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Future climate change may bring local benefits or penalties to surface air pollution, resulting from changing temperature, precipitation, and transport patterns, as well as changes in climate-sensitive natural precursor emissions. Here, we estimate the climate penalties and benefits at the end of this century with regard to surface ozone and fine particulate matter (PM ${}_{2.5}$; excluding dust and smoke) using a one-way offline coupling between a general circulation model and a global 3-D chemical-transport model. We archive meteorology for the present day (2005 to 2014) and end of this century (2090 to 2099) for seven future scenarios developed for Phase 6 of the Coupled Model Intercomparison Project. The model isolates the impact of forecasted anthropogenic precursor emission changes versus that of climate-only driven changes on surface ozone and PM ${}_{2.5}$for scenarios ranging from extreme mitigation to extreme warming. We then relate these changes to impacts on human mortality and crop production. We find ozone penalties over nearly all land areas with increasing warming. We find net benefits due to climate-driven changes in PM ${}_{2.5}$in the Northern Extratropics, but net penalties in the Tropics and Southern Hemisphere, where most population growth is forecast for the coming century. 

Abstract. Ground-level ozone (O3) is a major air pollutant that adversely affects human health and ecosystem productivity. Removal of troposphericO3 by plant stomatal uptake can in turn cause damage to plant tissues with ramifications for ecosystem and crop health. In manyatmospheric and land surface models, the functionality of stomata opening is represented by a bulk stomatal conductance, which is oftensemi-empirically parameterized and highly fitted to historical observations. A lack of mechanistic linkage to ecophysiological processes such asphotosynthesis may render models inadequate to represent plant-mediated responses of atmospheric chemistry to long-term changes in CO2,climate, and short-lived air pollutant concentrations. A new ecophysiology module was thus developed to mechanistically simulate land−atmosphereexchange of important gas species in GEOS-Chem, a chemical transport model widely used in atmospheric chemistry studies. The implementation not onlyallows for dry deposition to be coupled with plant ecophysiology but also enables plant and crop productivity and functions to respond dynamically toatmospheric chemical changes. We conduct simulations to evaluate the effects of the ecophysiology module on simulated dry deposition velocity andconcentration of surface O3 against an observation-derived dataset known as SynFlux. Our estimated stomatal conductance and dry depositionvelocity of O3 are close to SynFlux with root-mean-squared errors (RMSEs) below 0.3 cm s−1 across different plant functionaltypes (PFTs), despite an overall positive bias in surface O3 concentration (by up to 16 ppbv). Representing ecophysiology wasfound to reduce the simulated biases in deposition fluxes from the prior model but worsen the positive biases in simulated O3concentrations. The increase in positive concentration biases is mostly attributable to the ecophysiology-based stomatal conductance being generallysmaller (and closer to SynFlux values) than that estimated by the prior semi-empirical formulation, calling for further improvements in non-stomataldepositional and non-depositional processes relevant for O3 simulations. The estimated global O3 deposition flux is864 Tg O3 yr−1 with GEOS-Chem, and the new module decreases this estimate by 92 Tg O3 yr−1. Estimated global grossprimary production (GPP) without O3 damage is 119 Pg C yr−1. O3-induced reduction in GPP is 4.2 Pg C yr−1(3.5 %). An elevated CO2 scenario (580 ppm) yields higher global GPP (+16.8 %) and lower global O3depositional sink (−3.3 %). Global isoprene emission simulated with a photosynthesis-based scheme is 317.9 Tg C yr−1, which is31.2 Tg C yr−1 (−8.9 %) less than that calculated using the MEGAN(Model of Emissions of Gases and Aerosols from Nature) emission algorithm. This new model development dynamicallyrepresents the two-way interactions between vegetation and air pollutants and thus provides a unique capability in evaluating vegetation-mediatedprocesses and feedbacks that can shape atmospheric chemistry and air quality, as well as pollutant impacts on vegetation health, especially for anytimescales shorter than the multidecadal timescale. 

