Multi-scale modeling study of the source contributions to near-surface ozone and sulfur oxides levels over California during the ARCTAS-CARB period

Chronic high surface ozone (O_3) levels and the increasing sulfur oxides (SO_x = SO_2 + SO_4) ambient concentrations over South Coast (SC) and other areas of California (CA) are affected by both local emissions and long-range transport. In this paper, multi-scale tracer, full-chemistry and adjoint simulations using the STEM atmospheric chemistry model are conducted to assess the contribution of local emission sourcesto SC O_3 and to evaluate the impacts of transported sulfur and local emissions on the SC sulfur budgetduring the ARCTAS-CARB experiment period in 2008. Sensitivity simulations quantify contributions of biogenic and fire emissions to SC O_3 levels. California biogenic and fire emissions contribute 3–4 ppb to near-surface O_3 over SC, with larger contributions to other regions in CA. During a long-range transport event from Asia starting from 22 June, high SO_x levels (up to ~0.7 ppb of SO_2 and ~1.3 ppb of SO_4) is observed above ~6 km, but they did not affect CA surface air quality. The elevated SO_x observed at 1–4 km is estimated to enhance surface SO_x over SC by ~0.25 ppb (upper limit) on ~24 June. The near-surface SO_x levels over SC during the flight week are attributed mostly to local emissions. Two anthropogenic SO_x emission inventories (EIs) from the California Air Resources Board (CARB) and the US Environmental Protection Agency (EPA) are compared and applied in 60 km and 12 km chemical transport simulations, and the results are compared withobservations. The CARB EI shows improvements over the National Emission Inventory (NEI) by EPA, but generally underestimates surface SC SO_x by about a factor of two. Adjoint sensitivity analysis indicated that SO_2 levels at 00:00 UTC (17:00 local time) at six SC surface sites were influenced by previous day maritime emissions over the ocean, the terrestrial emissions over nearby urban areas, and by transported SO_2 from the north through both terrestrial and maritime areas. Overall maritime emissions contribute 10–70% of SO2 and 20–60% fine SO_4 on-shore and over the most terrestrial areas, with contributions decreasing with in-land distance from the coast. Maritime emissions also modify the photochemical environment, shifting O_3 production over coastal SC to more VOC-limited conditions. These suggest an important role for shipping emission controls in reducing fine particle and O_3 concentrations in SC

Impacts of transported background ozone on California air quality during the ARCTAS-CARB period – a multi-scale modeling study

Multi-scale tracer and full-chemistry simulations with the STEM atmospheric chemistry model are used to analyze the effects of transported background ozone (O<sub>3</sub>) from the eastern Pacific on California air quality during the ARCTAS-CARB experiment conducted in June, 2008. Previous work has focused on the importance of long-range transport of O<sub>3</sub> to North America air quality in springtime. However during this summer experiment the long-range transport of O<sub>3</sub> is also shown to be important. Simulated and observed O<sub>3</sub> transport patterns from the coast to inland northern California are shown to vary based on meteorological conditions and the O<sub>3</sub> profiles over the oceans, which are strongly episodically affected by Asian inflows. Analysis of the correlations of O<sub>3</sub> at various altitudes above the coastal site at Trinidad Head and at a downwind surface site in northern California, show that under long-range transport events, high O<sub>3</sub> air-masses (O<sub>3</sub>>60 ppb) at altitudes between about 2 and 4 km can be transported inland and can significantly influence surface O<sub>3</sub> 20–30 h later. These results show the importance of characterizing the vertical structure of the lateral boundary conditions (LBC) needed in air quality simulations. The importance of the LBC on O<sub>3</sub> prediction during this period is further studied through a series of sensitivity studies using different forms of LBC. It is shown that the use of the LBC downscaled from RAQMS global model that assimilated MLS and OMI data improves the model performance. We also show that the predictions can be further improved through the use of LBC based on NASA DC-8 airborne observations during the ARCTAS-CARB experiment. These results indicate the need to develop observational strategies to provide information on the three-dimensional nature of pollutant distributions, in order to improve our capability to predict pollution levels and to better quantify the influence of these Asian inflows on the US west coast air quality

