Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the ...formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.
Fully-coupled air-quality models running in “feedback” and “no-feedback” configurations were compared against each other and observation network data as part of Phase 2 of the Air Quality Model ...Evaluation International Initiative. In the “no-feedback” mode, interactions between meteorology and chemistry through the aerosol direct and indirect effects were disabled, with the models reverting to climatologies of aerosol properties, or a no-aerosol weather simulation, while in the “feedback” mode, the model-generated aerosols were allowed to modify the models' radiative transfer and/or cloud formation processes. Annual simulations with and without feedbacks were conducted for domains in North America for the years 2006 and 2010, and for Europe for the year 2010. Comparisons against observations via annual statistics show model-to-model variation in performance is greater than the within-model variation associated with feedbacks. However, during the summer and during intense emission events such as the Russian forest fires of 2010, feedbacks have a significant impact on the chemical predictions of the models.
The aerosol indirect effect was usually found to dominate feedbacks compared to the direct effect. The impacts of direct and indirect effects were often shown to be in competition, for predictions of ozone, particulate matter and other species. Feedbacks were shown to result in local and regional shifts of ozone-forming chemical regime, between NOx- and VOC-limited environments. Feedbacks were shown to have a substantial influence on biogenic hydrocarbon emissions and concentrations: North American simulations incorporating both feedbacks resulted in summer average isoprene concentration decreases of up to 10%, while European direct effect simulations during the Russian forest fire period resulted in grid average isoprene changes of −5 to +12.5%. The atmospheric transport and chemistry of large emitting sources such as plumes from forest fires and large cities were shown to be strongly impacted by the presence or absence of feedback mechanisms in the model simulations. Summertime model performance for ozone and other gases was improved through the inclusion of indirect effect feedbacks, while performance for particulate matter was degraded, suggesting that current parameterizations for in- and below cloud processes, once the cloud locations become more directly influenced by aerosols, may over- or under-predict the strength of these processes. Process parameterization-level comparisons of fully coupled feedback models are therefore recommended for future work, as well as further studies using these models for the simulations of large scale urban/industrial and/or forest fire plumes.
To quantify changes in air pollution over Europe at the 2050 horizon, we designed a comprehensive modelling system that captures the external factors considered to be most relevant, and that relies ...on up-to-date and consistent sets of air pollution and climate policy scenarios. Global and regional climate as well as global chemistry simulations are based on the recent representative concentration pathways (RCP) produced for the Fifth Assessment Report (AR5) of the IPCC (Intergovernmental Panel on Climate Change) whereas regional air quality modelling is based on the updated emissions scenarios produced in the framework of the Global Energy Assessment. We explored two diverse scenarios: a reference scenario where climate policies are absent and a mitigation scenario which limits global temperature rise to within 2 °C by the end of this century. This first assessment of projected air quality and climate at the regional scale based on CMIP5 (5th Coupled Model Intercomparison Project) climate simulations is in line with the existing literature using CMIP3. The discrepancy between air quality simulations obtained with a climate model or with meteorological reanalyses is pointed out. Sensitivity simulations show that the main factor driving future air quality projections is air pollutant emissions, rather than climate change or intercontinental transport of pollution. Whereas the well documented "climate penalty" that weights upon ozone (increase of ozone pollution with global warming) over Europe is confirmed, other features appear less robust compared to the literature, such as the impact of climate on PM2.5. The quantitative disentangling of external factors shows that, while several published studies focused on the climate penalty bearing upon ozone, the contribution of the global ozone burden is somewhat overlooked in the literature.
Wildland fires represent the major source of fine aerosols, i.e., atmospheric particles with diameters <1 μm. The largest numbers of these fires occur in Africa, Asia and South America, but a not ...negligible fraction also occurs in Eastern Europe and former USSR countries, particularly in the Russian Federation, Ukraine and Kazakhstan. Besides the impact of large forest fires, recent studies also highlighted the crucial role played by routine agricultural fires in Eastern Europe and Russia on the Arctic atmosphere. An evaluation of the impact of these fires over Europe is currently not available. The assessment of the relative contribution of fires to the European aerosol burden is hampered by the complex mixing of natural and anthropogenic particle types across the continent. In this study we use long term (2002–2007) satellite-based fires and aerosol data coupled to atmospheric trajectory modelling in the attempt to estimate the wildfires contribution to the European aerosol optical thickness (AOT). Based on this dataset, we provide evidence that fires-related aerosols play a major role in shaping the AOT yearly cycle at the continental scale. In general, the regions most impacted by wildfires emissions and/or transport are Eastern and Central Europe as well as Scandinavia. Conversely, a minor impact is found in Western Europe and in the Western Mediterranean. We estimate that in spring 5 to 35% of the European fine fraction AOT (FFAOT) is attributable to wildland fires. The estimated impact maximizes in April (20–35%) in Eastern and Central Europe as well as in Scandinavia and in the Central Mediterranean. An important contribution of wildfires to the FFAOT is also found in summer over most of the continent, particularly in August over Eastern Europe (28%) and the Mediterranean regions, from Turkey (34%) to the Western Mediterranean (25%). Although preliminary, our results suggest that this fires-related, continent-wide haze plays a not negligible role on the European radiation budget, and possibly, on the European air quality, therefore representing a clear target for mitigation.
