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Concentrations of both fine particulate matter (PM2.5) and ozone (O3) in the United States (US) have decreased significantly since 1990, mainly because of air quality regulations. Exposure to these air pollutants is associated with premature death. Here we quantify the annual mortality burdens from PM2.5 and O3 in the US from 1990 to 2010, estimate trends and inter-annual variability, and evaluate the contributions to those trends from changes in pollutant concentrations, population, and baseline mortality rates. We use a fine-resolution (36 km) self-consistent 21-year simulation of air pollutant concentrations in the US from 1990 to 2010, a health impact function, and annual county-level population and baseline mortality rate estimates. From 1990 to 2010, the modeled population-weighted annual PM2.5 decreased by 39 %, and summertime (April to September) 1 h average daily maximum O3 decreased by 9 % from 1990 to 2010. The PM2.5-related mortality burden from ischemic heart disease, chronic obstructive pulmonary disease, lung cancer, and stroke steadily decreased by 54 % from 123 700 deaths year−1 (95 % confidence interval, 70 800–178 100) in 1990 to 58 600 deaths year−1 (24 900–98 500) in 2010. The PM2.5-related mortality burden would have decreased by only 24 % from 1990 to 2010 if the PM2.5 concentrations had stayed at the 1990 level, due to decreases in baseline mortality rates for major diseases affected by PM2.5. The mortality burden associated with O3 from chronic respiratory disease increased by 13 % from 10 900 deaths year−1 (3700–17 500) in 1990 to 12 300 deaths year−1 (4100–19 800) in 2010, mainly caused by increases in the baseline mortality rates and population, despite decreases in O3 concentration. The O3-related mortality burden would have increased by 55 % from 1990 to 2010 if the O3 concentrations had stayed at the 1990 level. The detrended annual O3 mortality burden has larger inter-annual variability (coefficient of variation of 12 %) than the PM2.5-related burden (4 %), mainly from the inter-annual variation of O3 concentration. We conclude that air quality improvements have significantly decreased the mortality burden, avoiding roughly 35 800 (38 %) PM2.5-related deaths and 4600 (27 %) O3-related deaths in 2010, compared to the case if air quality had stayed at 1990 levels (at 2010 baseline mortality rates and population).

Downward transport of ozone (O3) from the stratosphere can be a significant contributor to tropospheric O3 background levels. However, this process often is not well represented in current regional models. In this study, we develop a seasonally and spatially varying potential vorticity (PV)-based function to parameterize upper tropospheric and/or lower stratospheric (UTLS) O3 in a chemistry transport model. This dynamic O3–PV function is developed based on 21-year ozonesonde records from World Ozone and Ultraviolet Radiation Data Centre (WOUDC) with corresponding PV values from a 21-year Weather Research and Forecasting (WRF) simulation across the Northern Hemisphere from 1990 to 2010. The result suggests strong spatial and seasonal variations of O3 ∕ PV ratios which exhibits large values in the upper layers and in high-latitude regions, with highest values in spring and the lowest values in autumn over an annual cycle. The newly developed O3 ∕ PV function was then applied in the Community Multiscale Air Quality (CMAQ) model for an annual simulation of the year 2006. The simulated UTLS O3 agrees much better with observations in both magnitude and seasonality after the implementation of the new parameterization. Considerable impacts on surface O3 model performance were found in the comparison with observations from three observational networks, i.e., EMEP, CASTNET and WDCGG. With the new parameterization, the negative bias in spring is reduced from −20 to −15 % in the reference case to −9 to −1 %, while the positive bias in autumn is increased from 1 to 15 % in the reference case to 5 to 22 %. Therefore, the downward transport of O3 from upper layers has large impacts on surface concentration and needs to be properly represented in regional models.

