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An explanation is provided for the ultrafast photo-excited electron dynamicsin low-spin Ruthenium (II) organic complexes. The experimentally-observedsinglet to triplet decay in the metal-to-ligand charge-transfer (MLCT) statescontradicts the expectation that the system should oscillate between thesinglet and triplet states in the presence of a large spin-orbit coupling andthe absence of a significance change in metal-ligand bond length. This dilemmais solved with a novel quantum decay mechanism that causes a singlet to tripletdecay in about 300 femtoseconds. The decay is mediated by the tripletmetal-centered state ($^3$MC) state even though there is no direct couplingbetween the $^1$MLCT and $^3$MC states. The coupling between the $^3$MLCT and$^3$MC via excited phonon states leads to vibrational cooling that allows thelocal system to dissipate the excess energy. In the relaxed state, thepopulation of the $^3$MC state is low and the metal-ligand bond length isalmost unchanged with respect to the initial photoexcited state, in agreementwith experiment.

Ultrafast Electron Dynamics Theory of Photo-excited Ruthenium Complexes