CHIMERE is a chemistry-transport model designed for regional atmospheric composition. It can be used at a variety of scales from local to continental domains. However, due to the model design and its historical use as a regional model, major limitations had remained, hampering its use at hemispheric scale, due to the coordinate system used for transport as well as to missing processes that are important in regions outside Europe. Most of these limitations have been removed in the CHIMERE-2017 version, allowing its use in any region of the world and at any scale, from the scale of a single urban area up to hemispheric scale, with or without polar regions included. Other important improvements have been made in the treatment of the physical processes affecting aerosols and the emissions of mineral dust. From a computational point of view, the parallelization strategy of the model has also been updated in order to improve model numerical performance and reduce the code complexity. The present article describes all these changes. Statistical scores for a model simulation over continental Europe are presented, and a simulation of the circumpolar transport of volcanic ash plume from the Puyehue volcanic eruption in June 2011 in Chile provides a test case for the new model version at hemispheric scale.

The CHIMERE chemistry-transport model v2020r1 replaces the v2017r5 version and provides numerous novelties. The most important of these is the online coupling with the Weather Research and Forecasting (WRF) meteorological model via the OASIS3 – Model Coupling Toolkit (MCT) external coupler. The model can still be used in offline mode; the online mode enables us to take into account the direct and indirect effects of aerosols on meteorology. This coupling also enables using the meteorological parameters with sub-hourly time steps. Some new parameterizations are implemented to increase the model performance and the user's choices: dimethyl sulfide (DMS) emissions, additional schemes for secondary organic aerosol (SOA) formation with volatility basis set (VBS) and H²O, improved schemes for mineral dust, biomass burning, and sea-salt emissions. The NO_x emissions from lightning are added. The model also includes the possibility to use the operator-splitting integration technique. The subgrid-scale variability calculation of concentrations due to emission activity sectors is now possible. Finally, a new vertical advection scheme has been implemented, which is able to simulate more correctly long-range transport of thin pollutant plumes.

Chemical Ionisation Mass Spectrometer measurements of hydroxyl radical (OH) and the sum of hydroperoxy and organic peroxy (HO₂+RO₂) radicals were conducted during the MEGAPOLI summer field campaign at the SIRTA observatory near Paris, France, in July 2009. OH and (HO₂+RO₂) showed a typical diurnal variation with averaged daytime maxima values around 5×10⁶ and 1.2×10⁸ molecule cm⁻³, respectively. Simultaneously, a large number of ancillary measurements, such as NO_x, O₃, HONO, HCHO and other VOCs were also conducted. These data provide an opportunity to assess our understanding of the radical chemistry in a suburban environment by comparing the radical observations to calculations. First, OH mixing ratios were estimated by a simple Photo Stationary State (PSS) calculation. PSS calculations overestimate the OH mixing ratio by 50%, especially at NO_x mixing ratios lower than 10 ppb, suggesting that some loss processes were missing in the calculation at low NO_x. Then, a photochemical box model simulation based on the Master Chemical Mechanism (MCM) and constrained by ancillary measurements was run to calculate radical concentrations. Three different modelling procedures were tested, varying the way the unconstrained secondary species were estimated, to cope with the unavoidable lack of their measurements. They led to significant differences in simulated radical concentrations. OH and (HO₂+RO₂) concentrations estimated by two selected model version were compared with measurements. These versions of the model were chosen because they lead, respectively, to the higher and lower simulated radical concentrations and are thus the two extremes versions. The box model showed better results than PSS calculations, with a slight overestimation of 12% and 5%, for OH and (HO₂+RO₂) respectively, in average for the reference model, and an overestimation of approximately 20% for OH and an underestimation for (HO₂+RO₂) for the other selected model version. Thus, we can conclude from our study that OH and (HO₂+RO₂) radical levels agree on average with observations within the uncertainty range. Finally, an analysis of the radical budget, on a daily basis (06:00–18:00 UTC), indicates that HONO photolysis (~35%), O₃ photolysis (~23%), and aldehydes and ketones photolysis (~16% for formaldehyde and 18% for others) are the main radical initiation pathways. According to the MCM modelling, the reactions of RO₂ with NO₂ (~19%), leading mainly to PAN formation, is a significant termination pathway in addition to the main net loss via reaction of OH with NO₂ (~50%).

