Abstract. We present a first description and evaluation of GEOS-CHEM, a global threedimensional (3-D

a b s t r a c tAir quality is strongly dependent on weather and is therefore sensitive to climate change. Recent studies have provided estimates of this climate effect through correlations of air quality with meteorological variables, perturbation analyses in chemical transport models (CTMs), and CTM simulations driven by general circulation model (GCM) simulations of 21st-century climate change. We review these different approaches and their results. The future climate is expected to be more stagnant, due to a weaker global circulation and a decreasing frequency of mid-latitude cyclones. The observed correlation between surface ozone and temperature in polluted regions points to a detrimental effect of warming. Coupled GCM-CTM studies find that climate change alone will increase summertime surface ozone in polluted regions by 1-10 ppb over the coming decades, with the largest effects in urban areas and during pollution episodes. This climate penalty means that stronger emission controls will be needed to meet a given air quality standard. Higher water vapor in the future climate is expected to decrease the ozone background, so that pollution and background ozone have opposite sensitivities to climate change. The effect of climate change on particulate matter (PM) is more complicated and uncertain than for ozone. Precipitation frequency and mixing depth are important driving factors but projections for these variables are often unreliable. GCM-CTM studies find that climate change will affect PM concentrations in polluted environments by AE0.1-1 mg m À3 over the coming decades. Wildfires fueled by climate change could become an increasingly important PM source. Major issues that should be addressed in future research include the ability of GCMs to simulate regional air pollution meteorology and its sensitivity to climate change, the response of natural emissions to climate change, and the atmospheric chemistry of isoprene. Research needs to be undertaken on the effect of climate change on mercury, particularly in view of the potential for a large increase in mercury soil emissions driven by increased respiration in boreal ecosystems.

Mercury (Hg) is a global pollutant that affects human and ecosystem health. We synthesize understanding of sources, atmosphere-land-ocean Hg dynamics and health effects, and consider the implications of Hg-control policies. Primary anthropogenic Hg emissions greatly exceed natural geogenic sources, resulting in increases in Hg reservoirs and subsequent secondary Hg emissions that facilitate its global distribution. The ultimate fate of emitted Hg is primarily recalcitrant soil pools and deep ocean waters and sediments. Transfers of Hg emissions to largely unavailable reservoirs occur over the time scale of centuries, and are primarily mediated through atmospheric exchanges of wet/dry deposition and evasion from vegetation, soil organic matter and ocean surfaces. A key link between inorganic Hg inputs and exposure of humans and wildlife is the net production of methylmercury, which occurs mainly in reducing zones in freshwater, terrestrial, and coastal environments, and the subsurface ocean. Elevated human exposure to methylmercury primarily results from consumption of estuarine and marine fish. Developing fetuses are most at risk from this neurotoxin but health effects of highly exposed populations and wildlife are also a concern. Integration of Hg science with national and international policy efforts is needed to target efforts and evaluate efficacy.

We use a global three‐dimensional coupled oxidant‐aerosol model (GEOS‐CHEM) to estimate natural and transboundary pollution influences on sulfate‐nitrate‐ammonium aerosol concentrations in the United States. This work is motivated in part by the Regional Haze Rule of the U.S. Environmental Protection Agency (EPA), which requires immediate action to improve visibility in U.S. wilderness areas along a linear trajectory toward an endpoint of “natural visibility conditions” by 2064. We present full‐year simulations for 1998 and 2001 and evaluate them with nationwide networks of observations in the United States and Europe (Interagency Monitoring of Protected Visual Environments (IMPROVE), Clean Air Status and Trends Network (CASTNET), National Atmospheric Deposition Program (NADP), European Monitoring and Evaluation Programme (EMEP)) and with Asian outflow observations from the NASA Transport and Chemical Evolution over the Pacific (TRACE‐P) aircraft mission. Shutting off U.S. anthropogenic emissions in the model defines “background” aerosol concentrations representing contributions from both natural and transboundary pollution sources. We find that transboundary transport of pollution from Canada, Mexico, and Asia dominates over natural influences for both sulfate and nitrate. Trans‐Pacific transport of Asian pollution accounts for 30% of background sulfate in both the western and eastern United States. Our best estimates of natural concentrations for ammonium sulfate and ammonium nitrate in the United States are either consistent with or lower than the default values recommended by EPA for natural visibility calculations. However, the large transboundary pollution influence in our calculation suggests that a natural visibility objective cannot be approached without international emission controls.