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

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.
Authors:
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
Publication Date:
Report Number(s):
BNL-203207-2018-JAAM; PNNL-SA-128966; BNL-203357-2018-JAAM
Journal ID: ISSN 0013-936X
Grant/Contract Number:
SC0012704; AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 52; Journal Issue: 3; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1424984
Alternate Identifier(s):
OSTI ID: 1426444