Seasonal source contributions of tropospheric ozone over East Asia based on CMAQ–HDDM

Determining the source contributions of tropospheric ozone concentration is an important issue for East Asia, due to the dramatic and rapid increase in emissions of atmospheric pollutants. To achieve this, the higher-order decoupled direct method (HDDM), a technique for efficient calculation of sensitivities, was applied in this study. Tropospheric ozone concentrations at observation sites located in remote areas of Japan were well-reproduced by Community Multi-scale Air Quality (CMAQ) model simulations, and exhibited a maximum peak in spring, a relatively small peak in autumn and a summer minimum. This seasonal pattern is a reflection of long-range transport and chemical processes, coupled with continental-oceanic air mass exchanges forced by the East Asian monsoon. For the HDDM simulation, we focused on episodic pollution events during each season of 2007 to clarify the seasonal characteristics, and then assessed source contributions paying attention to both precursor emissions (NOx and VOC) and source regions (China, central eastern China, Korea, and Japan). An ozone-sensitive regime (NOx- or VOC-sensitive regime) was also determined based on the HDDM results. This suggested a regime over East Asia that was NOx sensitive in summer, VOC sensitive in winter, and either NOx or VOC sensitive during spring and autumn. At observation sites in remote areas of Japan, by separating the precursor contribution into NOx and VOC components of ozone production, it was found that the contribution of NOx emissions was larger than that of VOC emissions in spring, autumn, and especially summer, therefore, a reduction in NOx emissions could reduce the severity of episodes of tropospheric ozone pollution in downwind areas. Due to the strong VOC-sensitive conditions in winter, NOx emissions enabled a reduction in surface ozone concentrations. In terms of the contributions attributed to source regions, the source contribution of China was relatively high during spring, but local-scale photochemical build-up was dominant during summer and autumn. It was also revealed that central eastern China (CEC), characterized by densely populated and industrialized regions, was the most significant source of Chinese source contributions in summer.