Articles | Volume 16, issue 12
https://doi.org/10.5194/acp-16-7623-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-7623-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
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. Romer
Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA
Kaitlin C. Duffey
Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA
Paul J. Wooldridge
Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA
Hannah M. Allen
Department of Chemistry, Reed College, Portland, OR, USA
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
Benjamin R. Ayres
Department of Chemistry, Reed College, Portland, OR, USA
Steven S. Brown
Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
William H. Brune
Department of Meteorology, Pennsylvania State University, University Park, PA, USA
John D. Crounse
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
Joost de Gouw
Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Danielle C. Draper
Department of Chemistry, Reed College, Portland, OR, USA
Department of Chemistry, University of California, Irvine, CA, USA
Philip A. Feiner
Department of Meteorology, Pennsylvania State University, University Park, PA, USA
Juliane L. Fry
Department of Chemistry, Reed College, Portland, OR, USA
Allen H. Goldstein
Department of Civil and Environmental Engineering, University of California at Berkeley, Berkeley, CA, USA
Department of Environmental Science, Policy and Management, University of California at Berkeley, Berkeley, CA, USA
Abigail Koss
Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Pawel K. Misztal
Department of Environmental Science, Policy and Management, University of California at Berkeley, Berkeley, CA, USA
Tran B. Nguyen
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
Department of Environmental Toxicology, University of California, Davis, CA, USA
Kevin Olson
Department of Environmental Science, Policy and Management, University of California at Berkeley, Berkeley, CA, USA
Alex P. Teng
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
Paul O. Wennberg
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA
Robert J. Wild
Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Li Zhang
Department of Meteorology, Pennsylvania State University, University Park, PA, USA
Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA
Department 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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How to cite. Romer, P. S., Duffey, K. C., Wooldridge, P. J., Allen, H. M., Ayres, B. R., Brown, S. S., Brune, W. H., Crounse, J. D., de Gouw, J., Draper, D. C., Feiner, P. A., Fry, J. L., Goldstein, A. H., Koss, A., Misztal, P. K., Nguyen, T. B., Olson, K., Teng, A. P., Wennberg, P. O., Wild, R. J., Zhang, L., and Cohen, R. C.: The lifetime of nitrogen oxides in an isoprene-dominated forest, Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, 2016.
Short summary
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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