ALBERT

Description: A number of attempts have been made to incorporate sea-salt aerosol (SSA) source functions in chemistry transport models with varying results according to the complexity of the scheme considered. This contribution compares the inclusion of two different SSA algorithms in two chemistry transport models: CMAQ and CHIMERE. The main goal is to examine the differences in average SSA mass and composition and to study the seasonality of the prediction of SSA when applied to the Mediterranean area with high resolution for a reference year. Dry and wet deposition schemes are also analyzed to better understand the differences observed between both models in the target area. The applied emission algorithm in CHIMERE uses a semi-empirical formulation which obtains the surface emission rate of SSA as a function of the particle size and the surface wind speed raised to the power 3.41. The emission parameterization included within CMAQ is somehow more sophisticated, since fluxes of SSA are corrected with relative humidity. In order to evaluate their strengths and weaknesses, the participating algorithms as implemented in the chemistry transport models were evaluated against AOD measurements from Aeronet and available surface measurements in Southern Europe and the Mediterranean area, showing biases around −0.002 and −1.2 μg m−3, respectively. The results indicate that both models represent accurately the patterns and dynamics of SSA and its non-uniform behavior in the Mediterranean basin, showing a strong seasonality. The levels of SSA strongly vary across the Western and the Eastern Mediterranean, reproducing CHIMERE higher annual levels in the Aegean Sea (12 μg m−3) and CMAQ in the Gulf of Lion (9 μg m−3). The large difference found for the ratio PM2.5/total SSA in CMAQ and CHIMERE is also investigated. The dry and wet removal rates are very similar for both models despite the different schemes implemented. Dry deposition essentially follows the surface drag stress patterns, meanwhile wet deposition is more scattered over the continent. CMAQ tends to provide larger amounts of SSA dry deposition over the Northern Mediterranean (0.7–1.0 g m−2 yr−1), meanwhile the Southeastern Mediterranean accounts for the maximum annual dry deposition in the CHIMERE model (0.9–1.5 g m−2 yr−1). The wet deposition is dominated by the accumulation mode and is strongly correlated to the precipitation patterns, showing CMAQ a higher wet deposition/total deposition ratio over coastal mountain chains. The results of both models constitute a step towards increasing the understanding of the SSA dynamics in a complex area as the Mediterranean.

Description: The CALIOPE air quality modelling system is developed and applied to Europe with high spatial resolution (12 km × 12 km). The modelled daily-to-seasonal aerosol variability over Europe in 2004 is evaluated and analysed. Aerosols are estimated from two models, CMAQv4.5 (AERO4) and BSC-DREAM8b. CMAQv4.5 calculates biogenic, anthropogenic and sea salt aerosol and BSC-DREAM8b provides the natural mineral dust contribution from North African deserts. For the evaluation, we use daily PM10, PM2.5 and aerosol components data from 55 stations of the EMEP/CREATE network and total, coarse and fine aerosol optical depth (AOD) data from 35 stations of the AERONET sun photometer network. Annual correlations between modelled and observed values for PM10 and PM2.5 are 0.55 and 0.47, respectively. Correlations for total, coarse and fine AOD are 0.51, 0.63, and 0.53, respectively. The higher correlations of the PM10 and the coarse mode AOD are largely due to the accurate representation of the African dust influence in the forecasting system. Overall PM and AOD levels are underestimated. The evaluation of the aerosol components highlights underestimations in the fine fraction of carbonaceous matter (EC and OC) and secondary inorganic aerosols (SIA; i.e. nitrate, sulphate and ammonium). The scores of the bulk parameters are significantly improved after applying a simple model bias correction based on the observed aerosol composition. The simulated PM10 and AOD present maximum values over the industrialized and populated Po Valley and Benelux regions. SIA are dominant in the fine fraction representing up to 80% of the aerosol budget in latitudes north of 40° N. In southern Europe, high PM10 and AOD are linked to the desert dust transport from the Sahara which contributes up to 40% of the aerosol budget. Maximum seasonal ground-level concentrations (PM10 〉 30 μg m−3) are found between spring and early autumn. We estimate that desert dust causes daily exceedances of the PM10 European air quality limit value (50 μg m−3) in large areas south of 45° N with more than 75 exceedances per year in the southernmost regions.

