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Title: Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter

Abstract

Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1619790
Alternate Identifier(s):
OSTI ID: 1611949
Grant/Contract Number:  
SC0012792
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 9 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Science & Technology - Other Topics

Citation Formats

Liu, Pengfei, Song, Mijung, Zhao, Tianning, Gunthe, Sachin S., Ham, Suhan, He, Yipeng, Qin, Yi Ming, Gong, Zhaoheng, Amorim, Juliana C., Bertram, Allan K., and Martin, Scot T. Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter. United Kingdom: N. p., 2018. Web. doi:10.1038/s41467-018-06622-2.
Liu, Pengfei, Song, Mijung, Zhao, Tianning, Gunthe, Sachin S., Ham, Suhan, He, Yipeng, Qin, Yi Ming, Gong, Zhaoheng, Amorim, Juliana C., Bertram, Allan K., & Martin, Scot T. Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter. United Kingdom. doi:10.1038/s41467-018-06622-2.
Liu, Pengfei, Song, Mijung, Zhao, Tianning, Gunthe, Sachin S., Ham, Suhan, He, Yipeng, Qin, Yi Ming, Gong, Zhaoheng, Amorim, Juliana C., Bertram, Allan K., and Martin, Scot T. Thu . "Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter". United Kingdom. doi:10.1038/s41467-018-06622-2.
@article{osti_1619790,
title = {Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter},
author = {Liu, Pengfei and Song, Mijung and Zhao, Tianning and Gunthe, Sachin S. and Ham, Suhan and He, Yipeng and Qin, Yi Ming and Gong, Zhaoheng and Amorim, Juliana C. and Bertram, Allan K. and Martin, Scot T.},
abstractNote = {Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.},
doi = {10.1038/s41467-018-06622-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1038/s41467-018-06622-2

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Cited by: 13 works
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