We now present and discuss our results obtained by the B3LYP and PBE0 global hybrid functionals and the CAM-B3LYP and LC-BLYP range-separated hybrids. As seen in Figure , in all cases, a non-negligible initial 1 MC population appears, with the 1 MLCT still being the major component of the excited-state manifold, generated by the electronic excitation. However, the 1 MC states here do play a role in the relaxation mechanism, which was not the case for the B3LYP* functional and the GGA methods (see Figure ). Furthermore, the 3 MLCT/ 3 MC branching disappears, as the 3 MLCT population decays rapidly, only up to ca. 5% remains at the final 1 ps step of the simulations. The 3 MC component, on the other hand, becomes dominant and no population decay is observed. These results are in clear disagreement with the experimental observations. We note that for PBE0, CAM-B3LYP, and LC-BLYP, 3 LL states (corresponding to ligand-ligand transitions) got included in the LVC models, thus 3 LL population curves appear in Figures , albeit these populations are so small that they are negligible (this is because the 3 LL states are located in higherenergy regions that are energetically not accessible for the dynamics).