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The terrestrial ecosystem is an integral component of the Earth System. Constant atmosphere-biosphere exchanges of energy and material affect both the physics and chemistry of the atmosphere. While the general roles of terrestrial ecosystems in regulating ozone and particulate matter air pollution have long been acknowledged, our understanding at both individual process and system level are far from perfect. Also, new process-level discoveries about terrestrial atmosphere-biosphere exchanges are not timely incorporated in numerical models routinely used to study and forecast air quality. These hinder our ability to understand how air quality respond to environmental changes and variabilities. Chapter 1 of this dissertation provides a brief overview on these topics. In Chapter 2 of this dissertation (Wong et al., 2019), we conduct global long-term simulations of ozone dry deposition velocity with four different types of dry deposition parameterizations. We find that none of the tested parameterizations universally stands out in terms of matching observed ozone deposition velocity over different land cover types. Combining this with sensitivity simulations from a global 3-D atmospheric chemistry model (GEOS-Chem), we find that the choice of dry deposition parameterizations can affect the mean, trend and variability of simulated surface O3 level. In Chapter 3 of this dissertation (Wong et al., 2022), we analyze long-term ozone flux observation from three field sites to examine the effects of extreme heat and dryness on ozone deposition. We find that non-stomatal ozone uptake tends to increase during hot days, which either partially offsets or dominates over the reduction in stomatal ozone uptake anticipated by ecophysiological theory. While the response of ozone deposition to dryness is more varied, changes in non-stomatal deposition are usually important. Current dry deposition parameterizations often fail to capture such changes in non-stomatal ozone uptake, resulting in considerable potential error in simulated surface ozone level during hot and dry days. In Chapter 4 of this dissertation (Wong and Geddes, 2021), we conduct global GEOS-Chem numerical experiments with anthropogenic emission inventories and land surface remote sensing products to compare the effects land cover versus land management changes on O3 and fine particulate matter air quality over 1992 – 2014. We find that land cover has stronger effects on O3, while land management has stronger effects on fine particulate matter pollution. We also find that land management has significantly altered regional and global nitrogen deposition, and therefore the risk of critical load exceedance. Chapter 5 of this dissertation includes the concluding remarks and suggestions for future work. In addition, I outline and present the preliminary result from a project examining the future of soil reactive nitrogen emissions and their impacts on air quality.