ALBERT

Description: We show that the frequency of summertime mid-latitude cyclones tracking across eastern North America at 40°–50° N (the southern climatological storm track) is a strong predictor of stagnation and ozone pollution episodes in the eastern United States. The NCEP/NCAR Reanalysis, going back to 1948, shows a significant long-term decline in the number of summertime mid-latitude cyclones in that track starting in 1980 (−0.15 a-1). The more recent but shorter NCEP/DOE Reanalysis (1979–2006) shows similar interannual variability in cyclone frequency but no significant long-term trend. A GISS general circulation model (GCM) simulation including historical forcing by greenhouse gases reproduces the cyclone trend seen in the NCEP/NCAR data. Such a long-term decrease in mid-latitude cyclone frequency over the 1980–2006 period would have offset by about a factor of 2 the ozone air quality gains from reductions in anthropogenic emissions in the northeastern United States. We find that if mid-latitude cyclone frequency had not declined, the northeastern US would have been largely compliant with the ozone air quality standard by 2001. Mid-latitude cyclone frequency is expected to decrease further over the coming decades in response to greenhouse warming and this trend needs to be considered in air quality management.

Description: We show that the frequency of summertime mid-latitude cyclones tracking across eastern North America at 40°–50° N (the southern climatological storm track) is a strong predictor of stagnation and ozone pollution days in the eastern US. The NCEP/NCAR Reanalysis, going back to 1948, shows a significant long-term decline in the number of summertime mid-latitude cyclones in that track starting in 1980 (−0.15 a−1). The more recent but shorter NCEP/DOE Reanalysis (1979–2006) shows similar interannual variability in cyclone frequency but no significant long-term trend. Analysis of NOAA daily weather maps for 1980–2006 supports the trend detected in the NCEP/NCAR Reanalysis 1. A GISS general circulation model (GCM) simulation including historical forcing by greenhouse gases reproduces this decreasing cyclone trend starting in 1980. Such a long-term decrease in mid-latitude cyclone frequency over the 1980–2006 period may have offset by half the ozone air quality gains in the northeastern US from reductions in anthropogenic emissions. We find that if mid-latitude cyclone frequency had not declined, the northeastern US would have been largely compliant with the ozone air quality standard by 2001. Mid-latitude cyclone frequency is expected to decrease further over the coming decades in response to greenhouse warming and this will necessitate deeper emission reductions to achieve a given air quality goal.

Description: Studies of the effect of climate change on fine particulate matter (PM2.5 air quality using general circulation models (GCMs) show inconsistent results including in the sign of the effect. This reflects uncertainty in the GCM simulations of the regional meteorological variables affecting PM2.5. Here we use the CMIP3 archive of data from fifteen different IPCC AR4 GCMs to obtain improved statistics of 21st-century trends in the meteorological modes driving PM2.5 variability over the contiguous US. We analyze 1999–2010 observations to identify the dominant meteorological modes driving interannual PM2.5 variability and their synoptic periods T. We find robust correlations (r 〉 0.5) of annual mean PM2.5 with T, especially in the eastern US where the dominant modes represent frontal passages. The GCMs all have significant skill in reproducing present-day statistics for T and we show that this reflects their ability to simulate atmospheric baroclinicity. We then use the local PM2.5-to-period sensitivity (dPM2.5/dT) from the 1999–2010 observations to project PM2.5 changes from the 2000–2050 changes in T simulated by the 15 GCMs following the SRES A1B greenhouse warming scenario. By weighted-average statistics of GCM results we project a likely 2000–2050 increase of ~ 0.1 μg m−3 in annual mean PM2.5 in the eastern US arising from less frequent frontal ventilation, and a likely decrease albeit with greater inter-GCM variability in the Pacific Northwest due to more frequent maritime inflows. Potentially larger regional effects of 2000–2050 climate change on PM2.5 may arise from changes in temperature, biogenic emissions, wildfires, and vegetation, but are still unlikely to affect annual PM2.5 by more than 0.5 μg m−3.

