Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow
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. T...
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Language: | English |
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American Geophysical Union
2007
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Online Access: | http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-003-909 https://doi.org/10.1029/2006JD007912 |
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ftncar:oai:drupal-site.org:articles_6619 2023-10-01T03:58:02+02:00 Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow Hudman, R. (author) Jacob, D. (author) Turquety, S. (author) Leibensperger, E. (author) Murray, L. (author) Wu, S. (author) Gilliland, A. (author) Avery, M. (author) Bertram, T. (author) Brune, W. (author) Cohen, R. (author) Dibb, J. (author) Flocke, Frank (author) Fried, Alan (author) Holloway, J. (author) Neuman, J. (author) Orville, R. (author) Perring, A. (author) Ren, X. (author) Sachse, G. (author) Singh, H. (author) Swanson, Aaron (author) Wooldridge, P. (author) 2007-04-18 application/pdf http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-003-909 https://doi.org/10.1029/2006JD007912 en eng American Geophysical Union Journal of Geophysical Research-Atmospheres http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-003-909 doi:10.1029/2006JD007912 ark:/85065/d75d8s28 Copyright 2007 American Geophysical Union. Text article 2007 ftncar https://doi.org/10.1029/2006JD007912 2023-09-04T18:22:22Z 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. Article in Journal/Newspaper North Atlantic OpenSky (NCAR/UCAR - National Center for Atmospheric Research/University Corporation for Atmospheric Research) Journal of Geophysical Research 112 D12 |
institution |
Open Polar |
collection |
OpenSky (NCAR/UCAR - National Center for Atmospheric Research/University Corporation for Atmospheric Research) |
op_collection_id |
ftncar |
language |
English |
description |
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. |
author2 |
Hudman, R. (author) Jacob, D. (author) Turquety, S. (author) Leibensperger, E. (author) Murray, L. (author) Wu, S. (author) Gilliland, A. (author) Avery, M. (author) Bertram, T. (author) Brune, W. (author) Cohen, R. (author) Dibb, J. (author) Flocke, Frank (author) Fried, Alan (author) Holloway, J. (author) Neuman, J. (author) Orville, R. (author) Perring, A. (author) Ren, X. (author) Sachse, G. (author) Singh, H. (author) Swanson, Aaron (author) Wooldridge, P. (author) |
format |
Article in Journal/Newspaper |
title |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
spellingShingle |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
title_short |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
title_full |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
title_fullStr |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
title_full_unstemmed |
Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow |
title_sort |
surface and lightning sources of nitrogen oxides over the united states: magnitudes, chemical evolution, and outflow |
publisher |
American Geophysical Union |
publishDate |
2007 |
url |
http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-003-909 https://doi.org/10.1029/2006JD007912 |
genre |
North Atlantic |
genre_facet |
North Atlantic |
op_relation |
Journal of Geophysical Research-Atmospheres http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-003-909 doi:10.1029/2006JD007912 ark:/85065/d75d8s28 |
op_rights |
Copyright 2007 American Geophysical Union. |
op_doi |
https://doi.org/10.1029/2006JD007912 |
container_title |
Journal of Geophysical Research |
container_volume |
112 |
container_issue |
D12 |
_version_ |
1778530388444971008 |