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https://doi.org/10.5194/acp-2020-575
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-575
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 24 Jun 2020

Submitted as: research article | 24 Jun 2020

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This preprint is currently under review for the journal ACP.

Long-term observational constraints of organic aerosol dependence on inorganic species in the southeast US

Yiqi Zheng1,2, Joel A. Thornton3, Nga Lee Ng4,5,6, Hansen Cao7, Daven K. Henze7, Erin E. McDuffie8,9, Weiwei Hu10,11, Jose L. Jimenez11, Eloise A. Marais12, Eric Edgerton13, and Jingqiu Mao1,2 Yiqi Zheng et al.
  • 1Geophysical Institute, University of Alaska Fairbanks, Fairbanks, AK, USA
  • 2Department of Chemistry and Biochemistry, University of Alaska Fairbanks, Fairbanks, AK, USA
  • 3Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
  • 4School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
  • 5School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
  • 6School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, USA
  • 7Department of Mechanical Engineering, University of Colorado Boulder, Boulder, CO, USA
  • 8Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada
  • 9Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St Louis, MO, USA
  • 10State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Science (CAS), Guangzhou, China
  • 11Department of Chemistry and CIRES, University of Colorado Boulder, Boulder, CO, USA
  • 12School of Physics and Astronomy, University of Leicester, Leicester, LE1 7RH, UK
  • 13Atmospheric Research & Analysis, Inc., Cary, NC, USA

Abstract. Organic aerosol (OA), with a large biogenic fraction in summertime southeast US, adversely impacts on air quality and human health. Stringent air quality controls have recently reduced anthropogenic pollutants including sulfate, whose impact on OA remains unclear. Three filter measurement networks provide long-term constraints on the sensitivity of OA to changes in inorganic species, including sulfate and ammonia. The 2000–2013 summertime OA decreases by 1.7~1.9 %/year with little month-to-month variability, while sulfate declines rapidly with significant monthly difference in early 2000s. In contrast, modeled OA from a chemical-transport model (GEOS-Chem) decreases by 4.9 %/year with much larger month-to-month variability, largely due to the predominant role of acid-catalyzed reactive uptake of epoxydiols (IEPOX) onto sulfate. The overestimated modeled OA dependence on sulfate can be improved by implementing a coating effect and assuming constant aerosol acidity, suggesting the needs to revisit IEPOX reactive uptake in current models. Our work highlights the importance of secondary OA formation pathways that are weakly dependent on inorganic aerosol in a region that is heavily influenced by both biogenic and anthropogenic emissions.

Yiqi Zheng et al.

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Short summary
This study aims to address a challenge in biosphere-atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities. From 3 surface network observations, we show that OA is weakly dependent on sulfate and aerosol acidity in summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model GEOS-Chem, suggesting the needs to revisit the representation of aqueous-phase secondary OA formation.
This study aims to address a challenge in biosphere-atmosphere interactions: to what extent can...
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