Long-term simulations with the coupled WRF–CMAQ (Weather Research and Forecasting–Community Multi-scale Air Quality) model have been conducted to systematically investigate the changes in anthropogenic emissions of SO2 and NOx over the past 16 years (1995–2010) across the United States (US), their impacts on anthropogenic aerosol loading over North America, and subsequent impacts on regional radiation budgets. In particular, this study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act (CAA) especially on trends in solar radiation. Extensive analyses conducted by Gan et al. (2014a) utilizing observations (e.g., SURFRAD, CASTNET, IMPROVE, and ARM) over the past 16 years (1995–2010) indicate a shortwave (SW) radiation (both all-sky and clear-sky) "brightening" in the US. The relationship of the radiation brightening trend with decreases in the aerosol burden is less apparent in the western US. One of the main reasons for this is that the emission controls under the CAA were aimed primarily at reducing pollutants in areas violating national air quality standards, most of which were located in the eastern US, while the relatively less populated areas in the western US were less polluted at the beginning of this study period. Comparisons of model results with observations of aerosol optical depth (AOD), aerosol concentration, and radiation demonstrate that the coupled WRF–CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD. In particular, the sulfate concentration predictions were well matched with the observations. The discrepancies found in the clear-sky diffuse SW radiation are likely due to several factors such as the potential increase of ice particles associated with increasing air traffic, the definition of "clear-sky" in the radiation retrieval methodology, and aerosol semi-direct and/or indirect effects which cannot be readily isolated from the observed data.

The ability of a coupled meteorology–chemistry model, i.e., Weather Research and Forecast and Community Multiscale Air Quality (WRF-CMAQ), to reproduce the historical trend in aerosol optical depth (AOD) and clear-sky shortwave radiation (SWR) over the Northern Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Six satellite-retrieved AOD products including AVHRR, TOMS, SeaWiFS, MISR, MODIS-Terra and MODIS-Aqua as well as long-term historical records from 11 AERONET sites were used for the comparison of AOD trends. Clear-sky SWR products derived by CERES at both the top of atmosphere (TOA) and surface as well as surface SWR data derived from seven SURFRAD sites were used for the comparison of trends in SWR. The model successfully captured increasing AOD trends along with the corresponding increased TOA SWR (upwelling) and decreased surface SWR (downwelling) in both eastern China and the northern Pacific. The model also captured declining AOD trends along with the corresponding decreased TOA SWR (upwelling) and increased surface SWR (downwelling) in the eastern US, Europe and the northern Atlantic for the period of 2000–2010. However, the model underestimated the AOD over regions with substantial natural dust aerosol contributions, such as the Sahara Desert, Arabian Desert, central Atlantic and northern Indian Ocean. Estimates of the aerosol direct radiative effect (DRE) at TOA are comparable with those derived by measurements. Compared to global climate models (GCMs), the model exhibits better estimates of surface-aerosol direct radiative efficiency (Eτ). However, surface-DRE tends to be underestimated due to the underestimated AOD in land and dust regions. Further investigation of TOA-Eτ estimations as well as the dust module used for estimates of windblown-dust emissions is needed.

