Evaluation of space-based constraints on global nitrogen oxide emissions with regional aircraft measurements over and downwind of eastern North America

被引:137
作者
Martin, Randall V. [1 ]
Sioris, Christopher E.
Chance, Kelly
Ryerson, Thomas B.
Bertram, Timothy H.
Wooldridge, Paul J.
Cohen, Ronald C.
Neuman, J. Andy
Swanson, Aaron
Flocke, Frank M.
机构
[1] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS B3H 3J5, Canada
[2] Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA
[3] NOAA, Div Chem Sci, Earth Syst Res Lab, Boulder, CO 80307 USA
[4] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[5] Cooperat Inst Res Atmosphere Sci, Boulder, CO USA
[6] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80307 USA
关键词
D O I
10.1029/2005JD006680
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[ 1] We retrieve tropospheric nitrogen dioxide (NO2) columns for May 2004 to April 2005 from the SCIAMACHY satellite instrument to derive top-down emissions of nitrogen oxides (NOx = NO + NO2) via inverse modeling with a global chemical transport model (GEOS-Chem). Simulated NO2 vertical profiles used in the retrieval are evaluated with airborne measurements over and downwind of North America (ICARTT); a northern midlatitude lightning source of 1.6 Tg N yr(-1) minimizes bias in the retrieval. Retrieved NO2 columns are validated (r(2) = 0.60, slope = 0.82) with coincident airborne in situ measurements. The top-down emissions are combined with a priori information from a bottom-up emission inventory with error weighting to achieve an improved a posteriori estimate of the global distribution of surface NOx emissions. Our a posteriori NOx emission inventory for land surface NOx emissions (46.1 Tg N yr(-1)) is 22% larger than the GEIA-based a priori bottom-up inventory for 1998, a difference that reflects rising anthropogenic emissions, especially from East Asia. A posteriori NOx emissions for East Asia (9.8 Tg N yr(-1)) exceed those from other continents. The a posteriori inventory improves the GEOS-Chem simulation of NOx, peroxyacetylnitrate, and nitric acid with respect to airborne in situ measurements over and downwind of New York City. The a posteriori is 7% larger than the EDGAR 3.2FT2000 global inventory, 3% larger than the NEI99 inventory for the United States, and 68% larger than a regional inventory for 2000 for eastern Asia. SCIAMACHY NO2 columns over the North Atlantic show a weak plume from lightning NOx.
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页数:15
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