Air pollution reaching hazardous levels in many Chinese cities has been a major concern in China over the past decades. New policies have been applied to regulate anthropogenic pollutant emissions, leading to changes in atmospheric composition and in particulate matter (PM) production. Increasing levels of atmospheric ammonia columns have been observed by satellite during recent years. In particular, observations from the Infrared Atmospheric Sounding Interferometer (IASI) reveal an increase of these columns by 15 % and 65 % from 2011 to 2013 and 2015, respectively, over eastern China. In this paper we performed model simulations for 2011, 2013 and 2015 in order to understand the origin of this increase and to quantify the link between ammonia and the inorganic components of particles: ${\mathrm{NH}}_{\mathrm{4}\left(\mathrm{p}\right)}^{+}/{\mathrm{SO}}_{\mathrm{4}\left(\mathrm{p}\right)}^{\mathrm{2}-}/{\mathrm{NO}}_{\mathrm{3}\left(\mathrm{p}\right)}^{-}$ . Interannual change of meteorology can be excluded as a reason: year 2015 meteorology leads to enhanced sulfate production over eastern China, which increases the ammonium and decreases the ammonia content, which is contrary to satellite observations. Reductions in SO₂ and NO_x emissions from 2011 to 2015 of 37.5 % and 21 % respectively, as constrained from satellite data, lead to decreased inorganic matter (by 14 % for ${\mathrm{NH}}_{\mathrm{4}\left(\mathrm{p}\right)}^{+}+{\mathrm{SO}}_{\mathrm{4}\left(\mathrm{p}\right)}^{\mathrm{2}-}+{\mathrm{NO}}_{\mathrm{3}\left(\mathrm{p}\right)}^{-}$ ). This in turn leads to increased gaseous NH_3(g) tropospheric columns by as much as 24 % and 49 % (sampled corresponding to IASI data availability) from 2011 to 2013 and 2015 respectively and thus can explain most of the observed increase.

The indirect effects of aerosol are particularly important over regions where meteorological conditions and aerosol content are favourable to cloud formation. This was observed during the Intensive Cloud Aerosol Measurement Campaign (IMPACT) (European Integrated project on Aerosol Cloud Climate and Air quality Interaction (EUCAARI) project) in the Benelux Union during May 2008. To better understand this cloud formation variability, the indirect effects of aerosol have been included within the WRF-CHIMERE online model. By comparing model results to the aircraft measurements of IMPACT, to surface measurements from EMEP and AIRBASE and to MODIS satellite measurements, we showed that the model is able to simulate the variability and order of magnitude of the observed number of condensation nuclei (CN), even if some differences are identified for specific aerosol size and location. To quantify the impact of the local anthropogenic emissions on cloud formation, a sensitivity study is performed by halving the surface emissions fluxes. It is shown that the indirect radiative effect (IRE) at the surface is positive for both shortwave and longwave with a net warming of +0.99 W/m². In addition, important instantaneous changes are modelled at local scale with up to ±6 °C for temperatures and ±50 mm/day for precipitation.

The atypical huge forest fires observed in France during the summer of 2022 are modeled using the CHIMERE model. The impact of these emissions is quantified on ozone, aerosols and aerosol optical depth (AOD). The fires also influence the surface by destroying the vegetation and creating new erodible surfaces. This increases the mineral dust emissions but also reduces the leaf area index (LAI), and then it decreases the biogenic emissions and the dry deposition of gases such as ozone. Results show that the fires induce numerous increases in surface ozone and particulate matter (PM) concentrations close to the sources but also in downwind remote sites such as the Paris area. During the period of the most intense fires in July, the impact of concentrations is mainly due to emissions themselves, and later, in August, ozone and PM concentrations continue to increase but this time due to changes in the burned surfaces.