Transition metal complexes are widely applied as catalysts, photosensitizers and dyes. Popular examples are six-coordinated ruthenium(II) and iridium(III) polypyridine complexes that have found numerous applications in photocatalysis and light-harvesting technologies including dye-sensitized solar cells. However, due to the costs of rare metals, there is a significant tendency to switch to the more abundant and economically feasible copper or iron complexes. Unfortunately, the usage of the latter in standard polypyrdine complexes is still rather limited due to the fast deactivation of metal-to-ligand charge-transfer (MLCT) states via metal-centered (MC) ones to the ground state. This relaxation prevents utilizing the initial charge separation in MLCT states for further redox reactions. In order to find novel complexes with long-lived MLCT states, the excited-state behavior of such compounds should be carefully rationalized. A detailed picture of the excitedstate reactivity can be obtained by simulating the photodynamics of the transition metal complexes explicitly. If the reaction coordinates of the problem at hand are known and comprise only a few degrees of freedom, it it possible to simulate the excited-state processes with high accuracy using quantum wave packet dynamics. However, if the reaction includes too many degrees of freedom or the relevant ones cannot be guessed a priori, an extended strategy is to leverage ab initio molecular dynamics methods such a) Electronic mail: olga.bokareva@uni-rostock.de b) Electronic mail: jan.patrick.zobel@univie.ac.at as trajectory surface hopping (TSH), which simulate the photodynamics of a molecule in full dimensionality. Here, the nuclear motion is described approximately by classical trajectories in place of the quantum wave packets.