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A computationally efficient model to represent the chemistry, thermodynamics, and microphysics of secondary organic aerosols (simpleSOM): model development and application to α-pinene SOA

Jathar, Shantanu H. and Cappa, Christopher D. and He, Yicong and Pierce, Jeffrey R. and Chuang, Wayne and Bilsback, Kelsey R. and Seinfeld, John H. and Zaveri, Rahul A. and Shrivastava, Manish (2021) A computationally efficient model to represent the chemistry, thermodynamics, and microphysics of secondary organic aerosols (simpleSOM): model development and application to α-pinene SOA. Environmental Science: Atmospheres, 1 (6). pp. 372-394. ISSN 2634-3606. doi:10.1039/d1ea00014d. https://resolver.caltech.edu/CaltechAUTHORS:20210825-140510722

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Abstract

Secondary organic aerosols (SOA) constitute an important fraction of fine-mode atmospheric aerosol mass. Frameworks used to develop SOA parameters from laboratory experiments and subsequently used to simulate SOA formation in atmospheric models make many simplifying assumptions about the processes that lead to SOA formation in the interest of computational efficiency. These assumptions can limit the ability of the model to predict the mass, composition, and properties of SOA accurately. In this work, we developed a computationally efficient, process-level model named simpleSOM to represent the chemistry, thermodynamic properties, and microphysics of SOA. simpleSOM simulates multigenerational gas-phase chemistry, phase-state-influenced kinetic gas/particle partitioning, heterogeneous chemistry, oligomerization reactions, and vapor losses to the walls of Teflon chambers. As a case study, we used simpleSOM to simulate SOA formation from the photooxidation of α-pinene. This was done to demonstrate the ability of the model to develop parameters that can reproduce environmental chamber data, to highlight the chemical and microphysical processes within simpleSOM, and discuss implications for SOA formation in chambers and in the real atmosphere. SOA parameters developed from experiments performed in the chamber at the California Institute of Technology (Caltech) reproduced observations of SOA mass yield, O : C, and volatility distribution gathered from other experiments. Sensitivity simulations suggested that multigenerational gas-phase aging contributed to nearly half of all SOA and that in the absence of vapor wall losses, SOA production in the Caltech chamber could be nearly 50% higher. Heterogeneous chemistry did not seem to affect SOA formation over the short timescales for oxidation experienced in the chamber experiments. Simulations performed under atmospherically relevant conditions indicated that the SOA mass yields were sensitive to whether and how oligomerization reactions and the particle phase state were represented in the chamber experiment from which the parameters were developed. simpleSOM provides a comprehensive, process-based framework to consistently model the SOA formation and evolution in box and 3D models.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1039/d1ea00014dDOIArticle
https://www.rsc.org/suppdata/d1/ea/d1ea00014d/d1ea00014d1.pdfPublisherSupporting Information
https://icarus.ucdavis.edu/Related ItemIndex of Chamber Atmospheric Research
http://dx.doi.org/10.25675/10217/232634DOIData
https://github.com/ARM-Synergy/simpleSOM_boxmodelRelated ItemCode
ORCID:
AuthorORCID
Jathar, Shantanu H.0000-0003-4106-2358
Cappa, Christopher D.0000-0002-3528-3368
He, Yicong0000-0001-8969-1167
Pierce, Jeffrey R.0000-0002-4241-838X
Bilsback, Kelsey R.0000-0002-5996-1522
Seinfeld, John H.0000-0003-1344-4068
Zaveri, Rahul A.0000-0001-9874-8807
Shrivastava, Manish0000-0002-9053-2400
Additional Information:© 2021 The Author(s). Published by the Royal Society of Chemistry. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Submitted 26 Feb 2021; Accepted 26 May 2021; First published 07 Jun 2021. This work was supported by the U.S. Department of Energy (DOE), Office of Science (DE-SC0017975). RAZ acknowledges support from the U.S. DOE Office of Science as part of the Atmospheric System Research Program at the Pacific Northwest National Laboratory (PNNL). MS was supported by the U.S. DOE, Office of Science, and Office of Biological and Environmental Research through the Early Career Research Program. PNNL is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL0 1830. We thank Dr Benjamin Murphy at the U.S. Environmental Protection Agency for helpful conversations concerning CMAQ. Data availability: Experimental data used in this work are from Dr John Seinfeld’s group at the California Institute of Technology and are now available as part of the Index of Chamber Atmospheric Research in the United States (ICARUS; https://icarus.ucdavis.edu). The latest versions of the IGOR and Fortran models for simpleSOM/simpleSOM-MOSAIC along with the simulation data are archived with Colorado State University Libraries (http://dx.doi.org/10.25675/10217/232634) and Github (https://github.com/ARM-Synergy/simpleSOM_boxmodel). The data from all the figures in the paper are also available with Colorado State University Libraries (http://dx.doi.org/10.25675/10217/232634). Author contributions: SHJ and CDC designed the model framework and overall study. CDC developed the IGOR model and YH and WC updated the model. YH developed the Fortran-Python model and YH and KRB benchmarked this model against the IGOR model. YH performed the simulations and YH and SHJ analyzed the data. JHS provided the experimental data. RAZ, MS, and JRP supported the model development and analysis. KRB helped with archiving the code and model output. SHJ and YH wrote the paper with contributions from all co-authors. There are no conflicts to declare.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0017975
Department of Energy (DOE)DE-AC05-76RL0 1830
Issue or Number:6
DOI:10.1039/d1ea00014d
Record Number:CaltechAUTHORS:20210825-140510722
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210825-140510722
Official Citation:A computationally efficient model to represent the chemistry, thermodynamics, and microphysics of secondary organic aerosols (simpleSOM): model development and application to α-pinene SOA. Environ. Sci.: Atmos., 2021, 1, 372-394; DOI: 10.1039/d1ea00014d
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110407
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:25 Aug 2021 17:32
Last Modified:28 Sep 2021 16:48

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