Journal Article
Atmospheric Chemistry and Physics, vol. 22, iss. 2, pp. 1333-1349, 2022
Authors
Fei Liu, Zhining Tao, Steffen Beirle, Joanna Joiner, Yasuko Yoshida, Steven J. Smith, K. Emma Knowland, Thomas Wagner
Abstract
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
4 km × 4 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 2 % ± 17 % (mean ± standard deviation) and 15 % ± 25 %
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 9 h data prior
to satellite observations, respectively. We estimate that uncertainties in NOx lifetime and emissions arising from the method are
approximately 15 % and 20 %, respectively, for typical (US) cities. The total uncertainties reach up to 43 % (lifetimes) and 45 %
(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.
