Growth Kinetics and Size Distribution Dynamics of Viscous Secondary Organic Aerosol

Zaveri, Rahul A.; Shilling, John E.; Zelenyuk, Alla; Liu, Jiumeng; Bell, David M.; D’Ambro, Emma L.; Gaston, Cassandra J.; Thornton, Joel A.; Laskin, Alexander; Lin, Peng; Wilson, Jacqueline; Easter, Richard C.; Wang, Jian; Bertram, Allan K.; Martin, Scot T.; Seinfeld, John H.; Worsnop, Douglas R.

doi:10.1021/acs.est.7b04623

Growth Kinetics and Size Distribution Dynamics of Viscous Secondary Organic Aerosol

Journal Article · Fri Dec 15 00:00:00 EST 2017 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b04623· OSTI ID:1424984

^[1]; Shilling, John E. ^[1]; Zelenyuk, Alla ^[2]; Liu, Jiumeng ^[1]; Bell, David M. ^[3]; ^[4]; Gaston, Cassandra J. ^[5]; ^[4]; ^[6]; Lin, Peng ^[6]; Wilson, Jacqueline ^[2]; Easter, Richard C. ^[1]; Wang, Jian ^[7]; Bertram, Allan K. ^[8]; Martin, Scot T. ^[9]; Seinfeld, John H. ^[10]; Worsnop, Douglas R. ^[11]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Div.
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Div.; Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. of Atmospheric Chemistry
Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences and Dept. of Chemistry
Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences; Univ. of Miami, Miami, FL (United States). Rosenstiel School of Marine and Atmospheric Science
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Purdue Univ., West Lafayette, IN (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Environmental & Climate Sciences Dept.
Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS) and Dept. of Earth and Planetary Sciences
California Inst. of Technology (CalTech), Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering and Div. of Engineering and Applied Science
Aerodyne Research, Billerica, MA (United States). Center for Aerosol and Cloud Chemistry

Low bulk diffusivity inside viscous semisolid atmospheric secondary organic aerosol (SOA) can prolong equilibration time scale, but its broader impacts on aerosol growth and size distribution dynamics are poorly understood. In this article, we present quantitative insights into the effects of bulk diffusivity on the growth and evaporation kinetics of SOA formed under dry conditions from photooxidation of isoprene in the presence of a bimodal aerosol consisting of Aitken (ammonium sulfate) and accumulation (isoprene or α-pinene SOA) mode particles. Aerosol composition measurements and evaporation kinetics indicate that isoprene SOA is composed of several semivolatile organic compounds (SVOCs), with some reversibly reacting to form oligomers. Model analysis shows that liquid-like bulk diffusivities can be used to fit the observed evaporation kinetics of accumulation mode particles but fail to explain the growth kinetics of bimodal aerosol by significantly under-predicting the evolution of the Aitken mode. In contrast, the semisolid scenario successfully reproduces both evaporation and growth kinetics, with the interpretation that hindered partitioning of SVOCs into large viscous particles effectively promotes the growth of smaller particles that have shorter diffusion time scales. This effect has important implications for the growth of atmospheric ultrafine particles to climatically active sizes.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830; SC0012704

OSTI ID:: 1424984

Alternate ID(s):: OSTI ID: 1421345
OSTI ID: 1426444

Report Number(s):: BNL--203207-2018-JAAM; BNL--203357-2018-JAAM; PNNL-SA--128966

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 3 Vol. 52; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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