Atmospheric composition forecasting in Europe

The atmospheric composition is a societal issue and, following new European directives, its forecast is now recommended to quantify the air quality. It concerns both gaseous and particles species, identified as potential problems for health. In Europe, numerical systems providing daily air quality forecasts are numerous and, mostly, operated by universities. Following recent European research projects (GEMS, PROMOTE), an organization of the air quality forecast is currently under development. But for the moment, many platforms exist, each of them with strengths and weaknesses. This overview paper presents all existing systems in Europe and try to identify the main remaining gaps in the air quality forecast knowledge. As modeling systems are now able to reasonably forecast gaseous species, and in a lesser extent aerosols, the future directions would concern the use of these systems with ensemble approaches and satellite data assimilation. If numerous improvements were recently done on emissions and chemistry knowledge, improvements are still needed especially concerning meteorology, which remains a weak point of forecast systems. Future directions will also concern the use of these forecast tools to better understand and quantify the air pollution impact on health

Aerosol chemical and optical properties over the Paris area within ESQUIF project

Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given

Direct radiative effect of the Russian wildfires and its impact on air temperature and atmospheric dynamics during August 2010

International audienceIn this study, we investigate the shortwave aerosol direct radiative forcing (ADRF) and its feedback on air temperature and atmospheric dynamics during a major fire event that occurred in Russia during August 2010. The methodology is based on an offline coupling between the CHIMERE chemistry-transport and the Weather Research and Forecasting (WRF) models. First, simulations for the period 5–12 August 2010 have been evaluated by using AERONET (AErosol RObotic NETwork) and satellite measurements of the POLarization and Directionality of the Earth's Reflectance (POLDER) and the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) sensors. During this period, elevated POLDER aerosol optical thickness (AOT) is found over a large part of eastern Europe, with values above 2 (at 550 nm) in the aerosol plume. According to CALIOP observations, particles remain confined to the first five kilometres of the atmospheric layer. Comparisons with satellite measurements show the ability of CHIMERE to reproduce the regional and vertical distribution of aerosols during their transport from the source region. Over Moscow, AERONET measurements indicate an important increase of AOT (340 nm) from 0.7 on 5 August to 2–4 between 6 and 10 August when the aerosol plume was advected over the city. Particles are mainly observed in the fine size mode (radius in the range 0.2–0.4 μm) and are characterized by elevated single-scattering albedo (SSA) (0.95–0.96 between 440 and 1020 nm). Comparisons of simulations with AERONET measurements show that aerosol physical–optical properties (size distribution, AOT, SSA) have been well simulated over Moscow in terms of intensity and/or spectral dependence. Secondly, modelled aerosol optical properties have been used as input in the radiative transfer code of WRF to evaluate their direct radiative impact. Simulations indicate a significant reduction of solar radiation at the ground (up to 80–150 W m−2 in diurnal averages over a large part of eastern Europe due to the presence of the aerosol plume. This ADRF causes an important reduction of the near-surface air temperature between 0.2 and 2.6° on a regional scale. Moscow has been affected by the aerosol plume, especially between 6 and 10 August. During this period, aerosol causes a significant reduction of surface shortwave radiation (up to 70–84 W m−2 in diurnal averages) with a moderate part (20–30%) due to solar absorption within the aerosol layer. The resulting feedbacks lead to a cooling of the air up to 1.6° at the surface and 0.1° at an altitude of 1500–2000 m (in diurnal averages), that contribute to stabilize the atmospheric boundary layer (ABL). Indeed, a reduction of the ABL height of 13 to 65% has been simulated during daytime in presence of aerosols. This decrease is the result of a lower air entrainment as the vertical wind speed in the ABL is shown to be reduced by 5 to 80% (at midday) when the feedback of the ADRF is taken into account. However, the ADRF is shown to have a lower impact on the horizontal wind speed, suggesting that the dilution of particles would be mainly affected by the weakening of the ABL development and associated vertical entrainment. Indeed, CHIMERE simulations driven by the WRF meteorological fields including this ADRF feedback result in a large increase in the modelled near-surface PM10 concentrations (up to 99%). This is due to their lower vertical dilution in the ABL, which tend to reduce model biases with the ground PM10 values observed over Moscow during this specific period

