First implementation of secondary inorganic aerosols in the MOCAGE version R2.15.0 chemistry transport model

In this study we develop a secondary inorganic aerosol (SIA) module for the MOCAGE chemistry transport model developed at CNRM. The aim is to have a module suitable for running at different model resolutions and for operational applications with reasonable computing times. Based on the ISORROPIA II thermodynamic equilibrium module, the new version of the model is presented and evaluated at both the global and regional scales. The results show high concentrations of secondary inorganic aerosols in the most polluted regions: Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emission reductions in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the global model outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement with MODIS AOD retrievals in all geographical regions after introducing the new SIA scheme. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA generally gives a better agreement with observations for secondary inorganic aerosol precursors (nitric acid, sulfur dioxide, ammonia), in particular with a reduction of the modified normalized mean bias (MNMB). At the regional scale, over Europe, the model simulation with SIA is compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained from the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants: particulate matter, ozone and nitrogen dioxide concentrations. Introduction of the SIA in MOCAGE provides a reduction in the PM2.5 MNMB of 0.44 on a yearly basis and up to 0.52 for the 3 spring months (March, April, May) when SIAs are at their maximum.