Abstract. Dry deposition is a key process for surface ozone(O3) removal. Stomatal uptake is a major component of O3 drydeposition, which is parameterized differently in current land surfacemodels and chemical transport models. We developed and used a standaloneterrestrial biosphere model, driven by a unified set of prescribedmeteorology, to evaluate two widely used dry deposition modeling frameworks,Wesely (1989) and Zhang et al. (2003), with different configurations ofstomatal resistance: (1) the default multiplicative method in the Weselyscheme (W89) and Zhang et al. (2003) scheme (Z03), (2) the traditionalphotosynthesis-based Farquhar–Ball–Berry (FBB) stomatal algorithm, and (3) theMedlyn stomatal algorithm (MED) based on optimization theory. We found thatusing the FBB stomatal approach that captures ecophysiological responses toenvironmental factors, especially to water stress, can generally improve thesimulated dry deposition velocities compared with multiplicative schemes.The MED stomatal approach produces higher stomatal conductance than FBB andis likely to overestimate dry deposition velocities for major vegetationtypes, but its performance is greatly improved when spatially varying slopeparameters based on annual mean precipitation are used. Large discrepancieswere also found in stomatal responses to rising CO2 levels from 390to 550 ppm: the multiplicative stomatal method with an empirical CO2response function produces reduction (−35 %) in global stomatalconductance on average much larger than that with the photosynthesis-basedstomatal method (−14 %–19 %). Our results show the potential biases inO3 sink caused by errors in model structure especially in the Weselydry deposition scheme and the importance of using photosynthesis-basedrepresentation of stomatal resistance in dry deposition schemes under achanging climate and rising CO2 concentration. 

Abstract. Dry deposition is a major sink of tropospheric ozone.Increasing evidence has shown that ozone dry deposition actively linksmeteorology and hydrology with ozone air quality. However, there is littlesystematic investigation on the performance of different ozone drydeposition parameterizations at the global scale and how parameterizationchoice can impact surface ozone simulations. Here, we present the results ofthe first global, multidecadal modelling and evaluation of ozone drydeposition velocity (vd) using multiple ozone dry depositionparameterizations. We model ozone dry deposition velocities over 1982–2011using four ozone dry deposition parameterizations that are representative ofcurrent approaches in global ozone dry deposition modelling. We useconsistent assimilated meteorology, land cover, and satellite-derived leafarea index (LAI) across all four, such that the differences in simulatedvd are entirely due to differences in deposition model structures orassumptions about how land types are treated in each. In addition, we usethe surface ozone sensitivity to vd predicted by a chemical transportmodel to estimate the impact of mean and variability of ozone dry depositionvelocity on surface ozone. Our estimated vd values from four differentparameterizations are evaluated against field observations, and whileperformance varies considerably by land cover types, our results suggestthat none of the parameterizations are universally better than the others.Discrepancy in simulated mean vd among the parameterizations isestimated to cause 2 to 5 ppbv of discrepancy in surface ozone in theNorthern Hemisphere (NH) and up to 8 ppbv in tropical rainforests in July,and up to 8 ppbv in tropical rainforests and seasonally dry tropical forestsin Indochina in December. Parameterization-specific biases based onindividual land cover type and hydroclimate are found to be the two maindrivers of such discrepancies. We find statistically significant trends inthe multiannual time series of simulated July daytime vd in allparameterizations, driven by warming and drying (southern Amazonia, southernAfrican savannah, and Mongolia) or greening (high latitudes). The trend inJuly daytime vd is estimated to be 1 % yr−1 and leadsto up to 3 ppbv of surface ozone changes over 1982–2011. The interannual coefficient ofvariation (CV) of July daytime mean vd in NH is found to be5 %–15 %, with spatial distribution that varies with the dry depositionparameterization. Our sensitivity simulations suggest this can contributebetween 0.5 to 2 ppbv to interannual variability (IAV) in surface ozone, butall models tend to underestimate interannual CV when compared to long-termozone flux observations. We also find that IAV in some dry depositionparameterizations is more sensitive to LAI, while in others it is more sensitiveto climate. Comparisons with other published estimates of the IAV ofbackground ozone confirm that ozone dry deposition can be an important partof natural surface ozone variability. Our results demonstrate the importanceof ozone dry deposition parameterization choice on surface ozone modellingand the impact of IAV of vd on surface ozone, thus making a strong casefor further measurement, evaluation, and model–data integration of ozone drydeposition on different spatiotemporal scales.