Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow

R. C. Hudman, Daniel J. Jacob, Solène Turquety, E. M. Leibensperger, L. T. Murray, S. Wu, A. B. Gilliland, M. Avery, T. H. Bertram, William Brune, Ronald C. Cohen, Jack E. Dibb, F. M. Flocke, Alan Fried, J. Holloway, J. A. Neuman, R. Orville, A. Perring, X. Ren, Glen W. SachseHanwant B. Singh, A. Swanson, P. J. Wooldridge

Research output: Contribution to journalArticle

210 Scopus citations

Abstract

We use observations from two aircraft during the ICARTT campaign over the eastern United States and North Atlantic during summer 2004, interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem) to test current understanding of regional sources, chemical evolution, and export of NOx. The boundary layer NOx data provide top-down verification of a 50% decrease in power plant and industry NOx emissions over the eastern United States between 1999 and 2004. Observed NOx concentrations at 8-12 km altitude were 0.55 ± 0.36 ppbv, much larger than in previous U.S. aircraft campaigns (ELCHEM, SUCCESS, SONEX) though consistent with data from the NOXAR program aboard commercial aircraft. We show that regional lightning is the dominant source of this upper tropospheric NOx and increases upper tropospheric ozone by 10 ppbv. Simulating ICARTT upper tropospheric NOx observations with GEOS-Chem requires a factor of 4 increase in modeled NOx yield per flash (to 500 mol/flash). Observed OH concentrations were a factor of 2 lower than can be explained from current photochemical models, for reasons that are unclear. A NOy-CO correlation analysis of the fraction f of North American NOx emissions vented to the free troposphere as NOy (sum of NOx and its oxidation products) shows observed f = 16 ± 10% and modeled f = 14 ± 9%, consistent with previous studies. Export to the lower free troposphere is mostly HNO3 but at higher altitudes is mostly PAN. The model successfully simulates NOy export efficiency and speciation, supporting previous model estimates of a large U.S. anthropogenic contribution to global tropospheric ozone through PAN export.

Original languageEnglish (US)
Article numberD12S05
JournalJournal of Geophysical Research Atmospheres
Volume112
Issue number12
DOIs
StatePublished - Jun 27 2007

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Forestry
  • Oceanography
  • Aquatic Science
  • Ecology
  • Water Science and Technology
  • Soil Science
  • Geochemistry and Petrology
  • Earth-Surface Processes
  • Atmospheric Science
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science
  • Palaeontology

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    Hudman, R. C., Jacob, D. J., Turquety, S., Leibensperger, E. M., Murray, L. T., Wu, S., Gilliland, A. B., Avery, M., Bertram, T. H., Brune, W., Cohen, R. C., Dibb, J. E., Flocke, F. M., Fried, A., Holloway, J., Neuman, J. A., Orville, R., Perring, A., Ren, X., ... Wooldridge, P. J. (2007). Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow. Journal of Geophysical Research Atmospheres, 112(12), [D12S05]. https://doi.org/10.1029/2006JD007912