Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility
Abstract
Aerosol particles strongly influence global climate by modifying the properties of clouds. An accurate assessment of the aerosol impact on climate requires knowledge of the concentration of cloud condensation nuclei (CCN), a subset of aerosol particles that can activate and form cloud droplets in the atmosphere. Atmospheric particles typically consist of a myriad of organic species, which frequently dominate the particle composition. As a result, CCN concentration is often a strong function of the hygroscopicity of organics in the particles. Earlier studies showed organic hygroscopicity increases nearly linearly with oxidation level. Such increase of hygroscopicity is conventionally attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for the majority of secondary organic aerosols (SOA), essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility, but is dictated mainly by the molecular weight of organic species. Instead of increased water solubility as previously thought, the increase of the organic hygroscopicity with oxidation level is largely because (1) SOA formed from smaller precursor molecules tend to be more oxidized and have lower average molecular weight and (2) during oxidation, fragmentationmore »
- Authors:
-
[2];
[2];
[3];
[2];
[2];
[1]
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- North Carolina State Univ., Raleigh, NC (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1483555
- Report Number(s):
- BNL-209494-2018-JAAM
Journal ID: ISSN 1680-7375
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Atmospheric Chemistry and Physics Discussions (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics Discussions (Online); Journal Volume: 19; Journal Issue: 2; Journal ID: ISSN 1680-7375
- Publisher:
- European Geosciences Union
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
Wang, Jian, Shilling, John E., Liu, Jiumeng, Zelenyuk, Alla, Bell, David M., Petters, Markus, Thalman, Ryan, Mei, Fan, Zaveri, Rahul A., and Zheng, Guangjie. Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility. United States: N. p., 2018.
Web. doi:10.5194/acp-2018-715.
Wang, Jian, Shilling, John E., Liu, Jiumeng, Zelenyuk, Alla, Bell, David M., Petters, Markus, Thalman, Ryan, Mei, Fan, Zaveri, Rahul A., & Zheng, Guangjie. Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility. United States. https://doi.org/10.5194/acp-2018-715
Wang, Jian, Shilling, John E., Liu, Jiumeng, Zelenyuk, Alla, Bell, David M., Petters, Markus, Thalman, Ryan, Mei, Fan, Zaveri, Rahul A., and Zheng, Guangjie. Tue .
"Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility". United States. https://doi.org/10.5194/acp-2018-715. https://www.osti.gov/servlets/purl/1483555.
@article{osti_1483555,
title = {Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility},
author = {Wang, Jian and Shilling, John E. and Liu, Jiumeng and Zelenyuk, Alla and Bell, David M. and Petters, Markus and Thalman, Ryan and Mei, Fan and Zaveri, Rahul A. and Zheng, Guangjie},
abstractNote = {Aerosol particles strongly influence global climate by modifying the properties of clouds. An accurate assessment of the aerosol impact on climate requires knowledge of the concentration of cloud condensation nuclei (CCN), a subset of aerosol particles that can activate and form cloud droplets in the atmosphere. Atmospheric particles typically consist of a myriad of organic species, which frequently dominate the particle composition. As a result, CCN concentration is often a strong function of the hygroscopicity of organics in the particles. Earlier studies showed organic hygroscopicity increases nearly linearly with oxidation level. Such increase of hygroscopicity is conventionally attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for the majority of secondary organic aerosols (SOA), essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility, but is dictated mainly by the molecular weight of organic species. Instead of increased water solubility as previously thought, the increase of the organic hygroscopicity with oxidation level is largely because (1) SOA formed from smaller precursor molecules tend to be more oxidized and have lower average molecular weight and (2) during oxidation, fragmentation reactions reduce average organic molecule weight, leading to increased hygroscopicity. A simple model of organic hygroscopicity based on molecular weight, oxidation level, and volatility is developed, and it successfully reproduces the variation of SOA hygroscopicity with oxidation level observed in the laboratory and field studies.},
doi = {10.5194/acp-2018-715},
journal = {Atmospheric Chemistry and Physics Discussions (Online)},
number = 2,
volume = 19,
place = {United States},
year = {Tue Jul 24 00:00:00 EDT 2018},
month = {Tue Jul 24 00:00:00 EDT 2018}
}
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Table 1: The molecular formula, molecular weight, density, and intrinsic organic hygroscopicity derived using Eq. 2 for major monoterpene SOA products. The density was calculated from O:C and O:H values (Kuwata et al., 2012).
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Surface tension prevails over solute effect in organic-influenced cloud droplet activation
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Identification of Polymers as Major Components of Atmospheric Organic Aerosols
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Cloud droplet activation of mixed organic-sulfate particles produced by the photooxidation of isoprene
journal, January 2010
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The role of surfactants in Köhler theory reconsidered
journal, January 2004
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journal, January 2006
- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics Discussions, Vol. 6, Issue 5
SIMPOL.1: A simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds
journal, January 2007
- Pankow, J. F.; Asher, W. E.
- Atmospheric Chemistry and Physics Discussions, Vol. 7, Issue 4
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions
journal, January 2012
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