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Title: Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

Abstract

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3];  [4];  [1];  [5]; ORCiD logo [6]; ORCiD logo [7];  [8];  [9];  [10]; ORCiD logo [11];  [12]; ORCiD logo [13];  [14]; ORCiD logo [15];  [16];  [17]; ORCiD logo [18] more »; ORCiD logo [19];  [16]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [20];  [21]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1] « less
  1. Stockholm Univ. (Sweden). Department of Environmental Science and Analytical Chemistry (ACES) and Bolin Centre for Climate research
  2. University of Eastern Finland, Kuopio (Finland). Department of Applied Physics
  3. McGill Univ., Montreal, QC (Canada). Department of Atmospheric and Oceanic Sciences
  4. Chonbuk National University, Jeonju (Korea). Department of Earth and Environmental Sciences; Univ. of British Columbia, Vancouver, BC (Canada). Department of Chemistry
  5. Norwegian Meteorological Institute, Oslo (Norway)
  6. University of Eastern Finland, Kuopio (Finland). Department of Applied Physics; Rice Univ., Houston, TX (United States). Department of Civil and Environmental Engineering
  7. Univ. of Colorado, Boulder, CO (United States). Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry
  8. Texas A & M Univ., College Station, TX (United States). Department of Atmospheric Sciences
  9. Aerodyne Research Inc., Billerica, MA (United States); Boston College, Chestnut Hill, MA (United States). Department of Chemistry
  10. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
  11. Georgia Inst. of Technology, Atlanta, GA (United States). School of Earth and Atmospheric Sciences ; Institute for Environmental Research and Sustainable Development, National Observatory of Athens, Palea Penteli (Greece)
  12. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences
  13. Department of Environmental Science and Analytical Chemistry (ACES) and Bolin Centre for Climate research, Stockholm University, Stockholm Sweden
  14. Univ. of Helsinki (Finland). Department of Physics
  15. Univ. of Manchester (United Kingdom). School of Earth and Environmental Sciences
  16. Boston College, Chestnut Hill, MA (United States). Department of Chemistry
  17. Aerodyne Research Inc., Billerica, MA (United States)
  18. Stockholm Univ. (Sweden). Department of Meteorology
  19. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences; Institute for Environmental Research and Sustainable Development, National Observatory of Athens, Palea Penteli (Greece); Institute of Chemical Engineering Sciences, Foundation for Research and Technology-Hellas, Patras (Greece)
  20. Univ. of Manchester (United Kingdom). School of Earth and Environmental Sciences and National Centre for Atmospheric Science (NCAS)
  21. Univ. of British Columbia, Vancouver, BC (Canada). Department of Chemistry
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1358118
Alternate Identifier(s):
OSTI ID: 1377937; OSTI ID: 1429324
Grant/Contract Number:  
SC0016559; SC0012792
Resource Type:
Journal Article: Published Article
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 44; Journal Issue: 10; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; atmospheric aerosol; secondary organic aerosol; hygroscopicity; aerosol-water interactions; aerosol-climate interactions

Citation Formats

Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge, D. G., Kirkevag, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petaja, T., Percival, C., Davidovits, P., Worsnop, D. R., Ekman, A. M. L., Nenes, A., Martin, S., Jimenez, J. L., Collins, D. R., Topping, D. O., Bertram, A. K., Zuend, A., Virtanen, A., and Riipinen, I. Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate. United States: N. p., 2017. Web. doi:10.1002/2017GL073056.
Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge, D. G., Kirkevag, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petaja, T., Percival, C., Davidovits, P., Worsnop, D. R., Ekman, A. M. L., Nenes, A., Martin, S., Jimenez, J. L., Collins, D. R., Topping, D. O., Bertram, A. K., Zuend, A., Virtanen, A., & Riipinen, I. Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate. United States. doi:10.1002/2017GL073056.
Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge, D. G., Kirkevag, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petaja, T., Percival, C., Davidovits, P., Worsnop, D. R., Ekman, A. M. L., Nenes, A., Martin, S., Jimenez, J. L., Collins, D. R., Topping, D. O., Bertram, A. K., Zuend, A., Virtanen, A., and Riipinen, I. Fri . "Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate". United States. doi:10.1002/2017GL073056.
@article{osti_1358118,
title = {Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate},
author = {Rastak, N. and Pajunoja, A. and Acosta Navarro, J. C. and Ma, J. and Song, M. and Partridge, D. G. and Kirkevag, A. and Leong, Y. and Hu, W. W. and Taylor, N. F. and Lambe, A. and Cerully, K. and Bougiatioti, A. and Liu, P. and Krejci, R. and Petaja, T. and Percival, C. and Davidovits, P. and Worsnop, D. R. and Ekman, A. M. L. and Nenes, A. and Martin, S. and Jimenez, J. L. and Collins, D. R. and Topping, D. O. and Bertram, A. K. and Zuend, A. and Virtanen, A. and Riipinen, I.},
abstractNote = {A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.},
doi = {10.1002/2017GL073056},
journal = {Geophysical Research Letters},
number = 10,
volume = 44,
place = {United States},
year = {Fri Apr 28 00:00:00 EDT 2017},
month = {Fri Apr 28 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/2017GL073056

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Cited by: 7 works
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