Understanding the exchange processes between the atmospheric boundary layer and the free troposphere is crucial for estimating hemispheric transport of air pollution. Most studies of hemispheric air pollution transport have taken a large-scale perspective using global chemical transport models with fairly coarse spatial and temporal resolutions. In support of United Nations Task Force on Hemispheric Transport of Air Pollution (TF HTAP; www.htap.org), this study employs two high-resolution atmospheric chemistry models (WRF-Chem and CMAQ; 3636 km) driven with chemical boundary conditions from a global model (MOZART; 1.91.9) to examine the role of fine-scale transport and chemistry processes in controlling pollution export and import over the Asian continent in spring (March 2001). Our analysis indicates the importance of rapid venting through deep convection that develops along the leading edge of frontal system convergence bands, which are not adequately resolved in either of two global models compared with TRACE-P aircraft observations during a frontal event. Both regional model simulations and observations show that frontal outflows of CO, O3 and PAN can extend to the upper troposphere (6–9 km). Pollution plumes in the global MOZART model are typically diluted and insufficiently lofted to higher altitudes where they can undergo more efficient transport in stronger winds. We use sensitivity simulations that perturb chemical boundary conditions in the CMAQ regional model to estimate that the O3 production over East Asia (EA) driven by PAN decomposition contributes 20% of the spatial averaged total O3 response to European (EU) emission perturbations in March, and occasionally contributes approximately 50% of the total O3 response in subsiding plumes at mountain observatories (at approximately 2 km altitude). The response to decomposing PAN of EU origin is strongly affected by the O3 formation chemical regimes, which vary with the model chemical mechanism and NOx/VOC emissions. Our high-resolution models demonstrate a large spatial variability (by up to a factor of 6) in the response of local O3 to 20% reductions in EU anthropogenic O3 precursor emissions. The response in the highly populated Asian megacities is 40–50% lower in our high-resolution models than the global model, suggesting that the source-receptor relationships inferred from the global coarse-resolution models likely overestimate health impacts associated with intercontinental O3 transport. Our results highlight the important roles of rapid convective transport, orographic forcing, urban photochemistry and heterogeneous boundary layer processes in controlling intercontinental transport; these processes may not be well resolved in the large-scale models.
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