Electronic coherence in mixed-valence systems: Spectral analysis

Details Electronic coherence in mixed-valence systems: Spectral analysis Electronic coherence in mixed-valence systems: Spectral analysis

2000-08-18

arxiv.org/abs/physics/0008164v1

J. Phys. Chem.A, vol.103, 9460-9468 (1999)

Physics

Chemical Physics

24 pages, 11 figures

Scientific paper

The electron transfer kinetics of mixed-valence systems is studied via solving the eigen-structure of the two-state non-adiabatic diffusion operator for a wide range of electronic coupling constants and energy bias constants. The calculated spectral structure consists of three branches in the eigen-diagram, a real branch corresponding to exponential or multi-exponential decay and two symmetric branches corresponding to population oscillations between donor and acceptor states. The observed electronic coherence is shown as a result of underdamped Rabi oscillations in an overdamped solvent environment. The time-evolution of electron population is calculated by applying the propagator constructed from the eigen-solution to the non-equilibrium initial preparation, and it agrees perfectly with the result of a direct numerical propagation of the density matrix. The resulting population dynamics confirms that increasing the energy bias destroys electronic coherence.

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