A new method for inferring city emissions and lifetimes of nitrogen oxides from high-resolution nitrogen dioxide observations: A model study

Abstract

We present a new method to infer emissions and lifetimes of nitrogen oxides (NOx) based on tropospheric nitrogen dioxide (NO2) observations together with reanalysis wind fields for cities located in polluted backgrounds. Since the accuracy of the method is difficult to assess due to lack of "true values"that can be used as a benchmark, we apply the method to synthetic NO2 observations derived from the NASA-Unified Weather Research and Forecasting (NU-WRF) model at a high horizontal spatial resolution of 4ĝ€¯kmĝ€¯×ĝ€¯4ĝ€¯km for cities over the continental United States. We compare the inferred emissions and lifetimes with the values given by the NU-WRF model to evaluate the method. The method is applicable to 26 US cities. The derived results are generally in good agreement with the values given by the model, with the relative differences of 2ĝ€¯%ĝ€¯±ĝ€¯17ĝ€¯% (meanĝ€¯±ĝ€¯standard deviation) and 15ĝ€¯%ĝ€¯±ĝ€¯25ĝ€¯% for lifetimes and emissions, respectively. Our investigation suggests that the use of wind data prior to the satellite overpass time improves the performance of the method. The correlation coefficients between inferred and NU-WRF lifetimes increase from 0.56 to 0.79 and for emissions increase from 0.88 to 0.96 when comparing results based on wind fields sampled simultaneously with satellite observations and averaged over 9ĝ€¯h data prior to satellite observations, respectively. We estimate that uncertainties in NOx lifetime and emissions arising from the method are approximately 15ĝ€¯% and 20ĝ€¯%, respectively, for typical (US) cities. The total uncertainties reach up to 43ĝ€¯% (lifetimes) and 45ĝ€¯% (emissions) by considering the additional uncertainties associated with satellite NO2 observations and wind data. We expect this new method to be applicable to NO2 observations from the TROPOspheric Monitoring Instrument (TROPOMI) and geostationary satellites, such as Geostationary Environment Monitoring Spectrometer (GEMS) or the Tropospheric Emissions: Monitoring Pollution (TEMPO) instrument, to estimate urban NOx emissions and lifetimes globally.