Source Attribution of Near-surface Ozone in the Western US: Improved Estimates by TF HTAP2 Multi-model Experiment and Multi-scale Chemical Data Assimilation
Friday, 19 December 2014
Near-surface ozone in the western US can be sensitive to transported background pollutants from the free troposphere over the eastern Pacific, as well as various local emissions sources. Accurately estimating ozone source contributions in this region has strong policy-relevant significance as the air quality standards tend to go down. Here we improve modeled contributions from local and non-local sources to western US ozone base on the HTAP2 (Task Force on Hemispheric Transport of Air Pollution) multi-model experiment, along with multi-scale chemical data assimilation. We simulate western US air quality using the STEM regional model on a 12 km horizontal resolution grid, during the NASA ARCTAS field campaign period in June 2008. STEM simulations use time-varying boundary conditions downscaled from global GEOS-Chem model simulations. Standard GEOS-Chem simulation overall underpredicted ozone at 1-5 km in the eastern Pacific, resulting in underestimated contributions from the transported background pollutants to surface ozone inland. These negative biases can be reduced by using the output from several global models that support the HTAP2 experiment, which all ran with the HTAP2 harmonized emission inventory and also calculated the contributions from east Asian anthropogenic emissions. We demonstrate that the biases in GEOS-Chem boundary conditions can be more efficiently reduced via assimilating satellite ozone profiles from the Tropospheric Emission Spectrometer (TES) instrument using the three dimensional variational (3D-Var) approach. Base upon these TES-constrained GEOS-Chem boundary conditions, we then update regional nitrogen dioxide and isoprene emissions in STEM through the four dimensional variational (4D-Var) assimilation of the Ozone Monitoring Instrument (OMI) nitrogen dioxide columns and the NASA DC-8 aircraft isoprene measurements. The 4D-Var assimilation spatially redistributed the emissions of nitrogen oxides and isoprene from various US sources, and in the meantime updated the modeled ozone and its US source contributions. Compared with available independent measurements (e.g., ozone observed on the DC-8 aircraft, and at EPA and Mt. Bachelor monitoring stations) during this period, modeled ozone fields after the multi-scale assimilation show overall improvement.