The time evolution of the adiabatic state populations for the two sets of range-separation parameters are shown in Figures ). For set A, the dynamics starts by exciting [Fe(cpmp) 2 ] 2+ into higher-lying singlet states S N (N≥ 2, orange curve), from which most of the population undergoes ultrafast intersystem crossing to higher-lying triplet states T N (N≥ 3, violet curve). Within the triplet manifold, further relaxation to the T 2 (light-blue curve) and T 1 (dark-blue curve) occur on sub-100 fs time scales. After ca. 300 fs, the population is stable in the T 1 , T 2 , and T N states. As a minor reaction channel, population initially decays from the S N to the S 1 state (red curve) on a 2 ps time scale, from where also the T N states are reached.