Trends in air quality across the Northern Hemisphere over a 21-year period (1990–2010) were simulated using the Community Multiscale Air Quality (CMAQ) multiscale chemical transport model driven by meteorology from Weather Research and Forecasting (WRF) simulations and internally consistent historical emission inventories obtained from EDGAR. Thorough comparison with several ground observation networks mostly over Europe and North America was conducted to evaluate the model performance as well as the ability of CMAQ to reproduce the observed trends in air quality over the past 2 decades in three regions: eastern China, the continental United States and Europe. The model successfully reproduced the observed decreasing trends in SO2, NO2, 8 h O3 maxima, SO42− and elemental carbon (EC) in the US and Europe. However, the model fails to reproduce the decreasing trends in NO3− in the US, potentially pointing to uncertainties of NH3 emissions. The model failed to capture the 6-year trends of SO2 and NO2 in CN-API (China – Air Pollution Index) from 2005 to 2010, but reproduced the observed pattern of O3 trends shown in three World Data Centre for Greenhouse Gases (WDCGG) sites over eastern Asia. Due to the coarse spatial resolution employed in these calculations, predicted SO2 and NO2 concentrations are underestimated relative to all urban networks, i.e., US-AQS (US – Air Quality System; normalized mean bias (NMB) = −38% and −48%), EU-AIRBASE (European Air quality data Base; NMB = −18 and −54%) and CN-API (NMB = −36 and −68%). Conversely, at the rural network EU-EMEP (European Monitoring and Evaluation Programme), SO2 is overestimated (NMB from 4 to 150%) while NO2 is simulated well (NMB within ±15%) in all seasons. Correlations between simulated and observed O3 wintertime daily 8 h maxima (DM8) are poor compared to other seasons for all networks. Better correlation between simulated and observed SO42− was found compared to that for SO2. Underestimation of summer SO42− in the US may be associated with the uncertainty in precipitation and associated wet scavenging representation in the model. The model exhibits worse performance for NO3− predictions, particularly in summer, due to high uncertainties in the gas/particle partitioning of NO3− as well as seasonal variations of NH3 emissions. There are high correlations (R > 0.5) between observed and simulated EC, although the model underestimates the EC concentration by 65% due to the coarse grid resolution as well as uncertainties in the PM speciation profile associated with EC emissions. The almost linear response seen in the trajectory of modeled O3 changes in eastern China over the past 2 decades suggests that control strategies that focus on combined control of NOx and volatile organic compound (VOC) emissions with a ratio of 0.46 may provide the most effective means for O3 reductions for the region devoid of nonlinear response potentially associated with NOx or VOC limitation resulting from alternate strategies. The response of O3 is more sensitive to changes in NOx emissions in the eastern US because the relative abundance of biogenic VOC emissions tends to reduce the effectiveness of VOC controls. Increasing NH3 levels offset the relative effectiveness of NOx controls in reducing the relative fraction of aerosol NO3− formed from declining NOx emissions in the eastern US, while the control effectiveness was assured by the simultaneous control of NH3 emission in Europe.

Long-term data sets of all-sky and clear-sky downwelling shortwave (SW) radiation, cloud cover fraction, and aerosol optical depth (AOD) were analyzed together with surface concentrations from several networks (e.g., Surface Radiation Budget Network (SURFRAD), Clean Air Status and Trend Network (CASTNET), Interagency Monitoring of Protection Visual Environments (IMPROVE) and Atmospheric Radiation Measurement (ARM)) in the United States (US). Seven states with varying climatology were selected to better understand the effects of aerosols and clouds on SW radiation. This analysis aims to assess the effects of reductions in anthropogenic aerosol burden resulting from substantial reductions in emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) over the past 16 yr across the US, based on trends in SW radiation. The SO2 and NOx emission data show decreasing trends from 1995 to 2010, which indirectly validates the effects of the Clean Air Act (CAA) in the US. Meanwhile, the total column AOD and surface total PM2.5 observations also show decreasing trends in the eastern US but slightly increasing trends in the western US. Moreover, measured surface concentrations of several other pollutants (i.e., SO2, SO4 and NOx) have similar behavior to AOD and total PM2.5. Analysis of the observed data shows strong increasing trends in all-sky downwelling SW radiation with decreasing trends in cloud cover. However, since observations of both all-sky direct and diffuse SW radiation show increasing trends, there may be other factors contributing to the radiation trends in addition to the decreasing trends in overall cloud cover. To investigate the role of direct radiative effects of aerosols, clear-sky downwelling radiation is analyzed so that cloud effects are eliminated. However, similar increasing trends in clear-sky total and diffuse SW radiation are observed. While significantly decreasing trends in AOD and surface PM2.5 concentrations along with increasing SW radiation (both all-sky and clear-sky) in the eastern US during 1995–2010 imply the occurrence of direct aerosol mediated "brightening", the increasing trends of both all-sky and clear-sky diffuse SW radiation contradicts this conclusion since diffuse radiation would be expected to decrease as aerosols direct effects decrease and cloud cover decreases. After investigating several confounding factors, the increasing trend in clear-sky diffuse SW may be due to more high-level cirrus from increasing air traffic over the US. The clear-sky radiation observations in the western US also show indications of "brightening" even though the AOD, PM2.5 and surface concentration do not vary drastically. This outcome was not unexpected because the CAA controls were mainly aimed at reducing air pollutant emissions in the eastern US and air pollutant levels in the western US were much lower at the onset. This suggests other factors affect the "brightening" especially in the western US.

