We now turn to the comparison between TDDFT and CASPT2 results. For singlet states, CASPT2 predicts the MC state (blue line) above the MLCT state (red line). This situation is independent of the IPEA shift, as discussed in more detail in Section From comparing the excitation energies of the lowestenergy singlet and triplet states of MC and MLCT character, the best agreement between CASPT2 and TDDFT is reached for the range-separation parameters (0.20; 0.08) marked in the future discussion as Set B. This is the only parameter pair for which the same state ordering as in the CASPT2 calculations is found. Note that the J * value for the Set B is 0.018 compared to the 0.007 for the Set A suggested by the optimal tuning procedure, see Section II. In addition, the difference between the TDDFT and CASPT2 excitation energies is only 0.1-0.3 eV. While the (0.20; 0.08) parameter set B differs notably from the optimaltuned set A of (0.00; 0.14), it also provided a reasonable description of the absorption spectrum (Figure ), albeit with somewhat larger deviations from the experimental reference. In an effort to solve for this dilemma, we will now analyse the consequences of using both sets beyond the Franck-Condon region. First, we evaluate the agreement of the absorption spectra with the experimental data. Second, we investigate the behavior of the potential en- ergy curves along the important Fe-N bond length. Then, we simulate the excited-state dynamics of the complex.