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Title: Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling

Abstract

Here, oxidation flow reactors (OFRs) allow the concentration of a given atmospheric oxidant to be increased beyond ambient levels in order to study secondary organic aerosol (SOA) formation and aging over varying periods of equivalent aging by that oxidant. Previous studies have used these reactors to determine the bulk OA mass and chemical evolution. To our knowledge, no OFR study has focused on the interpretation of the evolving aerosol size distributions. In this study, we use size-distribution measurements of the OFR and an aerosol microphysics model to learn about size-dependent processes in the OFR. Specifically, we use OFR exposures between 0.09 and 0.9 equivalent days of OH aging from the 2011 BEACHON-RoMBAS and GoAmazon2014/5 field campaigns. We use simulations in the TOMAS (TwO-Moment Aerosol Sectional) microphysics box model to constrain the following parameters in the OFR: (1) the rate constant of gas-phase functionalization reactions of organic compounds with OH, (2) the rate constant of gas-phase fragmentation reactions of organic compounds with OH, (3) the reactive uptake coefficient for heterogeneous fragmentation reactions with OH, (4) the nucleation rate constants for three different nucleation schemes, and (5) an effective accommodation coefficient that accounts for possible particle diffusion limitations of particles larger thanmore » 60nm in diameter.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [1]; ORCiD logo [4];  [5]; ORCiD logo [4];  [6];  [7]; ORCiD logo [8];  [9]; ORCiD logo [10]; ORCiD logo [8];  [11];  [12];  [13]; ORCiD logo [4]; ORCiD logo [11]; ORCiD logo [11]; ORCiD logo [4] more »; ORCiD logo [1] « less
  1. Colorado State Univ., Fort Collins, CO (United States)
  2. Univ. of Colorado, Boulder, CO (United States); Univ. of Washington, Seattle, WA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Univ. of Colorado, Boulder, CO (United States)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Aerodyne Research, Inc., Billerica, MA (United States)
  6. Harvard Univ., Cambridge, MA (United States)
  7. Univ. of California, Irvine, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  8. Univ. of Innsbruck, Innsbruck (Austria)
  9. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  10. Univ. of Innsbruck, Innsbruck (Austria); Helmholtz Zentrum Munchen, Munich (Germany)
  11. Univ. of California, Irvine, CA (United States)
  12. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  13. National Center for Atmospheric Research, Boulder, CO (United States); National Institute of Environmental Research (NIER), Incheon (Republic of Korea)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1468955
Grant/Contract Number:  
AC05-76RL01830; SC0016559; NA17OAR430001; NA10OAR4310106; 83587701-0; L518-N20
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 16; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hodshire, Anna L., Palm, Brett B., Alexander, M. Lizabeth, Bian, Qijing, Campuzano-Jost, Pedro, Cross, Eben S., Day, Douglas A., de Sá, Suzane S., Guenther, Alex B., Hansel, Armin, Hunter, James F., Jud, Werner, Karl, Thomas, Kim, Saewung, Kroll, Jesse H., Park, Jeong -Hoo, Peng, Zhe, Seco, Roger, Smith, James N., Jimenez, Jose L., and Pierce, Jeffrey R. Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling. United States: N. p., 2018. Web. doi:10.5194/acp-18-12433-2018.
Hodshire, Anna L., Palm, Brett B., Alexander, M. Lizabeth, Bian, Qijing, Campuzano-Jost, Pedro, Cross, Eben S., Day, Douglas A., de Sá, Suzane S., Guenther, Alex B., Hansel, Armin, Hunter, James F., Jud, Werner, Karl, Thomas, Kim, Saewung, Kroll, Jesse H., Park, Jeong -Hoo, Peng, Zhe, Seco, Roger, Smith, James N., Jimenez, Jose L., & Pierce, Jeffrey R. Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling. United States. doi:10.5194/acp-18-12433-2018.
Hodshire, Anna L., Palm, Brett B., Alexander, M. Lizabeth, Bian, Qijing, Campuzano-Jost, Pedro, Cross, Eben S., Day, Douglas A., de Sá, Suzane S., Guenther, Alex B., Hansel, Armin, Hunter, James F., Jud, Werner, Karl, Thomas, Kim, Saewung, Kroll, Jesse H., Park, Jeong -Hoo, Peng, Zhe, Seco, Roger, Smith, James N., Jimenez, Jose L., and Pierce, Jeffrey R. Tue . "Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling". United States. doi:10.5194/acp-18-12433-2018. https://www.osti.gov/servlets/purl/1468955.
@article{osti_1468955,
title = {Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling},
author = {Hodshire, Anna L. and Palm, Brett B. and Alexander, M. Lizabeth and Bian, Qijing and Campuzano-Jost, Pedro and Cross, Eben S. and Day, Douglas A. and de Sá, Suzane S. and Guenther, Alex B. and Hansel, Armin and Hunter, James F. and Jud, Werner and Karl, Thomas and Kim, Saewung and Kroll, Jesse H. and Park, Jeong -Hoo and Peng, Zhe and Seco, Roger and Smith, James N. and Jimenez, Jose L. and Pierce, Jeffrey R.},
abstractNote = {Here, oxidation flow reactors (OFRs) allow the concentration of a given atmospheric oxidant to be increased beyond ambient levels in order to study secondary organic aerosol (SOA) formation and aging over varying periods of equivalent aging by that oxidant. Previous studies have used these reactors to determine the bulk OA mass and chemical evolution. To our knowledge, no OFR study has focused on the interpretation of the evolving aerosol size distributions. In this study, we use size-distribution measurements of the OFR and an aerosol microphysics model to learn about size-dependent processes in the OFR. Specifically, we use OFR exposures between 0.09 and 0.9 equivalent days of OH aging from the 2011 BEACHON-RoMBAS and GoAmazon2014/5 field campaigns. We use simulations in the TOMAS (TwO-Moment Aerosol Sectional) microphysics box model to constrain the following parameters in the OFR: (1) the rate constant of gas-phase functionalization reactions of organic compounds with OH, (2) the rate constant of gas-phase fragmentation reactions of organic compounds with OH, (3) the reactive uptake coefficient for heterogeneous fragmentation reactions with OH, (4) the nucleation rate constants for three different nucleation schemes, and (5) an effective accommodation coefficient that accounts for possible particle diffusion limitations of particles larger than 60nm in diameter.},
doi = {10.5194/acp-18-12433-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 16,
volume = 18,
place = {United States},
year = {2018},
month = {8}
}

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