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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 NOx and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NOx. Observational data suggest that lightning was a far greater contributor to NOx 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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