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Discussion papers
https://doi.org/10.5194/acp-2019-840
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-840
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 26 Sep 2019

Submitted as: research article | 26 Sep 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Aerosol pH and liquid water content determine when particulate matter is sensitive to ammonia and nitrate availability

Athanasios Nenes1,2, Spyros N. Pandis1,3, Rodney J. Weber4, and Armistead Russell5 Athanasios Nenes et al.
  • 1Institute for Chemical Engineering Sciences, Foundation for Research and Technology Hellas, Patras, GR-26504, Greece
  • 2School of Architecture, Civil & Environmental Engineering, Ecole polytechnique fédérale de Lausanne, CH-1015, Lausanne, Switzerland
  • 3Department of Chemical Engineering, University of Patras, GR-26504, Greece
  • 4School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA
  • 5School of Civil & Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA

Abstract. Nitrogen oxides (NOx) and ammonia (NH3) from anthropogenic and biogenic emissions are central contributors to particulate matter (PM) concentrations worldwide. The response of PM to changes in the emissions of both compounds is typically studied on a case-by-case basis, owing in part to the complex thermodynamic interactions of these aerosol precursors with other PM constituents. Here we present a simple but thermodynamically consistent approach that expresses the chemical domains of sensitivity of aerosol particulate matter to NH3 and HNO3 availability in terms of aerosol pH and liquid water content. From our analysis, four policy-relevant regimes emerge in terms of sensitivity: (i) NH3-dominated, (ii) HNO3-dominated, (iii) combined NH3 and HNO3 sensitive, and, (iv) a domain where neither NH3 and HNO3 are important for PM levels (but only nonvolatile precursors such as NVCs and sulfate). When this framework is applied to ambient measurements or predictions of PM and gaseous precursors, the chemical regime of PM sensitivity to NH3 and HNO3 availability is directly determined. The use of these regimes allows novel insights and is an important tool to evaluate chemical transport models. With this extended understanding, aerosol pH and associated liquid water content naturally emerge as previously ignored state parameters that drive PM formation.

Athanasios Nenes et al.
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Athanasios Nenes et al.
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Short summary
Here we show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid.
Here we show that aerosol acidity (pH) and liquid water content naturally emerge as previously...
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