Electron Transfer Theories

doi:10.1002/9783527647668.ch1

Cited by 2 publications

(1 citation statement)

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“…Many theoretical approaches describe electron transfer in condensed phase in terms of the energy-gap coordinate—the quantity evaluated by mapping the system’s nuclear degrees of freedom onto the energy gap

between the ET reactant and product states [ 26 , 27 , 28 ]. Using the

quantity as the reaction coordinate allows one to reduce the dimensionality of the nuclear configuration space, and ultimately admit the one-dimensional picture of ET with the two intersecting electronic surfaces for the reactant and product states in the diabatic presentation.…”

Section: Introductionmentioning

confidence: 99%

Semiclassical Theory of Multistage Nonequilibrium Electron Transfer in Macromolecular Compounds in Polar Media with Several Relaxation Timescales

Feskov

2022

IJMS

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Many specific features of ultrafast electron transfer (ET) reactions in macromolecular compounds can be attributed to nonequilibrium configurations of intramolecular vibrational degrees of freedom and the environment. In photoinduced ET, nonequilibrium nuclear configurations are often produced at the stage of optical excitation, but they can also be the result of electron tunneling itself, i.e., fast redistribution of charges within the macromolecule. A consistent theoretical description of ultrafast ET requires an explicit consideration of the nuclear subsystem, including its evolution between electron jumps. In this paper, the effect of the multi-timescale nuclear reorganization on ET transitions in macromolecular compounds is studied, and a general theory of ultrafast ET in non-Debye polar environments with a multi-component relaxation function is developed. Particular attention is paid to designing the multidimensional space of nonequilibrium nuclear configurations, as well as constructing the diabatic free energy surfaces for the ET states. The reorganization energies of individual ET transitions, the equilibrium energies of ET states, and the relaxation properties of the environment are used as input data for the theory. The effect of the system-environment interaction on the ET kinetics is discussed, and mechanisms for enhancing the efficiency of charge separation in macromolecular compounds are analyzed.

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between the ET reactant and product states [ 26 , 27 , 28 ]. Using the

Section: Introductionmentioning

confidence: 99%