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The main uncertainties regarding the estimation of changes in the Earth's energy budget are related to the role of atmospheric aerosols. These changes are caused by aerosol–radiation (ARIs) and aerosol–cloud interactions (ACIs), which heavily depend on aerosol properties. Since the 1980s, many international modeling initiatives have studied atmospheric aerosols and their climate effects. Phase 3 of the Air Quality Modelling Evaluation International Initiative (AQMEII) focuses on evaluating and intercomparing regional and linked global/regional modeling systems by collaborating with the Task Force on the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) initiative. Within this framework, the main aim of this work is the assessment of the representation of aerosol optical depth (AOD) and the Ångström exponent (AE) in AQMEII Phase 3 simulations over Europe. The evaluation was made using remote-sensing data from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard the Terra and Aqua platforms, and the instruments belonging to the ground-based Aerosol Robotic Network (AERONET) and the Maritime Aerosol Network (MAN). Overall, the skills of AQMEII simulations when representing AOD (mean absolute errors from 0.05 to 0.30) produced lower errors than for the AE (mean absolute errors from 0.30 to 1). Regardless of the models or the emissions used, models were skillful at representing the low and mean AOD values observed (below 0.5). However, high values (around 1.0) were overpredicted for biomass burning episodes, due to an underestimation in the common fires' emissions, and were overestimated for coarse particles – principally desert dust – related to the boundary conditions. Despite this behavior, the spatial and temporal variability of AOD was better represented by all the models than AE variability, which was strongly underestimated in all the simulations. Noticeably, the impact of the model selection when representing aerosol optical properties is higher than the use of different emission inventories. On the other hand, the influence of ARIs and ACIs has a little visible impact compared to the impact of the model used. [ABSTRACT FROM AUTHOR]