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

2017
期刊 Atmospheric Chemistry and Physics Discussions
Aerosol direct effects (ADE), i.e., scattering and absorption of incoming solar radiation, reduce radiation reaching the ground and the resultant photolysis attenuation can decrease ozone (O<sub>3</sub>) formation in polluted areas. One the other hand, evidence also suggests that ADE associated cooling suppresses atmospheric ventilation thereby enhancing surface-level O<sub>3</sub>. Assessment of ADE impacts is thus important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particulate matter and O<sub>3</sub> levels. This study quantifies the impacts of ADE on tropospheric ozone by using a two-way online coupled meteorology and atmospheric chemistry model, WRF-CMAQ, instrumented with process analysis methodology. Two manifestations of ADE impacts on O<sub>3</sub> including changes in atmospheric dynamics (&amp;Delta;Dynamics) and changes in photolysis rates (&amp;Delta;Photolysis) were assessed separately through multiple scenario simulations for January and July of 2013 over China. Results suggest that ADE reduced surface daily maxima 1&amp;thinsp;h O<sub>3</sub> (DM1O<sub>3</sub>) in China by up to 39&amp;thinsp;&amp;mu;g&amp;thinsp;m<sup>-3</sup> through the combination of &amp;Delta;Dynamics and &amp;Delta;Photolysis in January, but enhanced surface DM1O<sub>3</sub> by up to 4&amp;thinsp;&amp;mu;g&amp;thinsp;m<sup>-3</sup> in July. Increased O<sub>3</sub> in July is largely attributed to &amp;Delta;Dynamics which causes a weaker O<sub>3</sub> sink of dry deposition and a stronger O<sub>3</sub> source of photochemistry due to the stabilization of atmosphere. 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 VOC-limited condition are found due to ADE in both January and July. This study suggests that reducing ADE may have potential risk of increasing O<sub>3</sub> in winter, but it will benefit the reduction of maxima O<sub>3</sub> in summer.