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• W2027748614 abstract "The superexchange mechanism of electron-transfer reactions is studied for time-dependent donor–bridge–acceptor systems. It is shown that superexchange may not be a relevant mechanism in a situation where donor and acceptor states are off-resonant to the bridge with an energy gap much greater than KBT. The competing mechanism in this case involves coherent through-bridge transfer. Methods for estimating its contribution to the electron-transfer probability are presented. It is also shown that the superexchange component of the electron-transfer probability can generally be described by a time-dependent two-state effective Hamiltonian. The off-diagonal element of this Hamiltonian is a generalized superexchange matrix element applicable to time-dependent donor–bridge–acceptor systems. It is nonperturbative and should be used to compute time-dependent superexchange pathways. The derivation of the effective Hamiltonian also applies to time-dependent superexchange systems with multiple donor (acceptor) states. All calculations are carried out on azurin and they involve molecular dynamics simulations coupled to electronic-structure/dynamics calculations using the complete neglect of differential overlap method." @default.
• W2027748614 created "2016-06-24" @default.
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• W2027748614 date "2001-11-22" @default.
• W2027748614 modified "2023-09-25" @default.
• W2027748614 title "Electron transfer through fluctuating bridges: On the validity of the superexchange mechanism and time-dependent tunneling matrix elements" @default.
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• W2027748614 doi "https://doi.org/10.1063/1.1412874" @default.
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