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General theory of excitation energy transfer in donor-mediator-acceptor systems
Kimura, Akihiro
32402
excited states
luminescence
Markov processes
master equation
molecular electronic states
transition moments
General theory of the excitation energy transfer (EET) in the case of donor-mediator-acceptor system was constructed by using generalized master equation (GME). In this theory, we consider the direct and indirect transitions in the EET consistently. Hence, our theory includes the quantum mechanical interference between the direct and indirect transitions automatically. Memory functions in the GME were expressed by the overlap integrals among the time-dependent emission spectrum of the donor, the absorption spectrum of the mediator, the time-dependent emission spectrum of the mediator, and the absorption spectrum of the acceptor. In the Markov limit of the memory functions, we obtained the rate of EET which consists of three terms due to the direct transition, the indirect transition, and the interference between them. We found that the interference works effectively in the limit of slow thermalization at the intermediate state. The formula of EET rate in this limit was expressed by the convolution of the EET interaction and optical spectra. The interference effect strongly depends on the width of the absorption spectrum of mediator molecule and the energy gap between the donor and the mediator molecules.
journal article
American Institite of Physics
2009-04-16
application/pdf
THE JOURNAL OF CHEMICAL PHYSICS
15
130
154103
154103
http://hdl.handle.net/2237/12630
http://dx.doi.org/10.1063/1.3117622
0021-9606
https://nagoya.repo.nii.ac.jp/record/10787/files/JChemPhys_130_154103.pdf
eng
https://doi.org/10.1063/1.3117622
Copyright (2009) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior per mission of the author and the American Institute of Physics.