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Under What Conditions Can Equilibrium Gas–Particle Partitioning Be Expected to Hold in the Atmosphere?

Mai, Huajun and Shiraiwa, Manabu and Flagan, Richard C. and Seinfeld, John H. (2015) Under What Conditions Can Equilibrium Gas–Particle Partitioning Be Expected to Hold in the Atmosphere? Environmental Science and Technology, 49 (19). pp. 11485-11491. ISSN 0013-936X. doi:10.1021/acs.est.5b02587. https://resolver.caltech.edu/CaltechAUTHORS:20150921-111503736

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Abstract

The prevailing treatment of secondary organic aerosol formation in atmospheric models is based on the assumption of instantaneous gas–particle equilibrium for the condensing species, yet compelling experimental evidence indicates that organic aerosols can exhibit the properties of highly viscous, semisolid particles, for which gas–particle equilibrium may be achieved slowly. The approach to gas–particle equilibrium partitioning is controlled by gas-phase diffusion, interfacial transport, and particle-phase diffusion. Here we evaluate the controlling processes and the time scale to achieve gas–particle equilibrium as a function of the volatility of the condensing species, its surface accommodation coefficient, and its particle-phase diffusivity. For particles in the size range of typical atmospheric organic aerosols (∼50–500 nm), the time scale to establish gas–particle equilibrium is generally governed either by interfacial accommodation or particle-phase diffusion. The rate of approach to equilibrium varies, depending on whether the bulk vapor concentration is constant, typical of an open system, or decreasing as a result of condensation into the particles, typical of a closed system.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acs.est.5b02587DOIArticle
http://pubs.acs.org/doi/10.1021/acs.est.5b02587PublisherArticle
ORCID:
AuthorORCID
Mai, Huajun0000-0002-0616-1986
Shiraiwa, Manabu0000-0003-2532-5373
Flagan, Richard C.0000-0001-5690-770X
Seinfeld, John H.0000-0003-1344-4068
Additional Information:© 2015 American Chemical Society. Received: May 27, 2015; Revised: August 25, 2015; Accepted: September 4, 2015; Publication Date (Web): September 4, 2015. This work was supported by National Science Foundation grant AGS-1523500. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
NSFAGS-1523500
Issue or Number:19
DOI:10.1021/acs.est.5b02587
Record Number:CaltechAUTHORS:20150921-111503736
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150921-111503736
Official Citation:Under What Conditions Can Equilibrium Gas–Particle Partitioning Be Expected to Hold in the Atmosphere? Huajun Mai, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld Environmental Science & Technology 2015 49 (19), 11485-11491 DOI: 10.1021/acs.est.5b02587
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:60375
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:21 Sep 2015 18:41
Last Modified:10 Nov 2021 22:33

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