Late-spring and summertime tropospheric ozone and no2 in western siberia and the russian arctic: Regional model evaluation and sensitivities

Abstract

We use a regional chemistry transport model (Weather Research and Forecasting model coupled with chemistry, WRF-Chem) in conjunction with surface obser vations of tropospheric ozone and Ozone Monitoring Instru ment (OMI) satellite retrievals of tropospheric column NO2 to evaluate processes controlling the regional distribution of tropospheric ozone over western Siberia for late spring and summer in 2011. This region hosts a range of anthro pogenic and natural ozone precursor sources, and it serves as a gateway for near-surface transport of Eurasian pollution to the Arctic. However, there is a severe lack of in situ ob servations to constrain tropospheric ozone sources and sinks in the region. We show widespread negative bias in WRF Chem tropospheric column NO2 when compared to OMI satellite observations from May-August, which is reduced when using ECLIPSE (Evaluating the Climate and Air Qual ity Impacts of Short-Lived Pollutants) v5a emissions (frac tional mean bias (FMB)=-0.82 to-0.73) compared with the EDGAR (Emissions Database for Global Atmospheric Research)-HTAP (Hemispheric Transport of Air Pollution) v2.2 emissions data (FMB =-0.80 to -0.70). Despite the large negative bias, the spatial correlations between model and observed NO2 columns suggest that the spatial pattern of NOx sources in the region is well represented. Scaling trans port and energy emissions in the ECLIPSE v5a inventory by a factor of 2 reduces column NO2 bias (FMB=-0.66 to-0.35), but with overestimates in some urban regions and little change to a persistent underestimate in background re gions. Based on the scaled ECLIPSE v5a emissions, we as sess the influence of the two dominant anthropogenic emis sion sectors (transport and energy) and vegetation fires on surface NOx and ozone over Siberia and the Russian Arctic. Our results suggest regional ozone is more sensitive to an thropogenic emissions, particularly from the transport sector, and the contribution from fire emissions maximises in June and is largely confined to latitudes south of 60° N. Ozone dry deposition fluxes from the model simulations show that the dominant ozone dry deposition sink in the region is to for est vegetation, averaging 8.0 Tg of ozone per month, peak ing at 10.3 Tg of ozone deposition during June. The impact of fires on ozone dry deposition within the domain is small compared to anthropogenic emissions and is negligible north of 60° N. Overall, our results suggest that surface ozone in the region is controlled by an interplay between seasonality in atmospheric transport patterns, vegetation dry deposition, and a dominance of transport and energy sector emissions.