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Growth kinetics and size distribution dynamics of viscous secondary organic aerosol

Zaveri, Rahul A. and Shilling, John E. and Zelenyuk, Alla and Liu, Jiumeng and Bell, David M. and D'Ambro, Emma L. and Gaston, Cassandra J. and Thornton, Joel A. and Laskin, Alexander and Lin, Peng and Wilson, Jacqueline M. and Easter, Richard C. and Wang, Jian and Bertram, Allan K. and Martin, Scot T. and Seinfeld, John H. and Worsnop, Douglas R. (2018) Growth kinetics and size distribution dynamics of viscous secondary organic aerosol. Environmental Science and Technology, 52 (3). pp. 1191-1199. ISSN 0013-936X. doi:10.1021/acs.est.7b04623.

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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. Here, 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.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Zaveri, Rahul A.0000-0001-9874-8807
Shilling, John E.0000-0002-3728-0195
Zelenyuk, Alla0000-0002-0674-0910
Thornton, Joel A.0000-0002-5098-4867
Laskin, Alexander0000-0002-7836-8417
Easter, Richard C.0000-0002-8602-1464
Seinfeld, John H.0000-0003-1344-4068
Worsnop, Douglas R.0000-0002-8928-8017
Additional Information:© 2017 American Chemical Society. Received: September 7, 2017; Revised: December 4, 2017; Accepted: December 15, 2017; Published: December 15, 2017. This research was supported by the Office of Science of the U.S. Department of Energy (DOE) as part of the Atmospheric System Research program and by the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL). PNNL is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. Data used in this work are available from the corresponding author ( The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC05-76RL01830
Subject Keywords:Biogenic secondary organic aerosol, gas-particle partitioning, aerosol dynamics, semisolid phase state, viscosity, bulk diffusivity
Issue or Number:3
Record Number:CaltechAUTHORS:20171219-095249096
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Official Citation:Growth Kinetics and Size Distribution Dynamics of Viscous Secondary Organic Aerosol. Rahul A. Zaveri, John E. Shilling, Alla Zelenyuk, Jiumeng Liu, David M. Bell, Emma L. D’Ambro, Cassandra J. Gaston, Joel A. Thornton, Alexander Laskin, Peng Lin, Jacqueline Wilson, Richard C. Easter, Jian Wang, Allan K. Bertram, Scot T. Martin, John H. Seinfeld, and Douglas R. Worsnop. Environmental Science & Technology 2018 52 (3), 1191-1199 DOI: 10.1021/acs.est.7b04623
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:83960
Deposited By: Tony Diaz
Deposited On:19 Dec 2017 19:18
Last Modified:15 Nov 2021 20:15

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