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Volume 16, issue 12
Atmos. Chem. Phys., 16, 7623–7637, 2016
https://doi.org/10.5194/acp-16-7623-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 16, 7623–7637, 2016
https://doi.org/10.5194/acp-16-7623-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 23 Jun 2016

Research article | 23 Jun 2016

The lifetime of nitrogen oxides in an isoprene-dominated forest

Paul S. Romer1, Kaitlin C. Duffey1, Paul J. Wooldridge1, Hannah M. Allen2,3, Benjamin R. Ayres2, Steven S. Brown4, William H. Brune5, John D. Crounse6, Joost de Gouw4,7, Danielle C. Draper2,8, Philip A. Feiner5, Juliane L. Fry2, Allen H. Goldstein9,10, Abigail Koss4,7, Pawel K. Misztal10, Tran B. Nguyen6,11, Kevin Olson10, Alex P. Teng6, Paul O. Wennberg6,12, Robert J. Wild4,7, Li Zhang5, and Ronald C. Cohen1,13 Paul S. Romer et al.
  • 1Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA
  • 2Department of Chemistry, Reed College, Portland, OR, USA
  • 3Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
  • 4Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
  • 5Department of Meteorology, Pennsylvania State University, University Park, PA, USA
  • 6Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
  • 7Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 8Department of Chemistry, University of California, Irvine, CA, USA
  • 9Department of Civil and Environmental Engineering, University of California at Berkeley, Berkeley, CA, USA
  • 10Department of Environmental Science, Policy and Management, University of California at Berkeley, Berkeley, CA, USA
  • 11Department of Environmental Toxicology, University of California, Davis, CA, USA
  • 12Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA
  • 13Department of Earth and Planetary Sciences, University of California at Berkeley, Berkeley, CA, USA

Abstract. The lifetime of nitrogen oxides (NOx) affects the concentration and distribution of NOx and the spatial patterns of nitrogen deposition. Despite its importance, the lifetime of NOx is poorly constrained in rural and remote continental regions. We use measurements from a site in central Alabama during the Southern Oxidant and Aerosol Study (SOAS) in summer 2013 to provide new insights into the chemistry of NOx and NOx reservoirs. We find that the lifetime of NOx during the daytime is controlled primarily by the production and loss of alkyl and multifunctional nitrates (ΣANs). During SOAS, ΣAN production was rapid, averaging 90 ppt h−1 during the day, and occurred predominantly during isoprene oxidation. Analysis of the ΣAN and HNO3 budgets indicate that ΣANs have an average lifetime of under 2 h, and that approximately 45 % of the ΣANs produced at this site are rapidly hydrolyzed to produce nitric acid. We find that ΣAN hydrolysis is the largest source of HNO3 and the primary pathway to permanent removal of NOx from the boundary layer in this location. Using these new constraints on the fate of ΣANs, we find that the NOx lifetime is 11 ± 5 h under typical midday conditions. The lifetime is extended by storage of NOx in temporary reservoirs, including acyl peroxy nitrates and ΣANs.

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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the...
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