Description: We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by

Description: Simulations of present and future average regional ozone and PM2.5 concentrations over the United States were performed to investigate the potential impacts of global climate change and emissions on regional air quality using CMAQ. Various emissions and climate conditions with different biogenic emissions and domain resolutions were implemented to study the sensitivity of future air quality trends from the impacts of changing biogenic emissions. A comparison of GEOS-Chem and CMAQ was performed to investigate the effect of downscaling on the prediction of future air quality trends. For ozone, the impacts of global climate change are relatively smaller when compared to the impacts of anticipated future emissions reduction, except for the Northeast area, where increasing biogenic emissions due to climate change have stronger positive effects (increases) to the regional ozone air quality. The combination effect from both climate change and emission reductions leads to approximately a 10 % or 5 ppbv decrease of the maximum daily average eight-hour ozone (MDA8) over the Eastern United States. For PM2.5, the impacts of global climate change have shown insignificant effect, where as the impacts of anticipated future emissions reduction account for the majority of overall PM2.5 reductions. The annual average 24-h PM2.5 of the future-year condition was found to be about 40 % lower than the one from the present-year condition, of which 60 % of its overall reductions are contributed to by the decrease of SO4 and NO3 particulate matters. Changing the biogenic emissions model increases the MDA8 ozone by about 5–10 % or 3–5 ppbv in the Northeast area. Conversely, it reduces the annual average PM2.5 by 5 % or 1.0 μg m−3 in the Southeast region.

Description: The effects of future land use and land cover change on the chemical composition of the atmosphere and air quality are largely unknown. To investigate the potential effects associated with future changes in vegetation driven by atmospheric CO2 concentrations, climate, and anthropogenic land use over the 21st century, we performed a series of model experiments combining a general circulation model with a dynamic global vegetation model and an atmospheric chemical-transport model. Our results indicate that climate- and CO2-induced changes in vegetation composition and density between 2100 and 2000 could lead to decreases in summer afternoon surface ozone of up to 10 ppb over large areas of the northern mid-latitudes. This is largely driven by the substantial increases in ozone dry deposition associated with increases in vegetation density in a warmer climate with higher atmospheric CO2 abundance. Climate-driven vegetation changes over the period 2000–2100 lead to general increases in isoprene emissions, globally by 15% in 2050 and 36% in 2100. These increases in isoprene emissions result in decreases in surface ozone concentrations where the NOx levels are low, such as in remote tropical rainforests. However, over polluted regions, such as the northeastern United States, ozone concentrations are calculated to increase with higher isoprene emissions in the future. Increases in biogenic emissions also lead to higher concentrations of secondary organic aerosols, which increase globally by 10% in 2050 and 20% in 2100. Summertime surface concentrations of secondary organic aerosols are calculated to increase by up to 1 μg m−3 and double for large areas in Eurasia over the period of 2000–2100. When we use a scenario of future anthropogenic land use change, we find less increase in global isoprene emissions due to replacement of higher-emitting forests by lower-emitting cropland. The global atmospheric burden of secondary organic aerosols changes little by 2100 when we account for future land use change, but both secondary organic aerosols and ozone show large regional changes at the surface.

