Impacts of aerosol direct effects on tropospheric ozone through changes in atmospheric dynamics and photolysis rates

Atmos Chem Phys. 2017;17(16):9869-9883. doi: 10.5194/acp-17-9869-2017.

Abstract

Aerosol direct effects (ADEs), i.e., scattering and absorption of incoming solar radiation, reduce radiation reaching the ground and the resultant photolysis attenuation can decrease ozone (O3) formation in polluted areas. One the other hand, evidence also suggests that ADE-associated cooling suppresses atmospheric ventilation, thereby enhancing surface-level O3. Assessment of ADE impacts is thus important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particuate matter and O3 levels. This study quantifies the impacts of ADEs on tropospheric ozone by using a two-way online coupled meteorology and atmospheric chemistry model, WRF- CMAQ, using a process analysis methodology. Two mani-festations of ADE impacts on O3 including changes in atmospheric dynamics (ᐃDynamics) and changes in photolysis rates (∆Photolysis) were assessed separately through multiple scenario simulations for January and July of 2013 over China. Results suggest that ADEs reduced surface daily maxima 1 h O3 (DM1O3) in China by up to 39μgm-3 through the combination of ∆Dynamics and ∆Photolysis in January but enhanced surface DM1O3 by up to 4μgm-3 in July. Increased O3 in July is largely attributed to ∆Dynamics, which causes a weaker O3 sink of dry deposition and a stronger O3 source of photochemistry due to the stabilization of the at-mosphere. Meanwhile, surface OH is also enhanced at noon in July, though its daytime average values are reduced in January. An increased OH chain length and a shift towards more volatile organic compound (VOC)-limited conditions are found due to ADEs in both January and July. This study suggests that reducing ADEs may have the potential risk of increasing O3 in winter, but it will benefit the reduction in maxima O3 in summer.