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Hsu 2022 J Chem Phys

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Hsu CP, Hammarström L, Newton MD (2022) 65 years of electron transfer. J Chem Phys 157:020401. https://doi.org/10.1063/5.0102889

» PMID: 35840385 Open Access

Hsu CP, Hammarström L, Newton MD (2022) J Chem Phys

Abstract: Electron transfer (ET), as a simplest chemical reaction, is the fundamental step in the oxidation–reduction reaction, involved in a large class of electrochemistry, biochemistry, and organic and inorganic chemistry. 65 years have passed since the introduction of the series of work on the free energies and the rates for ET reactions.1,2 This contribution began a rapid transformation of the field that advanced through experimental work by Sutin,3 Taube,4 and others and detailed theoretical treatments by Marcus, Hush, Levitch, Dogonadze, and Jortner.5–11 For more than half of a century, ET has become an important ingredient in many modern research themes, which this special topic collection aimed to cover.

In the ET process, a charge is moved from one spatial part of the system to another, and thus, the energy difference of the two electronic states is coupled to the dielectric polarization from the environment, leading to the activation energy in the model of Rudy’s derivation. This concept serves as an important starting point for the quantum dissipative dynamics under various non-equilibrium statistical mechanical treatments, which is also generalized for linear and nonlinear spectroscopy. Discussions on various approximations, predictions, and extensions followed, such as the inner vs outer reorganization energy, inverted region behavior, adiabatic vs nonadiabatic models, solvent and solute dynamics, quantum vs classical treatment of nuclei motion, and strong vs weak coupling limit. The theoretical account of two-state and multi-state problems has been useful not only for ET, but it has also influenced the understanding of other processes, such as energy transfer, proton transfer, and proton-coupled electron transfer as well as nonlinear spectroscopy and, more recently, singlet fission.

Bioblast editor: Gnaiger E


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