The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, ...refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model intercomparison, we used the bulk mass profiles of aerosol chemical species sampled over the locations of AERONET stations across Europe and North America to calculate the aerosol optical properties under a range of common assumptions for all models. Several simulations with parameters perturbed within a range of observed values are carried out for July 2010 and compared in order to infer the assumptions that have the largest impact on the calculated aerosol optical properties. We calculate that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30–35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core–shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. The uncertainty introduced by the choice of mixing state choice on the calculation of the asymmetry parameter is the order of 10%. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. It is thus recommended to focus further research on a more accurate representation of the aerosol mixing state in models, in order to have a less uncertain simulation of the related optical properties.
•We calculate optical properties from several aerosol models using same assumptions.•We test choices on mixing state, refractive index, density and hygroscopicity.•The most sensitive parameter is the aerosol mixing state.•The related uncertainty on calculated AOD and SSA is 30–35%.
Emission of non-methane Volatile Organic Compounds (VOCs) to the atmosphere stems from biogenic and human activities, and their estimation is difficult because of the many and not fully understood ...processes involved. In order to narrow down the uncertainty related to VOC emissions, which negatively reflects on our ability to simulate the atmospheric composition, we exploit satellite observations of formaldehyde (HCHO), an ubiquitous oxidation product of most VOCs, focusing on Europe. HCHO column observations from the Ozone Monitoring Instrument (OMI) reveal a marked seasonal cycle with a summer maximum and winter minimum. In summer, the oxidation of methane and other long-lived VOCs supply a slowly varying background HCHO column, while HCHO variability is dominated by most reactive VOC, primarily biogenic isoprene followed in importance by biogenic terpenes and anthropogenic VOCs. The chemistry-transport model CHIMERE qualitatively reproduces the temporal and spatial features of the observed HCHO column, but display regional biases which are attributed mainly to incorrect biogenic VOC emissions, calculated with the Model of Emissions of Gases and Aerosol from Nature (MEGAN) algorithm. These "bottom-up" or a-priori emissions are corrected through a Bayesian inversion of the OMI HCHO observations. Resulting "top-down" or a-posteriori isoprene emissions are lower than "bottom-up" by 40% over the Balkans and by 20% over Southern Germany, and higher by 20% over Iberian Peninsula, Greece and Italy. We conclude that OMI satellite observations of HCHO can provide a quantitative "top-down" constraint on the European "bottom-up" VOC inventories.
In the framework of the AQMEII initiative WRF-Chem has been applied over Europe adopting two chemical configurations for the calendar year 2010. The first one employed the RADM2 gas-phase chemistry ...and MADE/SORGAM aerosol module, while the second one implemented the CBM-Z gaseous parameterization and MOSAIC aerosol chemistry. Configurations shared the same domain, meteorological setups and input data. The Comparison demonstrated that CBM-Z has a more efficient ozone-NO titration than RADM2 in regions with sufficiently high levels of NOx and VOCs. At the same time, CBM-Z is found to have a more effective NO2 + OH reaction. The parameterization of the relative humidity of deliquescence point has a strong impact on HNO3 and NO3 concentrations over Europe, particularly over the sea. The MADE approach showed to be more efficient than MOSAIC. Differently, particulate sulfate and SO2 ground concentrations proved to be more influenced by the heterogeneous SO2 cloud oxidation. PM10 and PM2.5 have shown similar results for MOSAIC and MADE/SORGAM, even though some differences were found in the dust and sea salt size partitioning between modes and bins. Indeed, in MADE the sea salt was distributed only in the coarse fraction, while the dust emissions were distributed mainly in the fine fraction. Finally, different chemical mechanisms give different Aerosol Optical Depths (AOD). WRF-Chem is found to under predict the AODs in both configurations because of the misrepresentation of the dust coarse particle, as shown by the analysis of the relationship between the Angstrom exponent and the AOD bias. Differently, when the AOD is dominated by fine particles, the differences in model performance are more evident, with MADE/SORGAM generally performing better than MOSAIC. Indeed the higher availability of both sulfate and nitrate has a significant influence on reconstruction of the AOD estimations. This paper shows the great importance of chemical mechanisms in both gaseous and aerosols predictions, as well as in the calculation of aerosol optical properties.
The meteorological predictions of fully coupled air-quality models running in “feedback” versus “no-feedback” simulations were compared against each other and observations as part of Phase 2 of the ...Air Quality Model Evaluation International Initiative. In the “no-feedback” mode, the aerosol direct and indirect effects were disabled, with the models reverting to either climatologies of aerosol properties, or a no-aerosol weather simulation. In the “feedback” mode, the model-generated aerosols were allowed to modify the radiative transfer and/or cloud formation parameterizations of the respective models. Annual simulations with and without feedbacks were conducted on domains over North America for the years 2006 and 2010, and over Europe for the year 2010.