Description: The CALIOPE high-resolution air quality modelling system is developed and applied to Europe (12 km × 12 km, 1 h). The modelled daily to seasonal aerosol variability over Europe in 2004 have been evaluated and analysed. The aerosols are estimated from two models, CMAQv4.5 (AERO4) and BSC-DREAM8b. CMAQv4.5 calculates biogenic, anthropogenic and sea salt aerosol and BSC-DREAM8b provides the natural mineral dust contribution from North African deserts. For the evaluation, we use daily PM10/PM2.5 and chemical composition data from 54 stations of the EMEP/CREATE network and coarse and fine aerosol optical depth (AOD) data from 35 stations of the AERONET sun photometer network. The model achieves daily PM10 and PM2.5 correlations of 0.57 and 0.47, respectively, and total, coarse and fine AOD correlations of 0.51, 0.63, and 0.53, respectively. The higher correlations of the PM10 and the coarse mode AOD are largely due to the accurate representation of the African dust influence in the forecasting system. Overall PM and AOD levels are underestimated. The evaluation of the chemical composition highlights underestimations of the modelled fine fractions particularly for carbonaceous matter (EC and OC) and secondary inorganic aerosols (SIA; i.e. nitrates, sulphates and ammonium). The scores of the bulk parameters are significantly improved after applying a simple model bias correction based on the chemical composition observations. SIA are dominant in the fine fractions representing up to 80 % of the aerosol budget in latitudes beyond 40° N. The highest aerosol concentrations are found over the industrialized and populated areas of the Po Valley and the Benelux regions. High values in southern Europe are linked to the transport of coarse particles from the Sahara desert which contributes up to 40 % of the total aerosol mass. Close to the surface, maxima dust seasonal concentrations (〉30 μg m–3) are found between spring and early autumn. We estimate that desert dust causes daily exceedances of the PM10 European air quality threshold (50 μg m–3) in large areas south of 45° N reaching up to more than 75 days per year in the southernmost regions.

Description: The EURODELTA III exercise allows a very comprehensive inter-comparison and evaluation of chemistry transport models performance. Participating models were applied over four different one month period, within a rather limited number of years (from June 2006 to March 2009) thus allowing evaluating the influence of different meteorological conditions on model performance. The exercise was performed under strict requirements concerning the input data. As a consequence, there were very limited differences in the models set up, representing a sort of sensitivity analysis to several aspects of the modelling chains. The models were evaluated mainly on background stations. Even if the meteorology was prescribed, some variables like the planetary boundary layer (PBL) height, the vertical diffusion coefficient are diagnosed in the model pre-processors and explain the spread of models results. For ozone, this study shows the importance of boundary conditions on model calculations and then on the regime of the gas and particle chemistry. The worst performances are observed for sulphur dioxide concentrations that are poorly captured by the models. The performances of models are rather good very similar for the nitrogen dioxide. On average, the models provide a rather good picture of the particulate matter (PM) concentrations over Europe even if the highest concentrations are underestimated. For the PM, the mean diurnal cycles show a general tendency to overestimate the effect of the PBL height rise while the afternoon chemistry (formation of secondary species) is certainly underestimated, PM observations show very flat diurnal profiles whatever the season. In general the day time PBL height is underestimated by all models, the largest variability of predicted PBL is observed over the ocean and seas. More generally, in most cases model performances are more influenced by the model setup than the season. The temporal evolution of wind speed is most responsible of model skilfulness in reproducing the daily variability of pollutant concentrations (e.g. the development of peak episodes), while the reconstruction of the PBL diurnal cycle seems more influencing in driving the corresponding pollutant diurnal cycle and hence the presence of systematic positive and negative biases detectable on daily basis.

Description: A number of attempts have been made to incorporate sea-salt aerosols (SSA) source functions in chemistry transport models with varying results according to the complexity of the scheme considered. This contribution compares the inclusion of two different SSA algorithms in two chemistry transport models: CMAQ and CHIMERE. The main goal is to examine the differences in average SSA mass and composition and to study the seasonality of the prediction of SSA when applied to the Mediterranean area with high resolution in a reference year. Dry and wet deposition schemes are also analyzed to better understand the differences observed between both models in the target area. The applied emission algorithm in CHIMERE uses a semi-empirical formulation which obtains the surface emission rate of SSA as a function of the surface wind speed cubed and particle size. The emission parameterization included within CMAQ is somehow more sophisticated, since fluxes of SSA are corrected with relative humidity. In order to evaluate their strengths and weaknesses, the participating algorithms as implemented in the chemistry transport models were evaluated against AOD measurements from Aeronet and available surface measurements in Southern Europe and the Mediterranean area, showing biases around −0.003 and −1.2 μg m−3, respectively. The results indicate that both models represent accurately the patterns and dynamics of SSA and its non-uniform behavior in the Mediterranean basin, showing a strong seasonality. The levels of SSA vary strongly across the Western and the Eastern Mediterranean, reproducing CHIMERE higher annual levels in the Aegean Sea (12 μg m−3) and CMAQ in the Gulf of Lion (9 μg m−3). The large difference found for the ratio PM2.5/total SSA in CMAQ and CHIMERE is also investigated. The dry and wet removal rates are very similar for both models despite the different schemes implemented. Dry deposition essentially follows the surface drag stress patterns, meanwhile wet deposition is more scattered over the continent. CMAQ tends to provide larger amounts of SSA dry deposition over the Northern Mediterranean (0.7–1.0 g m−2 yr−1), meanwhile the Southeastern Mediterranean accounts for the maximum annual dry deposition in the CHIMERE model (0.9–1.5 g m−2 yr−1). The wet deposition is dominated by the accumulation mode and is strongly correlated to the precipitation patterns, showing CMAQ a higher wet deposition/total deposition ratio over coastal mountain chains. The results of both models constitute a step towards increasing the understanding of the SSA dynamics in a complex area as the Mediterranean.

