Comprehensive analyses of source sensitivities and apportionments of PM_2.5 and ozone over Japan via multiple numerical techniques

Abstract

Abstract. Source sensitivity and source apportionment are two major indicators representing source–receptor relationships, which serve as essential information when considering effective strategies to accomplish improved air quality. This study evaluated source sensitivities and apportionments of ambient ozone and PM2.5 concentrations over Japan with multiple numerical techniques embedded in regional chemical transport models, including a brute-force method (BFM), a high-order decoupled direct method (HDDM), and an integrated source apportionment method (ISAM), to update the source–receptor relationships considering stringent emission controls recently implemented in Japan and surrounding countries. We also attempted to understand the differences among source sensitivities and source apportionments calculated by multiple techniques. While a part of ozone concentrations was apportioned to domestic sources, their sensitivities were small or even negative; ozone concentrations were exclusively sensitive to transport from outside Japan. Although the simulated PM2.5 concentrations were significantly lower than those reported by previous studies, their sensitivity to transport from outside Japan was still relatively large, implying that there has been a reduction in Japanese emissions, similar to surrounding countries including China, due to implementation of stringent emission controls. HDDM allowed us to understand the importance of the non-linear responses of PM2.5 concentrations to precursor emissions. Apportionments derived by ISAM were useful in distinguishing various direct and indirect influences on ozone and PM2.5 concentrations by combining with sensitivities. The results indicate that ozone transported from outside Japan plays a key role in exerting various indirect influences on the formation of ozone and secondary PM2.5 components. While the sensitivities come closer to the apportionments when perturbations in emissions are larger in highly non-linear relationships – including those between NH3 emissions and NH4+ concentrations, NOx emissions and NO3- concentrations, and NOx emissions and ozone concentrations – the sensitivities did not reach the apportionments because there were various indirect influences including other sectors, complex photochemical reactions, and gas–aerosol partitioning. It is essential to consider non-linear influences to derive strategies for effectively suppressing concentrations of secondary pollutants.