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The paper demonstrates the applicability of a special type of density matrix theory for the derivation of generalized Master equations. The density matrix theory has been formulated for the description of the dissipative electron transfer dynamics in molecular complexes. The theoretical approach is based on a representation of the density matrix in appropriately taken diabatic electron-vibrational states. Dissipative effects are taken into account by a coupling of these states to further vibrational modes of the molecular complex as well as to environmental degrees of freedom. The approach is applied to a two-center system as well as to a molecular chain. Memory kernels are derived in second order with respect to the inter-center coupling. The kernels are discussed under the assumption of a quick intra-center relaxation for a part of the vibrational modes as well as for all vibrational modes. Standard expressions for the transition rates between different sites are extended to include finite life times of the vibrational levels. Results which have been obtained in the study of the so-called spin boson model can be simply reproduced. The application of the derived generalized Master equations to the investigation of the motion of Frenkel excitons in molecular chains is also presented.
Michael Schreiber andV. May
"Generalized master equations for exciton dynamics in molecular systems", Proc. SPIE 2362, International Conference on Excitonic Processes in Condensed Matter, (9 February 1995); https://doi.org/10.1117/12.200959
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Michael Schreiber, V. May, "Generalized master equations for exciton dynamics in molecular systems," Proc. SPIE 2362, International Conference on Excitonic Processes in Condensed Matter, (9 February 1995); https://doi.org/10.1117/12.200959