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Title: Growth Kinetics and Size Distribution Dynamics of Viscous Secondary Organic Aerosol

Journal Article · · Environmental Science and Technology
ORCiD logo [1];  [1];  [2];  [1];  [3]; ORCiD logo [4];  [5]; ORCiD logo [4]; ORCiD logo [6];  [6];  [2];  [1];  [7];  [8];  [9];  [10];  [11]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Div.
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Div.; Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. of Atmospheric Chemistry
  4. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences and Dept. of Chemistry
  5. 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
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Purdue Univ., West Lafayette, IN (United States). Dept. of Chemistry
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). Environmental & Climate Sciences Dept.
  8. Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
  9. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS) and Dept. of Earth and Planetary Sciences
  10. California Inst. of Technology (CalTech), Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering and Div. of Engineering and Applied Science
  11. 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. Here, we present quantitative insights into the effects of bulk diffusivity on the growth and evaporation kinetics of SOA formed under dry condi- tions 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.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0012704; AC05-76RL01830
OSTI ID:
1424984
Alternate ID(s):
OSTI ID: 1426444
Report Number(s):
BNL-203207-2018-JAAM; PNNL-SA-128966; BNL-203357-2018-JAAM
Journal Information:
Environmental Science and Technology, Vol. 52, Issue 3; ISSN 0013-936X
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 65 works
Citation information provided by
Web of Science

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Cited By (11)

Comprehensive analysis of particle growth rates from nucleation mode to cloud condensation nuclei in boreal forest journal January 2018
Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility journal January 2019
Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition journal January 2018
Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling journal January 2018
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors journal January 2019
Viscosity of erythritol and erythritol–water particles as a function of water activity: new results and an intercomparison of techniques for measuring the viscosity of particles journal January 2018
Thermal desorption behavior of hemiacetal, acetal, ether, and ester oligomers journal February 2019
Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes–Einstein equation journal January 2019
Modelling the effect of condensed-phase diffusion on the homogeneous nucleation of ice in ultra-viscous particles journal January 2020
Thermal desorption behavior of hemiacetal, acetal, ether, and ester oligomers text January 2019
Thermal Desorption Behavior of Hemiacetal, Acetal, Ether, and Ester Oligomers text January 2019

Figures / Tables (5)


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