Impact of intercontinental pollution transport on North American ozone air pollution: an HTAP phase 2 multi-model study

The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (O-3 / can benefit from a better understanding of its source contributions in different US regions during recent years. In the Hemispheric Transport of Air Pollution experiment phase 1 (HTAP1), various global models were used to determine the O3 source-receptor (SR) relationships among three continents in the Northern Hemisphere in 2001. In support of the HTAP phase 2 (HTAP2) experiment that studies more recent years and involves higher-resolution global models and regional models' participation, we conduct a number of regional-scale Sulfur Transport and dEposition Model (STEM) air quality base and sensitivity simulations over North America during May-June 2010. STEM's top and lateral chemical boundary conditions were downscaled from three global chemical transport models' (i. e., GEOS-Chem, RAQMS, and ECMWF C-IFS) base and sensitivity simulations in which the East Asian (EAS) anthropogenic emissions were reduced by 20 %. The mean differences between STEM surface O3 sensitivities to the emission changes and its corresponding boundary condition model's are smaller than those among its boundary condition models, in terms of the regional/ period-mean (< 10 %) and the spatial distributions. An additional STEM simulation was performed in which the boundary conditions were downscaled from a RAQMS (Realtime Air Quality Modeling System) simulation without EAS anthropogenic emissions. The scalability of O3 sensitivities to the size of the emission perturbation is spatially varying, and the full (i. e., based on a 100% emission reduction) source contribution obtained from linearly scaling the North American mean O-3 sensitivities to a 20% reduction in the EAS anthropogenic emissions may be underestimated by at least 10 %. The three boundary condition models' mean O-3 sensitivities to the 20% EAS emission perturbations are similar to 8%(May-June 2010)/similar to 11%(2010 annual) lower than those estimated by eight global models, and the multi-model ensemble estimates are higher than the HTAP1 reported 2001 conditions. GEOS-Chem sensitivities indicate that the EAS anthropogenic NOx emissions matter more than the other EAS O3 precursors to the North American O-3, qualitatively consistent with previous adjoint sensitivity calculations.