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Abstract:
We present an evaluation of the online regional model WRF-Chem over Europe with a focus on ground-level ozone (O-3) and nitrogen oxides (NOx). The model performance is evaluated for two chemical mechanisms, MOZART-4 and RADM2, for year-long simulations. Model-predicted surface meteorological variables (e.g., temperature, wind speed and direction) compared well overall with surface-based observations, consistent with other WRF studies. WRF-Chem simulations employing MOZART-4 as well as RADM2 chemistry were found to reproduce the observed spatial variability in surface ozone over Europe. However, the absolute O-3 concentrations predicted by the two chemical mechanisms were found to be quite different, with MOZART-4 predicting O-3 concentrations up to 20 mu g m(-3) greater than RADM2 in summer. Compared to observations, MOZART-4 chemistry overpredicted O-3 concentrations for most of Europe in the summer and fall, with a summertime domain-wide mean bias of +10 mu g m(-3) against observations from the AirBase network. In contrast, RADM2 chemistry generally led to an underestimation of O-3 over the European domain in all seasons. We found that the use of the MOZART-4 mechanism, evaluated here for the first time for a European domain, led to lower absolute biases than RADM2 when compared to ground-based observations. The two mechanisms show relatively similar behavior for NOx, with both MOZART-4 and RADM2 resulting in a slight underestimation of NOx compared to surface observations. Further investigation of the differences between the two mechanisms revealed that the net midday photochemical production rate of O-3 in summer is higher for MOZART-4 than for RADM2 for most of the domain. The largest differences in O-3 production can be seen over Germany, where net O-3 production in MOZART-4 is seen to be higher than in RADM2 by 1.8 ppbh 1 (3.6 mu g m(-3) h(-1)) or more. We also show that while the two mechanisms exhibit similar NOx sensitivity, RADM2 is approximately twice as sensitive to increases in anthropogenic VOC emissions as MOZART-4. Additionally, we found that differences in reaction rate coefficients for inorganic gas-phase chemistry in MOZART-4 vs. RADM2 accounted for a difference of 8 mu g m(-3), or 40% of the summertime difference in O-3 predicted by the two mechanisms. Differences in deposition and photolysis schemes explained smaller differences in O-3. Our results highlight the strong dependence of modeled surface O-3 over Europe on the choice of gas-phase chemical mechanism, which we discuss in the context of overall uncertainties in prediction of ground-level O-3 and its associated health impacts (via the health-related metrics MDA8 and SOMO35).