Modelling street level PM10 concentrations across Europe: source apportionment and possible futures

Despite increasing emission controls, particulate matter (PM) has remained a critical issue for European air quality in recent years. The various sources of PM, both from primary particulate emissions as well as secondary formation from precursor gases, make this a complex problem to tackle. In order to allow for credible predictions of future concentrations under policy assumptions, a modelling approach is needed that considers all chemical processes and spatial dimensions involved, from long-range transport of pollution to local emissions in street canyons. Here we describe a modelling scheme which has been implemented in the GAINS integrated assessment model to assess compliance with PM10 (PM with aerodynamic diameter <10 um) limit values at individual air quality monitoring stations reporting to the AirBase database. The modelling approach relies on a combination of bottom up modelling of emissions, simplified atmospheric chemistry and dispersion calculations, and a traffic increment calculation wherever applicable. At each monitoring station fulfilling a few data coverage criteria, measured concentrations in the base year 2009 are explained to the extent possible and then modelled for the past and future. More than 1850 monitoring stations are covered, including more than 300 traffic stations and 80% of the stations which exceeded the EU air quality limit values in 2009. As a validation, we compare modelled trends in the period 2000-2008 to observations, which are well reproduced. The modelling scheme is applied here to quantify explicitly source contributions to ambient concentrations at several critical monitoring stations, displaying the differences in spatial origin and chemical composition of urban roadside PM10 across Europe. Furthermore, we analyse the predicted evolution of PM10 concentrations in the European Union until 2030 under different policy scenarios. Significant improvements in ambient PM10 concentrations are expected assuming successful implementation of already agreed legislation; however, these will not be large enough to ensure attainment of PM10 limit values in hot spot locations such as Southern Poland and major European cities. Remaining issues are largely eliminated in a scenario applying the best available emission control technologies to the maximal technically feasible extent

EURODELTA - Evaluation of a Sectoral Approach to Integrated Assessment Modeling - Second Report

The EURODELTA project is a continuing collaboration between the European Commission Joint Research Centre (JRC) at Ispra (Italy) and five air quality modeling teams at Ineris (France), the Free University of Berlin (Germany), Met.no (Norway), TNO (Netherlands) and SMHI (Sweden). This phase of Eurodelta investigates how different air quality models would represent the effect on pollutant impacts of applying, on a European scale, emission reductions to individual emission sectors. The reason for doing this is to test whether there are important sensitivities not captured by the sound science approach to air quality policy making on a European scale which is based on an integrated assessment (IA) approach and embodied in the IIASA RAINS/GAINS model. This study shows that there are important differences between sectors in the amount of concentration (deposition) reduction obtained by changing a pollutant emission. This difference is not accounted for in the present process used to evaluate future national emissions ceiling reductions for both beneficial effect and cost-effectiveness. This raises the possibility that, when national bodies consider how to implement an emission ceiling taking account of the information used in deriving that ceiling, choices might be made that are less effective than expected.JRC.DDG.H.4-Transport and air qualit

Emissions of Carbonaceous Particulate Matter and Ultrafine Particles from Vehicles-A Scientific Review in a Cross-Cutting Context of Air Pollution and Climate Change

Featured Application Key conclusions and recommendations are proposed to enlighten decision makers in view of the next regulations on vehicle emissions in Europe and worldwide through the synergistic contexts of air quality and climate change. Airborne particulate matter (PM) is a pollutant of concern not only because of its adverse effects on human health but also on visibility and the radiative budget of the atmosphere. PM can be considered as a sum of solid/liquid species covering a wide range of particle sizes with diverse chemical composition. Organic aerosols may be emitted (primary organic aerosols, POA), or formed in the atmosphere following reaction of volatile organic compounds (secondary organic aerosols, SOA), but some of these compounds may partition between the gas and aerosol phases depending upon ambient conditions. This review focuses on carbonaceous PM and gaseous precursors emitted by road traffic, including ultrafine particles (UFP) and polycyclic aromatic hydrocarbons (PAHs) that are clearly linked to the evolution and formation of carbonaceous species. Clearly, the solid fraction of PM has been reduced during the last two decades, with the implementation of after-treatment systems abating approximately 99% of primary solid particle mass concentrations. However, the role of brown carbon and its radiative effect on climate and the generation of ultrafine particles by nucleation of organic vapour during the dilution of the exhaust remain unclear phenomena and will need further investigation. The increasing role of gasoline vehicles on carbonaceous particle emissions and formation is also highlighted, particularly through the chemical and thermodynamic evolution of organic gases and their propensity to produce particles. The remaining carbon-containing particles from brakes, tyres and road wear will still be a problem even in a future of full electrification of the vehicle fleet. Some key conclusions and recommendations are also proposed to support the decision makers in view of the next regulations on vehicle emissions worldwide