Description: We applied a multiple linear regression model to understand the relationships of PM2.5 with meteorological variables in the contiguous US and from there to infer the sensitivity of PM2.5 to climate change. We used 2004–2008 PM2.5 observations from ~1000 sites (~200 sites for PM2.5 components) and compared to results from the GEOS-Chem chemical transport model (CTM). All data were deseasonalized to focus on synoptic-scale correlations. We find strong positive correlations of PM2.5 components with temperature in most of the US, except for nitrate in the Southeast where the correlation is negative. Relative humidity (RH) is generally positively correlated with sulfate and nitrate but negatively correlated with organic carbon. GEOS-Chem results indicate that most of the correlations of PM2.5 with temperature and RH do not arise from direct dependence but from covariation with synoptic transport. We applied principal component analysis and regression to identify the dominant meteorological modes controlling PM2.5 variability, and show that 20–40% of the observed PM2.5 day-to-day variability can be explained by a single dominant meteorological mode: cold frontal passages in the eastern US and maritime inflow in the West. These and other synoptic transport modes drive most of the overall correlations of PM2.5 with temperature and RH except in the Southeast. We show that interannual variability of PM2.5 in the US Midwest is strongly correlated with cyclone frequency as diagnosed from a spectral-autoregressive analysis of the dominant meteorological mode. An ensemble of five realizations of 1996–2050 climate change with the GISS general circulation model (GCM) using the same climate forcings shows inconsistent trends in cyclone frequency over the Midwest (including in sign), with a likely decrease in cyclone frequency implying an increase in PM2.5. Our results demonstrate the need for multiple GCM realizations (because of climate chaos) when diagnosing the effect of climate change on PM2.5, and suggest that analysis of meteorological modes of variability provides a computationally more affordable approach for this purpose than coupled GCM-CTM studies.

Description: We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950–2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970–1990, with values over the eastern US (east of 100° W) of −2.0 W m−2 for direct forcing including contributions from sulfate (−2.0 W m−2), nitrate (−0.2 W m−2), organic carbon (−0.2 W m−2), and black carbon (+0.4 W m−2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50%. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3 W m−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

Description: We investigate projected 2000–2050 changes in concentrations of aerosols in China and the associated transboundary aerosol transport by using the chemical transport model GEOS-Chem driven by the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 3 at 4° × 5° resolution. Future changes in climate and emissions projected by the IPCC A1B scenario are imposed separately and together through sensitivity simulations. Accounting for sulfate, nitrate, ammonium, black carbon (BC), and organic carbon (OC) aerosols, concentrations of individual aerosol species change by −1.5 to +0.8 μg m−3, and PM2.5 levels are projected to change by about 10–20% in eastern China as a result of 2000–2050 change in climate alone. With future changes in anthropogenic emissions alone, concentrations of sulfate, BC, and OC are simulated to decrease because of assumed reductions in emissions, and those of nitrate are predicted to increase because of higher NOx emissions combined with decreases in sulfate. The net result is a predicted reduction of seasonal mean PM2.5 concentrations in eastern China by 1–8 μg m−3 (or 10–40%) over 2000–2050. It is noted that current emission inventories for BC and OC over China are judged to be inadequate at present. Transboundary fluxes of different aerosol species show different sensitivities to future changes in climate and emissions. The annual outflow of PM2.5 from eastern China to the western Pacific is estimated to change by −7.0%, −0.7%, and −9.0% over 2000–2050 owing to climate change alone, changes in emissions alone, and changes in both climate and emissions, respectively. The fluxes of nitrate and ammonium aerosols from Europe and Central Asia into western China increase over 2000–2050 in response to projected changes in emissions, leading to a 10.5% increase in annual inflow of PM2.5 to western China with future changes in both emissions and climate. Fluxes of BC and OC from South Asia to China in spring contribute a large fraction of the annual inflow of PM2.5. The annual inflow of PM2.5 from South Asia and Southeast Asia to China is estimated to change by −8%, +281%, and +227% over 2000–2050 owing to climate change alone, changes in emissions alone, and changes in both climate and emissions, respectively. While the 4° × 5° spatial resolution is a limitation of the present study, the direction of predicted changes in aerosol levels and transboundary fluxes still provides valuable insight into future air quality.

Description: Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere (up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing. When only changes in chemistry are considered (constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9 DU to 13.8 DU among the ten participating models, while the stratospheric column reduction lies between 14.1 DU and 28.6 DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.25 Wm−2 and 0.45 Wm−2 due to ozone change in the troposphere and −0.123 Wm−2 and +0.066 Wm−2 due to the stratospheric ozone change. Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. In most models the isolated effect of climate change is an enhancement of the tropospheric ozone column increase, while the stratospheric reduction becomes slightly less severe. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.10 Wm−2, while the radiative forcing due to stratospheric ozone change is reduced by up to 0.034 Wm−2. Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive.