Inverse modeling constraints on sources of NH3 using CrIS remote sensing measurements

Hansen Cao1, Daven Henze2, Mark W. Shephard3, Karen Cady-Pereirda4, Matthew Alvarado5 and Chantelle Lonsdale6

Atmospheric NH3is an important precursor to particulate matter, and it has effects on ecosystem stability, soil acidification, aerosol acidity, and climate change. Previous estimates of NH3emissions in the US are quite uncertain both in terms of magnitude and seasonal variability. The most recent remote sensing measurements of NH3from CrIS can provide constraints on NH3sources at fine resolution, and with great spatial coverage and small noises. We conducted 4D-Var inversion experiments using high-resolution CrIS observations of NH3profiles, GEOS-Chem, and its adjoint model to estimate NH3emissions in the contiguous US for each month in 2014. Increases are found in CrIS-derived anthropogenic NH3emissions across most of contiguous US on an annual scale, while slight decreases are found over Northern Iowa and Southern California from March to July. CrIS-derived anthropogenic NH3emission estimates for the contiguous US is 4.27 Tg N a-1, ~45% higher than the HTAP v2 emission inventory (2.95 Tg N a-1). We evaluate our CrIS-derived NH3emissions using monthly mean AMoN surface NH3measurements in 2014. CrIS-derived monthly NH3emissions increased the correlation coefficient between national monthly average of GEOS-Chem surface NH3and AMoN surface NHmeasuremnents from 0.33 to 0.82, and decreased the normalized mean bias (NMB) from -0.34 to 0.10 on an annual and national scale. We will further evaluate our CrIS-derived NHemissions using NADP measurements of wet deposition of NH4+in 2014.

 

1University of Colorado Boulder, hansen.cao@colorado.edu
2University of Colorado Boulder, daven.henze@colorado.edu
3Environment Canada, Toronto, Ontario, Canada, mark.shephard@canada.ca
4Atmospheric and Environmental Research Inc., USA, kcadyper@aer.com
5Atmospheric and Environmental Research Inc., USA, malvarad@aer.com
6Atmospheric and Environmental Research Inc., USA, clonsdal@aer.com