Abstract

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We use a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicate that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we use a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We find that responses of simulated NO2 columns to changing NOx emissions are suppressed over low NOx regions, and account for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluate NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the low end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 12.9 ± 3.9 Tg N yr−1.

Highlights

  • An important source of biogenic nitrogen oxide (NOx = nitric oxide (NO) + NO2) emissions is bacteria in soils

  • We present a method to provide top-down constraints on soil nitrogen oxides (NOx) emissions using Ozone Monitoring Instrument (OMI) tropospheric NO2 columns and simulations from the GEOS-Chem global chemistry transport models (CTMs)

  • We develop a filtering scheme to select regions and periods wherein OMI tropospheric NO2 columns are dominated by soil NOx emissions, with minimal influence of anthropogenic, lightning and biomass burning sources

Read more

Summary

Introduction

An important source of biogenic nitrogen oxide (NOx = NO + NO2) emissions is bacteria in soils. NOx emissions contribute to increased nitrogen deposition, which is important for soil NOx emissions (via soil N content) (Hudman et al, 2012), and biomass. Natural sources include soil emissions (4–15 Tg N yr−1), biomass burning (6–12 Tg N yr−1) and lightning (2–8 Tg N yr−1) (Schumann and Huntrieser, 2007). The wide range in soil NOx emission estimates reflects our incomplete knowledge of emission factors and processes driving these emissions. Reducing these substantial uncertainties will improve our understanding of tropospheric O3 and aerosol burdens, and allow for a proper assessment of the impact of soil emissions on nitrogen deposition

Methods
Results
Conclusion
Full Text
Published version (Free)

Talk to us

Join us for a 30 min session where you can share your feedback and ask us any queries you have

Schedule a call