Modeling organic aerosols during MILAGRO: importance of biogenic secondary organic aerosols

The meso-scale chemistry-transport model CHIMERE is used to assess our understanding of major sources and formation processes leading to a fairly large amount of organic aerosols – OA, including primary OA (POA) and secondary OA (SOA) – observed in Mexico City during the MILAGRO field project (March 2006). Chemical analyses of submicron aerosols from aerosol mass spectrometers (AMS) indicate that organic particles found in the Mexico City basin contain a large fraction of oxygenated organic species (OOA) which have strong correspondence with SOA, and that their production actively continues downwind of the city. The SOA formation is modeled here by the one-step oxidation of anthropogenic (i.e. aromatics, alkanes), biogenic (i.e. monoterpenes and isoprene), and biomass-burning SOA precursors and their partitioning into both organic and aqueous phases. Conservative assumptions are made for uncertain parameters to maximize the amount of SOA produced by the model. The near-surface model evaluation shows that predicted OA correlates reasonably well with measurements during the campaign, however it remains a factor of 2 lower than the measured total OA. Fairly good agreement is found between predicted and observed POA within the city suggesting that anthropogenic and biomass burning emissions are reasonably captured. Consistent with previous studies in Mexico City, large discrepancies are encountered for SOA, with a factor of 2–10 model underestimate. When only anthropogenic SOA precursors were considered, the model was able to reproduce within a factor of two the sharp increase in OOA concentrations during the late morning at both urban and near-urban locations but the discrepancy increases rapidly later in the day, consistent with previous results, and is especially obvious when the column-integrated SOA mass is considered instead of the surface concentration. The increase in the missing SOA mass in the afternoon coincides with the sharp drop in POA suggesting a tendency of the model to excessively evaporate the freshly formed SOA. Predicted SOA concentrations in our base case were extremely low when photochemistry was not active, especially overnight, as the SOA formed in the previous day was mostly quickly advected away from the basin. These nighttime discrepancies were not significantly reduced when greatly enhanced partitioning to the aerosol phase was assumed. Model sensitivity results suggest that observed nighttime OOA concentrations are strongly influenced by a regional background SOA (~1.5 μg/m&lt;sup&gt;3&lt;/sup&gt;) of biogenic origin which is transported from the coastal mountain ranges into the Mexico City basin. The presence of biogenic SOA in Mexico City was confirmed by SOA tracer-derived estimates that have reported 1.14 (&amp;plusmn;0.22) μg/m&lt;sup&gt;3&lt;/sup&gt; of biogenic SOA at T0, and 1.35 (&amp;plusmn;0.24) μg/m&lt;sup&gt;3&lt;/sup&gt; at T1, which are of the same order as the model. Consistent with other recent studies, we find that biogenic SOA does not appear to be underestimated significantly by traditional models, in strong contrast to what is observed for anthropogenic pollution. The relative contribution of biogenic SOA to predicted monthly mean SOA levels (traditional approach) is estimated to be more than 30% within the city and up to 65% at the regional scale which may help explain the significant amount of modern carbon in the aerosols inside the city during low biomass burning periods. The anthropogenic emissions of isoprene and its nighttime oxidation by NO&lt;sub&gt;3&lt;/sub&gt; were also found to enhance the SOA mean concentrations within the city by an additional 15%. Our results confirm the large underestimation of the SOA production by traditional models in polluted regions (estimated as 10–20 tons within the Mexico City metropolitan area during the daily peak), and emphasize for the first time the role of biogenic precursors in this region, indicating that they cannot be neglected in urban modeling studies

