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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 15, issue 18 | Copyright
Atmos. Chem. Phys., 15, 10669-10685, 2015
https://doi.org/10.5194/acp-15-10669-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 25 Sep 2015

Research article | 25 Sep 2015

Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3 aerosol during the 2013 Southern Oxidant and Aerosol Study

H. M. Allena,1, D. C. Draper1,b, B. R. Ayres1, A. Ault3,2, A. Bondy2, S. Takahama4, R. L. Modini4, K. Baumann5, E. Edgerton5, C. Knote6, A. Laskin7, B. Wang7, and J. L. Fry1 H. M. Allen et al.
  • 1Department of Chemistry, Reed College, Portland, OR, USA
  • 2Department of Chemistry, University of Michigan, Ann Arbor, MI, USA
  • 3Department of Environmental Health Sciences, University of Michigan, Ann Arbor, MI, USA
  • 4École Polytechnique Fèdèrale de Lausanne, Lausanne, Switzerland
  • 5Atmospheric Research & Analysis, Inc., Cary, NC, USA
  • 6Meteorologisches Institut, Ludwig-Maximilians-Universität, Munich, Germany
  • 7William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USA
  • anow at: Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
  • bnow at: Department of Chemistry, University of California, Irvine, CA, USA

Abstract. Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3 is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3 and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.

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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the...
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