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Accepted (AM)Open Access (License Unspecified), Open
Journal article
4D-Var inversion of European NH3 emissions using CrIS NH3 measurements and GEOS-Chem adjoint with bi-directional and uni-directional flux schemes
14 Sep 2021
Abstract
We conduct the first 4D-Var inversion of NH3 accounting for NH3 bi-directional 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-down NH3 emissions estimates associated with treatment of NH3 surface exchange.
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Details
- Title
- 4D-Var inversion of European NH3 emissions using CrIS NH3 measurements and GEOS-Chem adjoint with bi-directional and uni-directional flux schemes
- Creators
- Hansen Cao - University of Colorado SystemDaven K. Henze - University of Colorado BoulderLiye Zhu - Sun Yat-sen UniversityMark W. Shephard - Environment and Climate Change CanadaKaren Cady-PereiraEnrico Dammers - Environment CanadaMichael Sitwell - Environment and Climate Change CanadaNicholas Heath - Atmospheric and Environmental ResearchChantelle Lonsdale - University at Buffalo, State University of New YorkJesse O. BashKazuyuki Miyazaki - Jet Propulsion LaboratoryChristophe FlechardYannick Fauvel - Institut National de Recherche pour l'Agriculture, l'Alimentation et l'EnvironnementRoy Wichink KruitStefan Feigenspan - German Environment AgencyChristian BrümmerFrederik SchraderMarsailidh M. Twigg - UK Centre for Ecology & HydrologySarah Leeson - UK Centre for Ecology & HydrologyYuk S. Tang - UK Centre for Ecology & HydrologyAmy C. M. StephensChristine BrabanKeith Vincent - RicardoMario Meier - Amt für UmweltEva Seitler - Amt für UmweltCamilla Geels - Aarhus UniversityThomas Ellermann - Aarhus UniversityAgnieszka Sanocka - RicardoShannon L. Capps - Georgia Institute of Technology
- Publisher
- Wiley
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Civil, Architectural, and Environmental Engineering
- Other Identifier
- 991021811628804721