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- W1985743171 abstract "Long-range coherent electron transfer between a donor and an acceptor is often assisted by intermediate molecular bridge, via the superexchange tunneling mechanism. The effect of electronic–nuclear coupling intensity on the tunneling rate and mechanism is analyzed using a generalized spin-boson model, in which the two level system, representing the donor and the acceptor is coupled to a dissipative nuclear bath only indirectly, via additional N bridge sites. A Langevin–Schroedinger equation, based on a mean field approximation, is applied in order to study the corresponding many-body dynamics, and the results are supported by numerically exact calculations for a single nuclear bridge mode. At zero temperature and when the electron tunneling is slower than the nuclear motion, the main effect of electronic–nuclear coupling is the dissipation of electronic energy at the bridge into nuclear vibrations. At small coupling intensities, the electronic tunneling rate increases due to this dissipative mechanism, but as the coupling intensity increases the tunneling into the acceptor is suppressed and efficient dissipation leads to electronic trapping (solvation) at the bridge. This analysis agrees with numerous experimental and theoretical studies, emphasizing the importance of the nuclear bridge conformation and the bridge flexibility in controlling the electron transfer rate in donor–bridge–acceptor systems." @default.
- W1985743171 created "2016-06-24" @default.
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- W1985743171 creator A5051518836 @default.
- W1985743171 date "2004-01-01" @default.
- W1985743171 modified "2023-09-27" @default.
- W1985743171 title "Modulations of electronic tunneling rates through flexible molecular bridges by a dissipative superexchange mechanism" @default.
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- W1985743171 doi "https://doi.org/10.1016/j.chemphys.2003.09.026" @default.
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