The dynamics were simulated by full-dimensional trajectory surface hopping (TSH) based on Tully's fewest switches 31 a threestep propagator technique , and local diabatisation , as implemented in the SHARC2.1 software. Our model includes the lowest 15 singlet and 18 triplet electronic states of [Fe(bmip) 2 ] 2+ . The B3LYP*/TZVP DFT/TD-DFT calculations for the LVC and full (on-the-fly) PESs were carried out using the ORCA5.0 quantum chemistry program package . Further details of the utilised methodology are given in the ESI.