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Title: Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A

Abstract

The GoAmazon 2014/5 field campaign took place in Manaus, Brazil, and allowed the investigation of the interaction between background-level biogenic air masses and anthropogenic plumes. We present in this work a box model built to simulate the impact of urban chemistry on biogenic secondary organic aerosol (SOA) formation and composition. An organic chemistry mechanism is generated with the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to simulate the explicit oxidation of biogenic and anthropogenic compounds. A parameterization is also included to account for the reactive uptake of isoprene oxidation products on aqueous particles. The biogenic emissions estimated from existing emission inventories had to be reduced to match measurements. The model is able to reproduce ozone and NOx for clean and polluted situations. The explicit model is able to reproduce background case SOA mass concentrations but does not capture the enhancement observed in the urban plume. The oxidation of biogenic compounds is the major contributor to SOA mass. A volatility basis set (VBS) parameterization applied to the same cases obtains better results than GECKO-A for predicting SOA mass in the box model. The explicit mechanism may be missing SOA-formation processes related to the oxidation of monoterpenesmore » that could be implicitly accounted for in the VBS parameterization.« less

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [3];  [4];  [4];  [5]; ORCiD logo [6]; ORCiD logo [1];  [7]; ORCiD logo [8];  [1]; ORCiD logo [6]; ORCiD logo [9]; ORCiD logo [9];  [1]
  1. National Center for Atmospheric Research, Boulder, CO (United States)
  2. National Center for Atmospheric Research, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  3. Univ. of Sao Paulo (Brazil)
  4. Centre National de la Recherche Scientifique (CNRS) (France); Univ. Paris-Est-Créteil (France); Univ. de Paris (France)
  5. Case Western Reserve Univ., Cleveland, OH (United States)
  6. Univ. of Colorado, Boulder, CO (United States)
  7. Harvard Univ., Cambridge, MA (United States)
  8. National Inst. for Amazonian Research, Manaus, AM (Brazil); Amazonas State Univ., Manaus, AM (Brazil)
  9. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
National Science Foundation (NSF); USEPA; USDOE Office of Science (SC), Biological and Environmental Research (BER); Brazilian National Council for Scientific and Technological Development (CNPq)
OSTI Identifier:
1639167
Report Number(s):
PNNL-SA-148940
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
AC05-76RL01830; SC0016331
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 20; Journal Issue: 10; 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

Mouchel-Vallon, Camille, Lee-Taylor, Julia, Hodzic, Alma, Artaxo, Paulo, Aumont, Bernard, Camredon, Marie, Gurarie, David, Jimenez, Jose-Luis, Lenschow, Donald H., Martin, Scot T., Nascimento, Janaina, Orlando, John J., Palm, Brett B., Shilling, John E., Shrivastava, Manish Kumar B., and Madronich, Sasha. Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A. United States: N. p., 2020. Web. https://doi.org/10.5194/acp-20-5995-2020.
Mouchel-Vallon, Camille, Lee-Taylor, Julia, Hodzic, Alma, Artaxo, Paulo, Aumont, Bernard, Camredon, Marie, Gurarie, David, Jimenez, Jose-Luis, Lenschow, Donald H., Martin, Scot T., Nascimento, Janaina, Orlando, John J., Palm, Brett B., Shilling, John E., Shrivastava, Manish Kumar B., & Madronich, Sasha. Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A. United States. https://doi.org/10.5194/acp-20-5995-2020
Mouchel-Vallon, Camille, Lee-Taylor, Julia, Hodzic, Alma, Artaxo, Paulo, Aumont, Bernard, Camredon, Marie, Gurarie, David, Jimenez, Jose-Luis, Lenschow, Donald H., Martin, Scot T., Nascimento, Janaina, Orlando, John J., Palm, Brett B., Shilling, John E., Shrivastava, Manish Kumar B., and Madronich, Sasha. Wed . "Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A". United States. https://doi.org/10.5194/acp-20-5995-2020. https://www.osti.gov/servlets/purl/1639167.
@article{osti_1639167,
title = {Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A},
author = {Mouchel-Vallon, Camille and Lee-Taylor, Julia and Hodzic, Alma and Artaxo, Paulo and Aumont, Bernard and Camredon, Marie and Gurarie, David and Jimenez, Jose-Luis and Lenschow, Donald H. and Martin, Scot T. and Nascimento, Janaina and Orlando, John J. and Palm, Brett B. and Shilling, John E. and Shrivastava, Manish Kumar B. and Madronich, Sasha},
abstractNote = {The GoAmazon 2014/5 field campaign took place in Manaus, Brazil, and allowed the investigation of the interaction between background-level biogenic air masses and anthropogenic plumes. We present in this work a box model built to simulate the impact of urban chemistry on biogenic secondary organic aerosol (SOA) formation and composition. An organic chemistry mechanism is generated with the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to simulate the explicit oxidation of biogenic and anthropogenic compounds. A parameterization is also included to account for the reactive uptake of isoprene oxidation products on aqueous particles. The biogenic emissions estimated from existing emission inventories had to be reduced to match measurements. The model is able to reproduce ozone and NOx for clean and polluted situations. The explicit model is able to reproduce background case SOA mass concentrations but does not capture the enhancement observed in the urban plume. The oxidation of biogenic compounds is the major contributor to SOA mass. A volatility basis set (VBS) parameterization applied to the same cases obtains better results than GECKO-A for predicting SOA mass in the box model. The explicit mechanism may be missing SOA-formation processes related to the oxidation of monoterpenes that could be implicitly accounted for in the VBS parameterization.},
doi = {10.5194/acp-20-5995-2020},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 10,
volume = 20,
place = {United States},
year = {2020},
month = {5}
}

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