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Vapors Are Lost to Walls, Not to Particles on the Wall: Artifact-Corrected Parameters from Chamber Experiments and Implications for Global Secondary Organic Aerosol

Bilsback, Kelsey R. and He, Yicong and Cappa, Christopher D. and Chang, Rachel Ying-Wen and Croft, Betty and Martin, Randall V. and Ng, Nga Lee and Seinfeld, John H. and Pierce, Jeffrey R. and Jathar, Shantanu H. (2023) Vapors Are Lost to Walls, Not to Particles on the Wall: Artifact-Corrected Parameters from Chamber Experiments and Implications for Global Secondary Organic Aerosol. Environmental Science and Technology, 57 (1). pp. 53-63. ISSN 0013-936X. doi:10.1021/acs.est.2c03967.

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Atmospheric models of secondary organic aerosol (OA) (SOA) typically rely on parameters derived from environmental chambers. Chambers are subject to experimental artifacts, including losses of (1) particles to the walls (PWL), (2) vapors to the particles on the wall (V2PWL), and (3) vapors to the wall directly (VWL). We present a method for deriving artifact-corrected SOA parameters and translating these to volatility basis set (VBS) parameters for use in chemical transport models (CTMs). Our process involves combining a box model that accounts for chamber artifacts (Statistical Oxidation Model with a TwO-Moment Aerosol Sectional model (SOM-TOMAS)) with a pseudo-atmospheric simulation to develop VBS parameters that are fit across a range of OA mass concentrations. We found that VWL led to the highest percentage change in chamber SOA mass yields (high NOₓ: 36–680%; low NOₓ: 55–250%), followed by PWL (high NOₓ: 8–39%; low NOₓ: 10–37%), while the effects of V2PWL are negligible. In contrast to earlier work that assumed that V2PWL was a meaningful loss pathway, we show that V2PWL is an unimportant SOA loss pathway and can be ignored when analyzing chamber data. Using our updated VBS parameters, we found that not accounting for VWL may lead surface-level OA to be underestimated by 24% (0.25 μg m⁻³) as a global average or up to 130% (9.0 μg m⁻³) in regions of high biogenic or anthropogenic activity. Finally, we found that accurately accounting for PWL and VWL improves model-measurement agreement for fine mode aerosol mass concentrations (PM₂.₅) in the GEOS-Chem model.

Item Type:Article
Related URLs:
URLURL TypeDescription
Bilsback, Kelsey R.0000-0002-5996-1522
He, Yicong0000-0001-8969-1167
Cappa, Christopher D.0000-0002-3528-3368
Chang, Rachel Ying-Wen0000-0003-2337-098X
Croft, Betty0000-0002-7009-1767
Martin, Randall V.0000-0003-2632-8402
Ng, Nga Lee0000-0001-8460-4765
Seinfeld, John H.0000-0003-1344-4068
Pierce, Jeffrey R.0000-0002-4241-838X
Jathar, Shantanu H.0000-0003-4106-2358
Additional Information:Research funding was provided by the Department of Energy’s Office of Science (DE-SC0017975) and National Oceanic and Atmospheric Administration (NA17OAR4310003 and NA17OAR4310001). This publication was partly developed under Assistance Agreement no. R840008 awarded by the U.S. Environmental Protection Agency to Colorado State University. It has not been formally reviewed by EPA. The views expressed in this document are solely those of the authors and do not necessarily reflect those of the Agency. EPA does not endorse any products or commercial services mentioned in this publication. C.D.C. was supported in part by the California Air Resources Board, contract 18RD009. We thank Prof. Arthur W. H. Chan for sharing PWL and naphthalene SOA data and providing useful comments on the manuscript.
Funding AgencyGrant Number
California Air Resources Board18RD009
National Oceanic and Atmospheric Administration (NOAA)NA17OAR4310001
National Oceanic and Atmospheric Administration (NOAA)NA17OAR4310003
Environmental Protection Agency (EPA)R840008
Department of Energy (DOE)DE-SC0017975
Issue or Number:1
Record Number:CaltechAUTHORS:20230125-515005200.30
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118948
Deposited By: Research Services Depository
Deposited On:24 Feb 2023 18:07
Last Modified:24 Feb 2023 18:07

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