First, the electronic structure is notorious for the many complications arising from static and dynamic correlations. Second, dynamics simulations for typical systems will have to cope with hundreds of nuclear degrees of freedom (DOFs). In terms of electronic structure theory, density functional theory (DFT) with tailored exchange-correlation (XC) functionals have proven a low-cost yet reasonably accurate alternative to expensive wave function calculations. In particular non-empirically tuned range-separated functionals 10,11 perform rather well, although often the actual agreement, e.g. with absorption spectra is hard to predict clear beforehand. A particular challenge is provided by the interplay between MC and MLCT transition as shown in Ref. 13.