Nonequilibrium generalization of Förster-Dexter theory for excitation energy transfer

Physics – Condensed Matter – Statistical Mechanics

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published in {\it Chemical Physics} (special issue on Photoprocesses in Multichromophoric Molecular Assemblies)

Scientific paper

10.1016/S0301-0104(01)00538-9

F\"{o}rster-Dexter theory for excitation energy transfer is generalized for the account of short time nonequilibrium kinetics due to the nonstationary bath relaxation. The final rate expression is presented as a spectral overlap between the time dependent stimulated emission and the stationary absorption profiles, which allows experimental determination of the time dependent rate. For a harmonic oscillator bath model, an explicit rate expression is derived and model calculations are performed in order to examine the dependence of the nonequilibrium kinetics on the excitation-bath coupling strength and the temperature. Relevance of the present theory with recent experimental findings and possible future theoretical directions are discussed.

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