An accurate description of emissions is crucial for model simulations to reproduce and interpret observed phenomena over extended time periods. In this study, we used an approach based on activity data to develop a consistent series of spatially resolved emissions in the United States from 1990 to 2010. The state-level anthropogenic emissions of SO2, NOx, CO, NMVOC (non-methane volatile organic compounds), NH3, PM10 and PM2.5 for a total of 49 sectors were estimated based on several long-term databases containing information about activities and emission controls. Activity data for energy-related stationary sources were derived from the State Energy Data System. Corresponding emission factors reflecting implemented emission controls were calculated back from the National Emissions Inventory (NEI) for seven years (i.e., 1990, 1995, 1996, 1999, 2001, 2002 and 2005), and constrained by the AP-42 (US EPA's Compilation of Air Pollutant Emissions Factors) dataset. Activity data for mobile sources including different types of highway vehicles and non-highway equipment were obtained from highway statistics reported by the Federal Highway Administration. The trends in emission factors for highway mobile source were informed by the 2011 National Transportation Statistics. Emissions for all non-energy-related sources were either scaled by the growth ratio of activity indicators or adjusted based on the NEI trends report. Because of the strengthened control efforts, particularly for the power sector and mobile sources, emissions of all pollutants except NH3 were reduced by half over the last two decades. The emission trends developed in this study are comparable with the NEI trend report and EDGAR (Emissions Database for Global Atmospheric Research) data, but better constrained by trends in activity data. Reductions in SO2, NOx, CO and EC (speciation of PM2.5 by SMOKE, Sparse Matrix Operator Kernel Emissions) emissions agree well with the observed changes in ambient SO2, NO2, CO and EC concentrations, suggesting that the various controls on emissions implemented over the last two decades are well represented in the emission inventories developed in this study. These inventories were processed by SMOKE and are now ready to be used for regional chemistry transport model simulations over the 1990–2010 period.

Long term datasets of all-sky and clear-sky downwelling shortwave (SW) radiation, cloud cover fraction and aerosol optical depth (AOD) are analyzed together with surface concentration from several networks (e.g. SURFRAD, CASTNET, IMPROVE and ARM) in the United States (US). Seven states with varying climatology are selected to better understand the effects of aerosols and clouds on SW radiation. This analysis aims to assess the effects of reductions in anthropogenic aerosol burden resulting from substantial reductions in emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) over the past 16 yr across the US on trends in SW radiation. The SO2 and NOx emission data show decreasing trends from 1995 to 2010 which indirectly validates the effects of the Clean Air Act (CAA) in the US. Meanwhile, the total column AOD and surface total PM2.5 observations also show decreasing trends in the eastern US but slightly increasing trends in the western US. Moreover, measured surface concentrations of several other pollutants (i.e. SO2, SO4 and NOx) have the same behavior as the AOD and total PM2.5. First, all-sky downwelling SW radiation is assessed together with the cloud cover. Results of this analysis show strong increasing trends in all-sky downwelling SW radiation with decreasing trends in cloud cover. However, since observations of both all-sky direct and diffuse SW radiation are increasing, there may be other factors contributing to the radiation trends in addition to the decreasing trends in overall cloud cover. To investigate the role of direct radiative effects of aerosols, clearsky downwelling radiation is analyzed so that cloud effects are eliminated. However, similar increasing trends in clear-sky direct and diffuse SW radiation are observed. While significantly decreasing trends in AOD and surface concentration along with increasing SW radiation (both all-sky and clear-sky) in the eastern US during 1995-2010 imply the occurrence of direct aerosol mediated "brightening", the increasing trends of both all-sky and clear sky diffuse SW radiation contradicts this conclusion since diffuse radiation would be expected to decrease as aerosols direct effects decrease. After investigating several confounding factors, the increasing trend in diffuse SW may be due to more high-level cirrus from increasing air traffic over the US. In contrast to the eastern US, radiation observations in the western US do not show any indication of "brightening" which is consistent with the observations (e.g. AOD, PM2.5 and surface concentration) that show the aerosol loading increasing slightly. This outcome is not unexpected because the CAA controls were mainly aimed at reducing air pollutants emission in the eastern US and air pollutant level in the western US are much lower. [ABSTRACT FROM AUTHOR]