Assessment of tropospheric ozone simulations in a regional chemical transport model using GEOS-Chem outputs as chemical boundary conditions

Regional chemical transport models (e.g., Community Multiscale Air Quality (CMAQ) Modeling System) are widely used to simulate the physical and chemical process of regional ozone (O3) pollution and its variation trend in recent years. However, chemical boundary condition (CBC) is an important input of these models and contributes to the model bias against observations. In this study, we develop a tool named GC2CMAQ that provides the CMAQ model with the CBCs from the GEOS-Chem simulation. Two experiments using different CBCs were conducted to evaluate their effect on seasonal O3 simulation in China. The Default experiment utilized the model-default static condition (the relatively clean atmosphere in the eastern United States), and the GC experiment employed the GEOS-Chem simulation results. Compared with the observation, the GC experiment has a much better performance in reproducing elevated O3 levels in the higher troposphere and lower stratosphere during different seasons. Near the earth's surface, the simulated concentrations of pollutants O3 (and PM2.5) in the GC experiment were also closer to the observation in April and July. The accuracy of simulation results in provinces close to the boundary was improved by approximately 20 %-30 % relative to the Default experiment. The CBCs provided by GEOS-Chem enabled a better simulation of stratosphere-troposphere O3 exchange in late spring and early summer, which then affected the pollutant concentration near surfaces through vertical transport. This finding was confirmed by a case study in southwestern Tibet on April 28, 2017, in which we quantified the contributions of different physical and chemical processes to O3 variations at different altitudes using the process analysis method. This study highlights the importance of using a reliable CBC for the regional chemical transport model to derive a better performance of O3 simulation.