ALBERT

Description: The accurate simulation of meteorological conditions, especially within the planetary boundary layer (PBL), is of major importance for air quality modeling. In the present work, we have used the Weather Research and Forecast (WRF) model coupled with the chemistry transport model (CTM) CHIMERE to understand the impact of physics parameterizations on air quality simulation during a short-term pollution episode on the Paris region. A lower first model layer with a 4 m surface layer could better reproduce the transport and diffusion of pollutants in a real urban environment. Three canopy models could better reproduce a 2 m temperature (T2) in the daytime but present a positive bias from 1 to 5 °C during the nighttime; the multi-urban canopy scheme “building effect parameterization” (BEP) underestimates the 10 m windspeed (W10) around 1.2 m s−1 for the whole episode, indicating the city cluster plays an important role in the diffusion rate in urban areas. For the simulation of pollutant concentrations, large differences were found between three canopy schemes, but with an overall overestimation during the pollution episode, especially for NO2 simulation, the average mean biases of NO2 prediction during the pollution episode were 40.9, 62.2, and 29.7 µg m−3 for the Bulk, urban canopy model (UCM), and BEP schemes, respectively. Meanwhile, the vertical profile of the diffusion coefficients and pollutants indicated an important impact of the canopy model on the vertical diffusion. The PBL scheme sensitivity tests displayed an underestimation of the height of the PBL when compared with observations issued from the Lidar. The YonSei University scheme YSU and Boulac PBL schemes improved the PBL prediction compared with the Mellor–Yamada–Janjic (MYJ) scheme. All the sensitivity tests, except the Boulac–BEP, could not fairly reproduce the PBL height during the pollution episode. The Boulac–BEP scheme had significantly better performances than the other schemes for the simulation of both the PBL height and pollutants, especially for the NO2 and PM2.5 (particulate matter 2.5 micrometers or less in diameter) simulations. The mean bias of the NO2, PM2.5, and PM10 (particulate matter 10 micrometers or less in diameter) prediction were −5.1, 1.2, and −8.6 µg m−3, respectively, indicating that both the canopy schemes and PBL schemes have a critical effect on air quality prediction in the urban region.

Description: The Paris megacity experiences frequent particulate matter (i.e.PM2.5, particulate matter with a diameter less than 2.5 µm) pollution episodes in spring (March–April). At this time of the year, large numbers of the particles consist of ammonium sulfate and nitrate which are formed from ammonia (NH3) released during fertilizer spreading practices and transported from the surrounding areas to Paris. There is still limited knowledge of the emission sources around Paris, their magnitude, and their seasonality. Using space-borne NH3 observation records of 10 years (2008–2017) and 5 years (2013–2017) provided by the Infrared Atmospheric Sounding Interferometer (IASI) and the Cross-Track Infrared Sounder (CrIS) instrument, regional patterns of NH3 variabilities (seasonal and interannual) are derived. Observations reveal identical high seasonal variability with three major NH3 hotspots found from March to August. The high interannual variability is discussed with respect to atmospheric total precipitation and temperature. A detailed analysis of the seasonal cycle is performed using both IASI and CrIS instrument data, together with outputs from the CHIMERE atmospheric model. For 2014 and 2015, the CHIMERE model shows coefficients of determination of 0.58 and 0.18 when compared to IASI and CrIS, respectively. With respect to spatial variability, the CHIMERE monthly NH3 concentrations in spring show a slight underrepresentation over Belgium and the United Kingdom and an overrepresentation in agricultural areas in the French Brittany–Pays de la Loire and Plateau du Jura region, as well as in northern Switzerland. In addition, PM2.5 concentrations derived from the CHIMERE model have been evaluated against surface measurements from the Airparif network over Paris, with which agreement was found (r2 = 0.56) with however an underestimation during spring pollution events. Using HYSPLIT cluster analysis of back trajectories, we show that NH3 total columns measured in spring over Paris are enhanced when air masses originate from the north-east (e.g. the Netherlands and Belgium), highlighting the importance of long-range transport in the NH3 budget over Paris. Variability in NH3 in the north-east region is likely to impact NH3 concentrations in the Parisian region since the cross-correlation function is above 0.3 (at lag = 0 and 1 d). Finally, we quantify the key meteorological parameters driving the specific conditions important for the formation of PM2.5 from NH3 in the Île-de-France region in spring. Data-driven results based on surface PM2.5 measurements from the Airparif network and IASI NH3 measurements show that a combination of the factors such as a low boundary layer of ∼500 m, a relatively low temperature of 5 ∘C, a high relative humidity of 70 %, and wind from the north-east contributes to a positive PM2.5 and NH3 correlation.

Description: Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.

Description: Agriculture is the main source of ammonia (NH3) in France, an important gaseous precursor of atmospheric particulate matter (PM). National and global emission inventories are known to have difficulty representing the large spatial and temporal variability inherent to atmospheric NH3. In this study, we compare NH3 emissions in France during spring 2011 from one reference inventory, the TNO inventory, and two alternative inventories that account in different manners for both the spatial and temporal variabilities of the emissions: (i) the NH3SAT satellite-derived inventory based on IASI NH3 columns and (ii) the CADASTRE-CIT inventory that combines NH3 emissions due to nitrogen fertilization calculated with the mechanistic model VOLT'AIR on the database of the CADASTRE_NH3 framework and other source emissions from the CITEPA. The total spring budgets, from March to May 2011, at the national level are higher when calculated with both alternative inventories than with the reference, the difference being more marked with CADASTRE-CIT. NH3SAT and CADASTRE-CIT inventories both yield to large NH3 spring emissions due to fertilization on soils with high pH in the northeastern part of France (65 and 135 kt NH3, respectively, vs. 48 kt NH3 for TNO-GEN), while soil properties are not accounted for by the TNO-GEN methodology. For the other parts of France, the differences are smaller. The timing of fertilization and associated ammonia emissions is closely related to the nitrogen requirements and hence the phenological stage of the crops, and therefore to the crop year's specific weather conditions. Maximum emissions are observed in March for 2011 for some regions for both alternative inventories, while April is the period with maximum emissions for the reference inventory regardless of the region or the year. Comparing the inventories at finer temporal resolutions, typically at daily scale, large differences are found. The convergence of alternative, independent and complementary methods on the spatiotemporal representation of the spring NH3 emissions, particularly over areas where the contribution of mineral fertilizer spreading to the spring budget is strong, encourages further developments in both prospective complementary directions, as this will help improve national NH3 emission inventories.