Abstract

An ensemble-variational inversion system is developed for the estimation of ammonia emissions using ammonia retrievals from the Cross-track Infrared Sounder (CrIS) for use in the Global Environmental Multiscale – Modelling Air quality and Chemistry (GEM-MACH) chemical weather model. A novel hybrid method to compare logarithmic retrieval parameters to model profiles is presented. Inversions for the monthly mean ammonia emissions over North America were performed for May to August 2016. Inversions using the hybrid comparison method increased ammonia emissions at most locations within the model domain, with total monthly mean emissions increasing by 11–41 %. The use of these revised emissions in GEM-MACH reduced biases with surface ammonia observations by as much as 25 %. The revised ammonia emissions also improved the forecasts of total (fine+coarse) ammonium and nitrate and ammonium wet deposition, with biases decreasing by as much as 13 %, but did not improve the forecasts of just the fine components of ammonium and nitrate. An additional area of 1.3 × 105 km2 of upland forests in Canada were estimated to exceed the ecosystem's critical load due to the changes in ammonia deposition from the inversion. A comparison of biases resulting from inversions using different comparison methods shows favourable results for the hybrid comparison method.

Highlights

  • Ammonia (NH3) is one of the most abundant reactive nitrogen species in the atmosphere

  • The aim of this work is to (1) develop an ensemblevariational inversion system that is capable of refining the ammonia emissions currently used in Global Environmental Multiscale (GEM)-MACH by using Cross-track Infrared Sounder (CrIS) ammonia retrievals and (2) determine the impact of these updated emissions on the ammonia fields predicted by GEM-MACH as well as on fields related to inorganic particulate matter (PM)

  • 4 Results 380 We begin this section by discussing the monthly mean ammonia emissions produced by the inversion and its impact on the ammonia fields in GEM-MACH

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Summary

Introduction

Ammonia (NH3) is one of the most abundant reactive nitrogen species in the atmosphere. Excess deposition of ammonia has been associated with eutrophication and soil acidification (Fangmeier et al, 1994; Krupa, 2003). As the primary basic gas in the atmosphere, ammonia plays a central role in the neutralization of acids and the formation of particulate matter (PM) in the atmosphere (Tsimpidi et al, 2007; Makar et al, 2009). While ammonia has a relatively short atmospheric lifetime, on the order of hours to days (Van Damme et al, 2018), fine particulate matter can last much longer in the atmosphere, on the 20 order of days to weeks (Seinfeld and Pandis, 2006).

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