We thus conclude that set B represents the best choice to simulate the dynamics of [Fe(cpmp) 2 ] 2+ . While it did not represent the optimal choice from the ∆SCF tuning (set A), the range-separation parameters from set B also fall in the minimal valley in ∆SCF tuning, thus indicating that it as a good parameter choice from an ab initio point of view. Furthermore, set B could give a good agreement with the experimental absorption spectrum. More importantly, however, set B provided the only range-separation parameters that predicted the lowest-energy states in the same as order as multi-reference CASPT2 calculations.