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

摘要

The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (Osub3/sub) 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 Osub3/sub 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 Osub3/sub 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 Osub3/sub 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 Osub3/sub sensitivities to a 20?% reduction in the EAS anthropogenic emissions may be underestimated by at least 10?%. The three boundary condition models' mean Osub3/sub sensitivities to the 20?% EAS emission perturbations are ～?8?% (May–June?2010)/～?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 NOsubix/i/sub emissions matter more than the other EAS Osub3/sub precursors to the North American Osub3/sub, qualitatively consistent with previous adjoint sensitivity calculations.brbr In addition to the analyses on large spatial–temporal scales relative to the HTAP1, we also show results on subcontinental and event scales that are more relevant to the US air quality management. The EAS pollution impacts are weaker during observed Osub3?/subexceedances than on all days in most US regions except over some high-terrain western US rural/remote areas. Satellite Osub3/sub (TES, JPL–IASI, and AIRS) and carbon monoxide (TES and AIRS) products, along with surface measurements and model calculations, show that during certain episodes stratospheric Osub3/sub intrusions and the transported EAS pollution influenced Osub3/sub in the western and the eastern US differently. Free-running (i.e., without chemical data assimilation) global models underpredicted the transported background Osub3/sub during these episodes, posing difficulties for STEM to accurately simulate the surface Osub3/sub and its source contribution. Although we effectively improved the modeled Osub3/sub by incorporating satellite Osub3/sub (OMI and MLS) and evaluated the quality of the HTAP2 emission inventory with the Royal Netherlands Meteorological Institute–Ozone Monitoring Instrument (KNMI–OMI) nitrogen dioxide, using observations to evaluate and improve Osub3/sub