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

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 (NO_x = 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 (r² = 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 NO_x emissions. Our a posteriori NO_x emission inventory for land surface NO_x 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 NO_x 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 NO_x, 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 NE199 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 NO_x.