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We investigate the cascade decay mechanism for ultrafast intersystem crossingmediated by the spin-orbit coupling in transition-metal complexes. Aquantum-mechanical description of the cascading process that occurs afterphotoexcitation is presented. The conditions for ultrafast cascading are given,which relate the energy difference between the levels in the cascading processto the electron-phonon self energy. These limitations aid in the determinationof the cascade path. For $Fe^{2+}$ spin-crossover complexes, this leads to theconclusion that the ultrafast decay primarily occurs in the manifold ofantibonding metal-to-ligand charge-transfer states. We also give aninterpretation why some intermediate states are bypassed.

Ultrafast Cascading Theory in Intersystem Crossings in Transition-Metal Complexes