Model of Ultrafast Intersystem Crossing in Photoexcited Transition-Metal Organic Compounds

作者:van Veenendaal Michel*; Chang Jun; Fedro A J
来源:Physical Review Letters, 2010, 104(6): 067401.
DOI:10.1103/PhysRevLett.104.067401

摘要

The mechanism behind fast intersystem crossing in transition-metal complexes is shown to be a result of the dephasing of the photoexcited state to the phonon continuum of a different state with a significantly different transition metal-ligand distance. The coupling is a result of the spin-orbit interaction causing a change in the local moment. A recurrence to the initial state is prevented by the damping of the phonon oscillation. The decay time is faster than the oscillation frequency of the transition metal-ligand stretch mode, in agreement with experiment. For energies above the region where the strongest coupling occurs, a slower "leakage-type'' decay is observed. If the photoexcited state is lower in energy than the state it couples to, then there is no decay.

  • 出版日期2010-2-12