Source sector and region contributions to BC and PM2.5 in Central Asia

Particulate matter (PM) mass concentrations, seasonal cycles, source sector, and source region contributions in Central Asia (CA) are analyzed for the period April 2008–July 2009 using the Sulfur Transport and dEposition Model (STEM) chemical transport model and modeled meteorology from the Weather Research and Forecasting (WRF) model. Predicted aerosol optical depth (AOD) values (annual mean value 0.2) in CA vary seasonally, with lowest values in the winter. Surface PM2:5 concentrations (annual mean value 10 μgm3/ also exhibit a seasonal cycle, with peak values and largest variability in the spring/summer, and lowest values and variability in the winter (hourly values from 2 to 90 μgm3/. Surface concentrations of black carbon (BC) (mean value 0.1 μgm3/ show peak values in the winter. The simulated values are compared to surface measurements of AOD as well as PM2:5, PM10, BC, and organic carbon (OC) mass concentrations at two regional sites in Kyrgyzstan (Lidar Station Teplokluchenka (LST) and Bishkek). The predicted values of AOD and PM mass concentrations and their seasonal cycles are fairly well captured. The carbonaceous aerosols are underpredicted in winter, and analysis suggests that the winter heating emissions are underestimated in the current inventory. Dust, from sources within and outside CA, is a significant component of the PM mass and drives the seasonal cycles of PM and AOD. On an annual basis, the power and industrial sectors are found to be the most important contributors to the anthropogenic portion of PM2:5. Residential combustion and transportation are shown to be the most important sectors for BC. Biomass burning within and outside the region also contributes to elevated PM and BC concentrations. The analysis of the transport pathways and the variations in particulate matter mass and composition in CA demonstrates that this region is strategically located to characterize regional and intercontinental transport of pollutants. Aerosols at these sites are shown to reflect dust, biomass burning, and anthropogenic sources from Europe; South, East, and Central Asia; and Russia depending on the time period. Simulations for a reference 2030 emission scenario based on pollution abatement measures already committed to in current legislation show that PM2:5 and BC concentrations in the region increase, with BC growing more than PM2:5 on a relative basis. This suggests that both the health impacts and the climate warming associated with these particles may increase over the next decades unless additional control measures are taken. The importance of observations in CA to help characterize the changes that are rapidly taking place in the region are discussed.JRC.H.2-Air and Climat

Source sector and region contributions to BC and PM2.5 in Central Asia

Particulate matter (PM) mass concentrations, seasonal cycles, source sector, and source region contributions in Central Asia (CA) are analyzed for the period April 2008-July 2009 using the Sulfur Transport and dEposition Model (STEM) chemical transport model and modeled meteorology from the Weather Research and Forecasting (WRF) model. Predicted aerosol optical depth (AOD) values (annual mean value ~0.2) in CA vary seasonally, with lowest values in the winter. Surface PM2.5 concentrations (annual mean value ~10 μg m&3) also exhibit a seasonal cycle, with peak values and largest variability in the spring/summer, and lowest values and variability in the winter (hourly values from 2 to 90 μg m&3). Surface concentrations of black carbon (BC) (mean value ~0.1 μg m&3) show peak values in the winter. The simulated values are compared to surface measurements of AOD as well as PM2.5, PM10, BC, and organic carbon (OC) mass concentrations at two regional sites in Kyrgyzstan (Lidar Station Teplokluchenka (LST) and Bishkek). The predicted values of AOD and PM mass concentrations and their seasonal cycles are fairly well captured. The carbonaceous aerosols are underpredicted in winter, and analysis suggests that the winter heating emissions are underestimated in the current inventory. Dust, from sources within and outside CA, is a significant component of the PM mass and drives the seasonal cycles of PM and AOD. On an annual basis, the power and industrial sectors are found to be the most important contributors to the anthropogenic portion of PM2.5. Residential combustion and transportation are shown to be the most important sectors for BC. Biomass burning within and outside the region also contributes to elevated PM and BC concentrations. The analysis of the transport pathways and the variations in particulate matter mass and composition in CA demonstrates that this region is strategically located to characterize regional and intercontinental transport of pollutants. Aerosols at these sites are shown to reflect dust, biomass burning, and anthropogenic sources from Europe; South, East, and Central Asia; and Russia depending on the time period. Simulations for a reference 2030 emission scenario based on pollution abatement measures already committed to in current legislation show that PM2.5 and BC concentrations in the region increase, with BC growing more than PM2.5 on a relative basis. This suggests that both the health impacts and the climate warming associated with these particles may increase over the next decades unless additional control measures are taken. The importance of observations in CA to help characterize the changes that are rapidly taking place in the region are discussed. © 2015 Atmos. Chem. Phys