The incorporation of feedbacks was found to result in systematic changes to forecast predictions of meteorological variables, both in time and space, with the largest impacts occurring in the summer and near large sources of pollution. Models incorporating only the aerosol direct effect predicted feedback-induced reductions in temperature, surface downward and upward shortwave radiation, precipitation and PBL height, and increased upward shortwave radiation, in both Europe and North America. The feedback response of models incorporating both the aerosol direct and indirect effects varied across models, suggesting the details of implementation of the indirect effect have a large impact on model results, and hence should be a focus for future research. The feedback response of models incorporating both direct and indirect effects was also consistently larger in magnitude to that of models incorporating the direct effect alone, implying that the indirect effect may be the dominant process. Comparisons across modelling platforms suggested that direct and indirect effect feedbacks may often act in competition: the sign of residual changes associated with feedbacks often changed between those models incorporating the direct effect alone versus those incorporating both feedback processes.
Model comparisons to observations for no-feedback and feedback implementations of the same model showed that differences in performance between models were larger than the performance changes associated with implementing feedbacks within a given model. However, feedback implementation was shown to result in improved forecasts of meteorological parameters such as the 2 m surface temperature and precipitation. These findings suggest that meteorological forecasts may be improved through the use of fully coupled feedback models, or through incorporation of improved climatologies of aerosol properties, the latter designed to include spatial, temporal and aerosol size and/or speciation variations.
•Fully coupled air pollution/weather models were compared as part of AQMEII-2.•Feedbacks systematically changed weather and air pollution forecasts.•Aerosol in-and direct effects were often opposed, and direct effects were smaller.•Indirect effect, cloud microphysics implementation likely caused model differences.•Feedbacks improved forecasts though model – based differences had greater magnitude.
The impact of biogenic volatile organic compound (BVOC) emissions on European ozone distributions has not yet been evaluated in a comprehensive way. Using the CHIMERE chemistry-transport model the ...variability of surface ozone levels from April to September for 4 years (1997, 2000, 2001, 2003) resulting from biogenic emissions is investigated. It is shown that BVOC emissions increased on average summer daily ozone maxima over Europe by 2.5
ppbv (5%). The impact is most significant in Portugal (up to 15
ppbv) and in the Mediterranean region (about 5
ppbv), being smaller in the northern part of Europe (1.3
ppbv north of 47.5°N). The average impact is rather similar for the three summers (1997, 2000, 2001), but is much larger during the extraordinarily hot summer of 2003. Here, the biogenic contribution to surface ozone doubles compared to other years at some locations. Interaction with anthropogenic NO
x
emissions is found to be a key process for ozone production of biogenic precursors. Comparing the impact of the state-of-the-art BVOC emission inventory compiled within the NatAir project and an earlier, widely used BVOC inventory derived from Simpson et al. 1999. Inventorying emissions from nature in Europe. Journal of Geophysical Research 104(D7), 8113–8152 on surface ozone shows that ozone produced from biogenic precursors is less in central and northern Europe but in certain southern areas much higher e.g. Iberian Peninsula and the Mediterranean Sea. The uncertainty in the regionally averaged impact of BVOC on ozone build-up in Europe is estimated to be ±50%.
Chemical and dynamical processes lead to the formation of aerosol layers in the upper planetary boundary layer (PBL) and above it. Through vertical mixing and entrainment into the PBL these layers ...may contribute to the ground-level particulate matter (PM); however, to date a quantitative assessment of such a contribution has not been carried out. This study investigates this aspect by combining chemical and physical aerosol measurements with WRF/Chem (Weather Research and Forecasting with Chemistry) model simulations. The observations were collected in the Milan urban area (northern Italy) during the summer of 2007. The period coincided with the passage of a meteorological perturbation that cleansed the lower atmosphere, followed by a high-pressure period favouring pollutant accumulation. Lidar observations revealed the formation of elevated aerosol layers and evidence of their entrainment into the PBL. We analysed the budget of ground-level PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 mu m) with the help of the online meteorology-chemistry WRF/Chem model, focusing in particular on the contribution of upper-level processes. Our findings show that an important player in determining the upper-PBL aerosol layer is particulate nitrate, which may reach higher values in the upper PBL (up to 30% of the aerosol mass) than in the lower PBL. The nitrate formation process is predicted to be largely driven by the relative-humidity vertical profile, which may trigger efficient aqueous nitrate formation when exceeding the ammonium nitrate deliquescence point. Secondary PM2.5 produced in the upper half of the PBL may contribute up to 7-8 mu g m-3 (or 25%) to ground-level concentrations on an hourly basis. The residual aerosol layer above the PBL is also found to potentially play a large role, which may occasionally contribute up to 10-12 mu g m-3 (or 40%) to hourly ground-level PM2.5 concentrations during the morning hours. Although the results presented here refer to one relatively short period in one location, this study highlights the importance of considering the interplay between chemical and dynamical processes occurring within and above the PBL when interpreting ground-level aerosol observations.
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