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:
-
more »
- Department of Environmental Science and Analytical Chemistry (ACES) and Bolin Centre for Climate research, Stockholm University, Stockholm Sweden
- Department of Applied Physics, University of Eastern Finland, Kuopio Finland
- Department of Atmospheric and Oceanic Sciences, McGill University, Montreal Quebec Canada
- Department of Earth and Environmental Sciences, Chonbuk National University, Jeonju Republic of Korea, Department of Chemistry, University of British Columbia, Vancouver British Columbia Canada
- Norwegian Meteorological Institute, Oslo Norway
- Department of Applied Physics, University of Eastern Finland, Kuopio Finland, Department of Civil and Environmental Engineering, Rice University, Houston Texas USA
- Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder Colorado USA, Department of Chemistry and Biochemistry, University of Colorado, Boudler Colorado USA
- Department of Atmospheric Sciences, Texas A&M University, College Station Texas USA
- Aerodyne Research Inc., Billerica Massachusetts USA, Department of Chemistry, Boston College, Chestnut Hill Massachusetts USA
- School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta Georgia USA
- School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA, Institute for Environmental Research and Sustainable Development, National Observatory of Athens, Palea Penteli Greece
- School of Engineering and Applied Sciences, Harvard University, Cambridge Massachusetts USA
- Department of Physics, University of Helsinki, Helsinki Finland
- School of Earth and Environmental Sciences, University of Manchester, Manchester UK
- Department of Chemistry, Boston College, Chestnut Hill Massachusetts USA
- Aerodyne Research Inc., Billerica Massachusetts USA
- Department of Meteorology, Stockholm University, Stockholm Sweden
- School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta Georgia USA, School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA, 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
- School of Earth and Environmental Sciences, University of Manchester, Manchester UK, National Centre for Atmospheric Science (NCAS), University of Manchester, Manchester UK
- Department of Chemistry, University of British Columbia, Vancouver British Columbia Canada
- Publication Date:
- Research Org.:
- Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1358118
- Alternate Identifier(s):
- OSTI ID: 1377937; OSTI ID: 1429324
- Grant/Contract Number:
- SC0016559; SC0012792
- Resource Type:
- Published Article
- Journal Name:
- Geophysical Research Letters
- Additional Journal Information:
- Journal Name: Geophysical Research Letters; 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., Kirkevåg, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, 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., Kirkevåg, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, 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. https://doi.org/10.1002/2017GL073056
Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge, D. G., Kirkevåg, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, 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. Sun .
"Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate". United States. https://doi.org/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 Kirkevåg, 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 Petäjä, 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 = ,
volume = ,
place = {United States},
year = {Sun May 21 00:00:00 EDT 2017},
month = {Sun May 21 00:00:00 EDT 2017}
}
https://doi.org/10.1002/2017GL073056
Web of Science
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