Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere

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Read Full Article (file size: 776989 bytes) Cited by JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 112, D12S04, doi:10.1029/2006JD007664, 2007 Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere H. B. Singh NASA Ames Research Center, Moffett Field, California, USA L. Salas NASA Ames Research Center, Moffett Field, California, USA D. Herlth NASA Ames Research Center, Moffett Field, California, USA R. Kolyer NASA Ames Research Center, Moffett Field, California, USA E. Czech NASA Ames Research Center, Moffett Field, California, USA M. Avery NASA Langley Research Center, Hampton, Virginia, USA J. H. Crawford NASA Langley Research Center, Hampton, Virginia, USA R. B. Pierce NASA Langley Research Center, Hampton, Virginia, USA G. W. Sachse NASA Langley Research Center, Hampton, Virginia, USA D. R. Blake Department of Chemistry, University of California, Irvine, California, USA R. C. Cohen Department of Chemistry and Department of Earth and Planetary Sciences, University of California, Berkeley, California, USA T. H. Bertram Department of Chemistry and Department of Earth and Planetary Sciences, University of California, Berkeley, California, USA A. Perring Department of Chemistry and Department of Earth and Planetary Sciences, University of California, Berkeley, California, USA P. J. Wooldridge Department of Chemistry and Department of Earth and Planetary Sciences, University of California, Berkeley, California, USA J. Dibb Institute for the Study of Earth Oceans and Space, University of New Hampshire, Durham, New Hampshire, USA G. Huey School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA R. C. Hudman Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts, USA S. Turquety Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts, USA L. K. Emmons National Center for Atmospheric Research, Boulder, Colorado, USA F. Flocke National Center for Atmospheric Research, Boulder, Colorado, USA Y. Tang Department of Chemical and Biochemical Engineering, University of Iowa, Iowa City, Iowa, USA G. R. Carmichael Department of Chemical and Biochemical Engineering, University of Iowa, Iowa City, Iowa, USA L. W. Horowitz NOAA Geophysical Fluid Dynamics Laboratory, Princeton, New Jersey, USA Abstract A comprehensive group of reactive nitrogen species (NO, NO₂, HNO₃, HO₂NO₂, PANs, alkyl nitrates, and aerosol-NO₃ ⁻) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1–12 km). Nitrogen containing tracers of biomass combustion (HCN and CH₃CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO_x and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO_x. Observational data suggest that lightning was a far greater contributor to NO_x in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (HO₂NO₂) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation. Received 15 June 2006; accepted 7 December 2006; published 4 April 2007. Keywords: nitrogen oxides; PAN; ozone; hydrogen cyanide; aerosol nitrate; lightning. Index Terms: 0365 Atmospheric Composition and Structure: Troposphere: composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere: constituent transport and chemistry; 0345 Atmospheric Composition and Structure: Pollution: urban and regional (0305, 0478, 4251); 0322 Atmospheric Composition and Structure: Constituent sources and sinks. Read Full Article (file size: 776989 bytes) Cited by Citation: Singh, H. B., et al. (2007), Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere, J. Geophys. Res., 112, D12S04, doi:10.1029/2006JD007664. Copyright 2007 by the American Geophysical Union.

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