Spatial and sector-specific contributions of emissions to ambient air pollution and mortality in European cities: a health impact assessment

Background Ambient air pollution is a major risk to health and wellbeing in European cities. We aimed to estimate spatial and sector-specific contributions of emissions to ambient air pollution and evaluate the effects of source-specific reductions in pollutants on mortality in European cities to support targeted source-specific actions to address air pollution and promote population health. Methods We conducted a health impact assessment of data from 2015 for 857 European cities to estimate source contributions to annual PM2·5 and NO2 concentrations using the Screening for High Emission Reduction Potentials for Air quality tool. We evaluated contributions from transport, industry, energy, residential, agriculture, shipping, and aviation, other, natural, and external sources. For each city and sector, three spatial levels were considered: contributions from the same city, the rest of the country, and transboundary. Mortality effects were estimated for adult populations (ie, ≥20 years) following standard comparative risk assessment methods to calculate the annual mortality preventable on spatial and sector-specific reductions in PM2·5 and NO2. Findings We observed strong variability in spatial and sectoral contributions among European cities. For PM2·5, the main contributors to mortality were the residential (mean contribution of 22·7% [SD 10·2]) and agricultural (18·0% [7·7]) sectors, followed by industry (13·8% [6·0]), transport (13·5% [5·8]), energy (10·0% [6·4]), and shipping (5·5% [5·7]). For NO2, the main contributor to mortality was transport (48·5% [SD 15·2]), with additional contributions from industry (15·0% [10·8]), energy (14·7% [12·9]), residential (10·3% [5·0]), and shipping (9·7% [12·7]). The mean city contribution to its own air pollution mortality was 13·5% (SD 9·9) for PM2·5 and 34·4% (19·6) for NO2, and contribution increased among cities of largest area (22·3% [12·2] for PM2·5 and 52·2% [19·4] for NO2) and among European capitals (29·9% [12·5] for PM2·5 and 62·7% [14·7] for NO2). Interpretation We estimated source-specific air pollution health effects at the city level. Our results show strong variability, emphasising the need for local policies and coordinated actions that consider city-level specificities in source contributions. Funding Spanish Ministry of Science and Innovation, State Research Agency, Generalitat de Catalunya, Centro de Investigación Biomédica en red Epidemiología y Salud Pública, and Urban Burden of Disease Estimation for Policy Making 2023-2026 Horizon Europe project

Exploration of the influence of environmental conditions on secondary organic aerosol formation and organic species properties using explicit simulations: development of the VBS-GECKO parameterization

Atmospheric chambers have been widely used to study secondary organic aerosol (SOA) properties and formation from various precursors under different controlled environmental conditions and to develop parameterization to represent SOA formation in chemical transport models (CTMs). Chamber experiments are however limited in number, performed under conditions that differ from the atmosphere and can be subject to potential artefacts from chamber walls. Here, the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) modelling tool has been used in a box model under various environmental conditions to (i) explore the sensitivity of SOA formation and properties to changes on physical and chemical conditions and (ii) develop a volatility basis set (VBS)-type parameterization. The set of parent hydrocarbons includes n-alkanes and 1-alkenes with 10, 14, 18, 22 and 26 carbon atoms, α-pinene, β-pinene and limonene, benzene, toluene, o-xylene, m-xylene and p-xylene. Simulated SOA yields and their dependences on the precursor structure, organic aerosol load, temperature and NOx levels are consistent with the literature. GECKO-A was used to explore the distribution of molar mass, vaporization enthalpy, OH reaction rate and Henry's law coefficient of the millions of secondary organic compounds formed during the oxidation of the different precursors and under various conditions. From these explicit simulations, a VBS-GECKO parameterization designed to be implemented in 3-D air quality models has been tuned to represent SOA formation from the 18 precursors using GECKO-A as a reference. In evaluating the ability of VBS-GECKO to capture the temporal evolution of SOA mass, the mean relative error is less than 20&thinsp;% compared to GECKO-A. The optimization procedure has been automated to facilitate the update of the VBS-GECKO on the basis of the future GECKO-A versions, its extension to other precursors and/or its modification to carry additional information.</p