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

Abstract

We retrieve tropospheric nitrogen dioxide (NO 2) columns for May 2004 to April 2005 from the SCIAMACHY satellite instrument to derive top‐down emissions of nitrogen oxides (NO x = NO + NO 2) via inverse modeling with a global chemical transport model (GEOS‐Chem). Simulated NO 2 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 NO 2 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 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 NEI99 inventory for the United States, and 68% larger than a regional inventory for 2000 for eastern Asia. SCIAMACHY NO 2 columns over the North Atlantic show a weak plume from lightning NO x.