spielman, Steve R., Hering, Susanne V., Wilson, Kevin R., Thornton, Joel A., & Goldstein, Allen H.. Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States. United States. doi:10.1073/pnas.1717513115.
Zhang, Haofei, Yee, Lindsay D., Lee, Ben H., Curtis, Michael P., Worton, David R., Isaacman-VanWertz, Gabriel, Offenberg, John H., Lewandowski, Michael, Kleindienst, Tadeusz E., Beaver, Melinda R., Holder, Amara L., Lonneman, William A., Docherty, Kenneth S., Jaoui, Mohammed, Pye, Havala O. T., Hu, Weiwei, Day, Douglas A., Campuzano-Jost, Pedro, Jimenez, Jose L., Guo, Hongyu, Weber, Rodney J., de Gouw, Joost, Koss, Abigail R., Edgerton, Eric S., Brune, William, Mohr, Claudia, Lopez-Hilfiker, Felipe D., Lutz, Anna, Kreisberg, Nathan M., Spielman, Steve R., Hering, Susanne V., Wilson, Kevin R., Thornton, Joel A., and Goldstein, Allen H.. 2018. "Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States". United States. doi:10.1073/pnas.1717513115.
@article{osti_1420215,
title = {Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States},
author = {Zhang, Haofei and Yee, Lindsay D. and Lee, Ben H. and Curtis, Michael P. and Worton, David R. and Isaacman-VanWertz, Gabriel and Offenberg, John H. and Lewandowski, Michael and Kleindienst, Tadeusz E. and Beaver, Melinda R. and Holder, Amara L. and Lonneman, William A. and Docherty, Kenneth S. and Jaoui, Mohammed and Pye, Havala O. T. and Hu, Weiwei and Day, Douglas A. and Campuzano-Jost, Pedro and Jimenez, Jose L. and Guo, Hongyu and Weber, Rodney J. and de Gouw, Joost and Koss, Abigail R. and Edgerton, Eric S. and Brune, William and Mohr, Claudia and Lopez-Hilfiker, Felipe D. and Lutz, Anna and Kreisberg, Nathan M. and Spielman, Steve R. and Hering, Susanne V. and Wilson, Kevin R. and Thornton, Joel A. and Goldstein, Allen H.},
abstractNote = {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.},
doi = {10.1073/pnas.1717513115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 9,
volume = 115,
place = {United States},
year = {2018},
month = {2}
}