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Zusammenfassung:
The Copernicus Atmosphere Monitoring Service (CAMS) provides routine analyses and forecasts of trace gases and aerosols on a global scale. The core is the European Centre for Medium Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS), where modules for atmospheric chemistry and aerosols have been introduced and which allows for data assimilation of satellite retrievals of composition.
We have updated both the homogeneous and heterogeneous NOx chemistry applied in the three independent tropospheric-stratospheric chemistry modules maintained within CAMS, referred to as IFS(CB05BASCOE), IFS(MOCAGE) and IFS(MOZART). Here we focus on the evaluation of main trace gas products from these modules that are of interest as markers of air quality, namely lower-tropospheric O-3, NO2 and CO, with a regional focus over the contiguous United States.
Evaluation against lower-tropospheric composition reveals overall good performance, with chemically induced biases within 10 ppb across species for regions within the US with respect to a range of observations. The versions show overall equal or better performance than the CAMS reanalysis, which includes data assimilation Evaluation of surface air quality aspects shows that annual cycles are captured well, albeit with variable seasonal biases. During wintertime conditions there is a large model spread between chemistry schemes in lower-tropospheric O-3 (similar to 10 %-35 %) and, in turn, oxidative capacity related to NOx lifetime differences. Analysis of differences in the HNO3 and PAN formation, which act as reservoirs for reactive nitrogen, revealed a general underestimate in PAN formation over polluted regions, likely due to too low organic precursors. Particularly during wintertime, the fraction of NO2 sequestered into PAN has a variability of 100 % across chemistry modules, indicating the need for further constraints. Notably, a considerable uncertainty in HNO3 formation associated with wintertime N2O5 conversion on wet particle surfaces remains.
In summary, this study has indicated that the chemically induced differences in the quality of CAMS forecast products over the United States depends on season, trace gas, altitude and region. While analysis of the three chemistry modules in CAMS provide a strong handle on uncertainties associated with chemistry modeling, the further improvement of operational products additionally requires coordinated development involving emissions handling, chemistry and aerosol modeling, complemented with data-assimilation efforts.
