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4D-Var inversion of European NH3 emissions using CrIS NH3 measurements and GEOS-Chem adjoint with bi-directional and uni-directional flux schemes
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  • Hansen Cao,
  • Daven K. Henze,
  • Liye Zhu,
  • Mark W Shephard,
  • Karen Cady-Pereira,
  • Enrico Dammers,
  • Michael Sitwell,
  • Nicholas Heath,
  • Chantelle Lonsdale,
  • Jesse Owen Bash,
  • Kazuyuki Miyazaki,
  • Chris Flechard,
  • Yannick Fauvel,
  • Roy J. Wichink Kruit,
  • Stefan Feigenspan,
  • Christian Brümmer,
  • Frederik Schrader,
  • Marsailidh Twigg,
  • sarah Leeson,
  • Yuk Sim Tang,
  • Amy C.M. Stephens,
  • Christine Braban,
  • Keith Vincent,
  • Mario Meier,
  • Eva Seitler,
  • Camilla Geels,
  • Thomas Ellermann,
  • Agnieszka Sanocka,
  • Shannon L Capps
Hansen Cao
University of Colorado Boulder
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Daven K. Henze
University of Colorado Boulder

Corresponding Author:[email protected]

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Liye Zhu
Sun Yat-sen University
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Mark W Shephard
Environment Canada
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Karen Cady-Pereira
Atmospheric and Environmental Research, Inc.
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Enrico Dammers
Environment and Climate Change Canada
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Michael Sitwell
Environment and Climate Change Canada
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Nicholas Heath
Atmospheric and Environmental Research Inc., USA
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Chantelle Lonsdale
Department of Civil, Structural and Environmental Engineering, University at Buffalo
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Jesse Owen Bash
U.S. EPA
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Kazuyuki Miyazaki
Jet Propulsion Laboratory
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Chris Flechard
INRAE (National Research Institute for Agriculture, Food and Environment), UMR SAS, Agrocampus Quest
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Yannick Fauvel
INRAE
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Roy J. Wichink Kruit
National Institute for Public Health and the Environment
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Stefan Feigenspan
German Environment Agency
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Christian Brümmer
Thünen Institute of Climate-Smart Agriculture
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Frederik Schrader
Thünen Institute of Climate-Smart Agriculture
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Marsailidh Twigg
UK Centre for Ecology & Hydrology, Bush Estate, Penicuik
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sarah Leeson
Centre of Ecology and Hydrology (CEH)
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Yuk Sim Tang
Centre for Ecology and Hydrology
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Amy C.M. Stephens
Centre for Ecology and Hydrology
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Christine Braban
Center for Ecology and Hydrology
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Keith Vincent
Ricardo Energy & Environment
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Mario Meier
Forschungsstelle fur Umweltbeobachtung
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Eva Seitler
Forschungsstelle fur Umweltbeobachtung
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Camilla Geels
Aarhus University
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Thomas Ellermann
Aarhus University
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Agnieszka Sanocka
Ricardo Energy & Environment
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Shannon L Capps
Georgia Institute of Technology
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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.