Abstract
Recent studies have focused on the chemistry of tropospheric halogen species which are able to deplete tropospheric ozone (O(3)). In this study, the effect of bromine and iodine chemistry on tropospheric O(3) within the annual cycle in Asia-Pacific is investigated using the CMAQ model with the newly embedded bromine and iodine chemistry and a blended and customized emission inventory considering marine halogen emission. Results indicate that the vertical profiles of bromine and iodine species show distinct features over land/ocean and daytime/nighttime, related to natural and anthropogenic emission distributions and photochemical reactions. The halogen-mediated O(3) loss has a strong seasonal cycle, and reaches a maximum of -15.9 ppbv (-44.3%) over the ocean and -13.4 ppbv (-38.9%) over continental Asia among the four seasons. Changes in solar radiation, dominant wind direction, and nearshore chlorophyll-a accumulation all contribute to these seasonal differences. Based on the distances to the nearest coastline, the onshore and offshore features of tropospheric O(3) loss caused by bromine and iodine chemistry are studied. Across a coastline-centric 400-km-wide belt from onshore to offshore, averaged maximum gradient of O(3) loss reaches 1.1 ppbv/100 km at surface level, while planetary boundary layer (PBL) column mean of O(3) loss is more moderate, being approximately 0.7 ppbv/100 km. Relative high halogen can be found over Tibetan Plateau (TP) and the largest O(3) loss (approximately 4-5 ppbv) in the PBL can be found between the western boundary of the domain and the TP. Halogens originating from marine sources can potentially affect O(3) concentration transported from the stratosphere over the TP region. As part of efforts to improve our understanding of the effect of bromine and iodine chemistry on tropospheric O(3), we call for more models and monitoring studies on halogen chemistry and be considered further in air pollution prevention and control policy.