A new method for estimating megacity NOx emissions and lifetimes from satellite observations

Abstract

We present a new method for estimating NOx emissions and effective lifetimes from large cities based on NO2 measurements from the TROPOspheric Monitoring Instrument (TROPOMI) (PAL dataset, May 2018-November 2021). As in previous studies, the estimate is based on the downwind plume evolution for different wind directions separately. The novelty of the presented approach lies in the simultaneous fit of downwind patterns for opposing wind directions, which makes the method far more robust (i.e., less prone to local minima with nonphysically high or low lifetimes) than a single exponential decay fit. In addition, the new method does not require the assumption of a city being a "point source"but also derives the spatial distribution of emissions. The method was successfully applied to 100 cities worldwide on a seasonal scale. Fitted emissions generally agree reasonably with the Emissions Database for Global Atmospheric Research (EDGAR) v6 (RCombining double low line0.72) and are on average 14ĝ€¯% lower, while estimated uncertainties are still rather large (≈ĝ€¯30ĝ€¯%-50ĝ€¯%). Lifetimes were found to be rather short (2.44ĝ€¯±ĝ€¯0.68ĝ€¯h) and show no distinct dependency on season or latitude, which might be a consequence of discarding observations at high solar zenith angles (>65°). The main limitations of this and similar methods are the underlying assumptions of steady state (meaning constant emissions, wind fields and chemical conditions) within about 100ĝ€¯km downwind from a city, which is probably a simplification that is too strong in order to reach higher accuracies.