Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility

Wang, Jian; Shilling, John E.; Liu, Jiumeng; Zelenyuk, Alla; Bell, David M.; Petters, Markus; Thalman, Ryan; Mei, Fan; Zaveri, Rahul A.; Zheng, Guangjie

doi:10.5194/acp-2018-715

Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility

Journal Article · Tue Jul 24 00:00:00 EDT 2018 · Atmospheric Chemistry and Physics Discussions (Online)

DOI:https://doi.org/10.5194/acp-2018-715· OSTI ID:1483555

Wang, Jian ^[1]; ^[2]; ^[2]; Zelenyuk, Alla ^[2]; Bell, David M. ^[2]; ^[3]; Thalman, Ryan ^[1]; ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: SC0012704

OSTI ID:: 1483555

Report Number(s):: BNL--209494-2018-JAAM

Journal Information:: Atmospheric Chemistry and Physics Discussions (Online), Journal Name: Atmospheric Chemistry and Physics Discussions (Online) Journal Issue: 2 Vol. 19; ISSN 1680-7375

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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