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The lifetime of nitrogen oxides in an isoprene-dominated forest

Romer, Paul S. and Duffey, Kaitlin C. and Wooldridge, Paul J. and Allen, Hannah M. and Ayres, Benjamin R. and Brown, Steven S. and Brune, William H. and Crounse, John D. and de Gouw, Joost and Draper, Danielle C. and Feiner, Philip A. and Fry, Juliane L. and Goldstein, Allen H. and Koss, Abigail and Misztal, Pawel K. and Nguyen, Tran B. and Olson, Kevin and Teng, Alex P. and Wennberg, Paul O. and Wild, Robert J. and Zhang, Li and Cohen, Ronald C. (2016) The lifetime of nitrogen oxides in an isoprene-dominated forest. Atmospheric Chemistry and Physics, 16 (12). pp. 7623-7637. ISSN 1680-7324.

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The lifetime of nitrogen oxides (NO_x) affects the concentration and distribution of NO_x and the spatial patterns of nitrogen deposition. Despite its importance, the lifetime of NO_x 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 NO_x and NO_x reservoirs. We find that the lifetime of NO_x 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 HNO_3 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 HNO_3 and the primary pathway to permanent removal of NO_x from the boundary layer in this location. Using these new constraints on the fate of ΣANs, we find that the NO_x lifetime is 11 ± 5 h under typical midday conditions. The lifetime is extended by storage of NO_x in temporary reservoirs, including acyl peroxy nitrates and ΣANs.

Item Type:Article
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URLURL TypeDescription
Crounse, John D.0000-0001-5443-729X
Wennberg, Paul O.0000-0002-6126-3854
Additional Information:© Author(s) 2016. CC Attribution 3.0 License. Received 12 Jan 2016; published in Atmos. Chem. Phys. Discuss. 21 Jan 2016; revised 4 May 2016; accepted 16 May 2016; published 23 Jun 2016. Financial and logistical support for SOAS was provided by the NSF, the Earth Observing Laboratory at the National Center for Atmospheric Research (operated by NSF), the personnel at Atmospheric Research and Analysis, and the Electric Power Research Institute. The Berkeley authors acknowledge the support of the NOAA Office of Global Programs (NA13OAR4310067) and the NSF (AGS-1352972) and by EPA STAR Grant 835407 (to Allen H. Goldstein). The Caltech authors acknowledge the support of the NSF (AGS-1331360, AGS-1240604). The Penn State authors acknowledge the support of the NSF (AGS-1246918). Ronald C. Cohen acknowledges support from the Miller Institute for Basic Research.
Funding AgencyGrant Number
National Center for Atmospheric Research (NCAR)UNSPECIFIED
Electric Power Research Institute (EPRI)UNSPECIFIED
National Oceanic and Atmospheric Administration (NOAA)NA13OAR4310067
Environmental Protection Agency (EPA)835407
Miller Institute for Basic Research in ScienceUNSPECIFIED
Issue or Number:12
Record Number:CaltechAUTHORS:20160804-150734787
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Official Citation: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, doi:10.5194/acp-16-7623-2016, 2016.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:69452
Deposited By: Melissa Ray
Deposited On:09 Aug 2016 02:36
Last Modified:03 Oct 2019 10:22

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