Description: The CALIOPE air quality modelling system, namely WRF-ARW/HERMES-EMEP/CMAQ/BSC-DREAM8b, has been used to perform the simulation of ground level O3 concentration for the year 2004, over the Iberian Peninsula. We use this system to study the daily ground-level O3 maximum. We investigate the use of a post-processing such as the Kalman Filter bias-adjustment technique to improve the simulated O3 maximum. The Kalman Filter bias-adjustment technique is a recursive algorithm to optimally estimate bias-adjustment terms from previous measurements and model results. The bias-adjustment technique is found to improve the simulated O3 maximum for the entire year and the whole domain. The corrected simulation presents improvements in statistical indicators such as correlation, root mean square error, mean bias, standard deviation, and gross error. After the post-processing the exceedances of O3 concentration limits, as established by the European Directive 2008/50/CE, are better reproduced and the uncertainty of the modelling system is reduced from 20% to 7.5%. Such uncertainty in the model results is under the established EU limit of the 50%. Significant improvements in the O3 average daily cycle and in its amplitude are also observed after the post-processing. The systematic improvements in the O3 maximum simulations suggest that the Kalman Filter post-processing method is a suitable technique to reproduce accurate estimate of ground-level O3 concentration.

Description: CALIOPE-AQFS represents the current state-of-the-art in air quality forecasting systems running at high resolution over high performance computing platforms. It provides 48 h forecast of main pollutants over Spain at 4 km horizontal resolution, and over the most populated areas with complex terrains in Spain (Barcelona, Madrid and Andalucia domains) at 1 km. Increased horizontal resolution from 4 km to 1 km over the aforementioned domains leads to finer texture and more realistic concentration maps, justified by the increase of NO2/O3 spatial correlation coefficients from 0.79/0.69 (4 km) to 0.81/0.73 (1 km). High resolution emissions using the bottom-up HERMESv2.0 model are essential to improve the model performance when increasing resolution at urban scale, but it is not sufficient. Decreasing grid spacing does not reveal the expected improvement on hourly statistics, decreasing NO2 bias only in ~ 2 μg m−3 and increasing O3 bias in ~ 1 μg m−3. The grid effect is less pronounced for PM10 because part of its mass consists of secondary aerosols which are less affected by a decreasing grid size in contrast to the locally emitted primary components. The resolution increase has the highest impact over Barcelona, where air flow is mainly controlled by mesoscale phenomena and a lower PBL. Despite the merits and potential uses of the 1 km simulation, the limitations of current model formulations do not allow confirming their expected superiority close to highly urbanized areas and large sources. Future work should combine high grid resolution with techniques that decrease subgrid variability and models that consider urban morphology and thermal parameters.

Description: The CALIOPE Air Quality Forecast System (CALIOPE-AQFS) represents the current state of the art in air quality forecasting systems of high-resolution running on high-performance computing platforms. It provides a 48 h forecast of NO2, O3, SO2, PM10, PM2.5, CO, and C6H6 at a 4 km horizontal resolution over all of Spain, and at a 1 km horizontal resolution over the most populated areas in Spain with complex terrains (the Barcelona (BCN), Madrid (MAD) and Andalusia (AND) domains). Increased horizontal resolution from 4 to 1 km over the aforementioned domains leads to finer textures and more realistic concentration maps, which is justified by the increase in NO2/O3 spatial correlation coefficients from 0.79/0.69 (4 km) to 0.81/0.73 (1 km). High-resolution emissions using the bottom-up HERMESv2.0 model are essential for improving model performance when increasing resolution on an urban scale, but it is still insufficient. Decreasing grid spacing does not reveal the expected improvement in hourly statistics, i.e., decreasing NO2 bias by only ~ 2 μg m−3 and increasing O3 bias by ~ 1 μg m−3. The grid effect is less pronounced for PM10, because part of its mass consists of secondary aerosols, which are less affected than the locally emitted primary components by a decreasing grid size. The resolution increase has the highest impact over Barcelona, where air flow is controlled mainly by mesoscale phenomena and a lower planetary boundary layer (PBL). Despite the merits and potential uses of the 1-km simulation, the limitations of current model formulations do not allow confirmation of their expected superiority close to highly urbanized areas and large emissions sources. Future work should combine high grid resolutions with techniques that decrease subgrid variability (e.g., stochastic field methods), and also include models that consider urban morphology and thermal parameters.