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Ozone, PM10 and PM2.5 concentrations over Paris, France and Stockholm, Sweden were modelled at 4 and 1 km horizontal resolutions respectively for the present and 2050 periods employing decade-long simulations. We account for large-scale global climate change (RCP-4.5) and fine-resolution bottom-up emission projections developed by local experts and quantify their impact on future pollutant concentrations. Moreover, we identify biases related to the implementation of regional-scale emission projections by comparing modelled pollutant concentrations between the fine- and coarse-scale simulations over the study areas. We show that over urban areas with major regional contribution (e.g. the city of Stockholm) the bias related to coarse-scale projections may be significant and lead to policy misclassification. Our results stress the need to better understand the mechanism of bias propagation across the modelling scales in order to design more successful local-scale strategies. We find that the impact of climate change is spatially homogeneous in both regions, implying strong regional influence. The climate benefit for ozone (daily mean and maximum) is up to −5 % for Paris and −2 % for Stockholm city. The climate benefit on PM2.5 and PM10 in Paris is between −5 and −10 %, while for Stockholm we estimate mixed trends of up to 3 % depending on season and size class. In Stockholm, emission mitigation leads to concentration reductions up to 15 % for daily mean and maximum ozone and 20 % for PM. Through a sensitivity analysis we show that this response is entirely due to changes in emissions at the regional scale. On the contrary, over the city of Paris (VOC-limited photochemical regime), local mitigation of NOx emissions increases future ozone concentrations due to ozone titration inhibition. This competing trend between the respective roles of emission and climate change, results in an increase in 2050 daily mean ozone by 2.5 % in Paris. Climate and not emission change appears to be the most influential factor for maximum ozone concentration over the city of Paris, which may be particularly interesting from a health impact perspective.

While previous research helped to identify and prioritize the sources of error in air-quality modeling due to anthropogenic emissions and spatial scale effects, our knowledge is limited on how these uncertainties affect climate-forced air-quality assessments. Using as reference a 10-year model simulation over the greater Paris (France) area at 4 km resolution and anthropogenic emissions from a 1 km resolution bottom-up inventory, through several tests we estimate the sensitivity of modeled ozone and PM2.5 concentrations to different potentially influential factors with a particular interest over the urban areas. These factors include the model horizontal and vertical resolution, the meteorological input from a climate model and its resolution, the use of a top-down emission inventory, the resolution of the emissions input and the post-processing coefficients used to derive the temporal, vertical and chemical split of emissions. We show that urban ozone displays moderate sensitivity to the resolution of emissions (~ 8 %), the post-processing method (6.5 %) and the horizontal resolution of the air-quality model (~ 5 %), while annual PM2.5 levels are particularly sensitive to changes in their primary emissions (~ 32 %) and the resolution of the emission inventory (~ 24 %). The air-quality model horizontal and vertical resolution have little effect on model predictions for the specific study domain. In the case of modeled ozone concentrations, the implementation of refined input data results in a consistent decrease (from 2.5 up to 8.3 %), mainly due to inhibition of the titration rate by nitrogen oxides. Such consistency is not observed for PM2.5. In contrast this consistency is not observed for PM2.5. In addition we use the results of these sensitivities to explain and quantify the discrepancy between a coarse (~ 50 km) and a fine (4 km) resolution simulation over the urban area. We show that the ozone bias of the coarse run (+9 ppb) is reduced by ~ 40 % by adopting a higher resolution emission inventory, by 25 % by using a post-processing technique based on the local inventory (same improvement is obtained by increasing model horizontal resolution) and by 10 % by adopting the annual emission totals of the local inventory. The bias of PM2.5 concentrations follows a more complex pattern, with the positive values associated with the coarse run (+3.6 μg m−3), increasing or decreasing depending on the type of the refinement. We conclude that in the case of fine particles, the coarse simulation cannot selectively incorporate local-scale features in order to reduce its error.

