4D-Var inversion of European NH3 emissions using CrIS NH3 measurements
and GEOS-Chem adjoint with bi-directional and uni-directional flux
schemes
Abstract
We conduct the first 4D-Var inversion of NH3 accounting for NH3
bidirectional flux, using CrIS satellite NH3 observations over Europe in
2016. We find posterior NH3 emissions peak more in springtime than prior
emissions at continental to national scales, and annually they are
generally smaller than the prior emissions over central Europe, but
larger over most of the rest of Europe. Annual posterior anthropogenic
NH3 emissions for 25 European Union members (EU25) are 25% higher than
the prior emissions and very close(<2% difference) to other
inventories. Our posterior annual anthropogenic emissions for EU25, the
UK, the Netherlands, and Switzerland are generally 10-20% smaller than
when treating NH3 fluxes as uni-directional emissions, while the monthly
regional difference can be up to 34% (Switzerland in July). Compared to
monthly mean in-situ observations, our posterior NH3 emissions from both
schemes generally improve the magnitude and seasonality of simulated
surface NH3 and bulk NHx wet deposition throughout most of Europe,
whereas evaluation against hourly measurements at a background site
shows the bi-directional scheme better captures observed diurnal
variability of surface NH3. This contrast highlights the need for
accurately simulating diurnal variability of NH3 in assimilation of
sun-synchronous observations and also the potential value of future
geostationary satellite observations. Overall, our top-down ammonia
emissions can help to examine the effectiveness of air pollution control
policies to facilitate future air pollution management, as well as
helping us understand the uncertainty in top-downNH3emission estimates
associated with treatment of NH3surface exchange.