Ozone and PM2.5 concentrations over the city of Paris are modeled with the CHIMERE air-quality model at 4 km × 4 km horizontal resolution for two future emission scenarios. A high-resolution (1 km × 1 km) emission projection until 2020 for the greater Paris region is developed by local experts (AIRPARIF) and is further extended to year 2050 based on regional-scale emission projections developed by the Global Energy Assessment. Model evaluation is performed based on a 10-year control simulation. Ozone is in very good agreement with measurements while PM2.5 is underestimated by 20% over the urban area mainly due to a large wet bias in wintertime precipitation. A significant increase of maximum ozone relative to present-day levels over Paris is modeled under the "business-as-usual" scenario (+7 ppb) while a more optimistic "mitigation" scenario leads to a moderate ozone decrease (−3.5 ppb) in year 2050. These results are substantially different to previous regional-scale projections where 2050 ozone is found to decrease under both future scenarios. A sensitivity analysis showed that this difference is due to the fact that ozone formation over Paris at the current urban-scale study is driven by volatile organic compound (VOC)-limited chemistry, whereas at the regional-scale ozone formation occurs under NOx-sensitive conditions. This explains why the sharp NOx reductions implemented in the future scenarios have a different effect on ozone projections at different scales. In rural areas, projections at both scales yield similar results showing that the longer timescale processes of emission transport and ozone formation are less sensitive to model resolution. PM2.5 concentrations decrease by 78% and 89% under business-as-usual and mitigation scenarios, respectively, compared to the present-day period. The reduction is much more prominent over the urban part of the domain due to the effective reductions of road transport and residential emissions resulting in the smoothing of the large urban increment modeled in the control simulation.

Changes in temperature due to variability in meteorology and climate change are expected to significantly impact atmospheric composition. The Mediterranean is a climate sensitive region and includes megacities like Istanbul and large urban agglomerations such as Athens. The effect of temperature changes on gaseous air pollutant levels and the atmospheric processes that are controlling them in the Eastern Mediterranean are here investigated. The WRF/CMAQ mesoscale modeling system is used, coupled with the MEGAN model for the processing of biogenic volatile organic compound emissions. A set of temperature perturbations (spanning from 1 to 5 K) is applied on a base case simulation corresponding to July 2004. The results indicate that the Eastern Mediterranean basin acts as a reservoir of pollutants and their precursor emissions from large urban agglomerations. During summer, chemistry is a major sink at these urban areas near the surface, and a minor contributor at downwind areas. On average, the atmospheric processes are more effective within the first 1000 m above ground. Temperature increases lead to increases in biogenic emissions by 9±3% K−1. Ozone mixing ratios increase almost linearly with the increases in ambient temperatures by 1±0.1 ppb O3 K−1 for all studied urban and receptor stations except for Istanbul, where a 0.4±0.1 ppb O3 K−1 increase is calculated, which is about half of the domain-averaged increase of 0.9±0.1 ppb O3 K−1. The computed changes in atmospheric processes are also linearly related with temperature changes.

This study investigates the effects of the total solar eclipse of 29 March 2006 on surface air-quality levels over Greece based on observations at a number of sites in conjunction with chemical box modelling and 3-D air-quality modelling. Emphasis is given on surface ozone and other photooxidants at four Greek sites Kastelorizo, Finokalia (Crete), Pallini (Athens) and Thessaloniki, which are located at gradually increasing distances from the path of the eclipse totality and are characterized by different air pollution levels. The eclipse offered the opportunity to test our understanding of air pollution build-up and the response of the gas-phase chemistry of photo-oxidants during a photolytical perturbation using both a photochemical box model and a regional air-quality offline model based on the modeling system WRF/CAMx. At the relatively unpolluted sites of Kastelorizo and Finokalia no clear signal of the solar eclipse on surface O3, NO2 and NO concentrations can be deduced from the observations while there is no correlation of observed O3, NO2 and NO with observed global radiation. The box and regional model simulations for the two relatively unpolluted sites indicate that the calculated changes in net ozone production rates between eclipse and non eclipse conditions are rather small compared to the observed short-term ozone variability. Furthermore the simulated ozone lifetime is in the range of a few days at these sites and hence the solar eclipse effects on ozone can be easily masked by local and regional transport. At the polluted sites of Thessaloniki and Pallini, the solar eclipse effects on O3, NO2 and NO concentrations are revealed from both the measurements and modeling with the net effect being a decrease in O3 and NO and an increase in NO2 as NO2 formed from the reaction of O3 with NO while at the same time NO2 is not efficiently photolysed. This result is also supported by a positive correlation of observed global radiation with O3 and NO and a negative correlation with NO2. It is evident from the 3-D air quality modeling over Greece that the maximum effects of the eclipse on O3, NO2 and NO are reflected on the large urban agglomerations of Athens, and Thessaloniki where the maximum of the emissions occur.