DOI: 10.1063/1.451952. Effect of friction on electron transfer: The two reaction coordinate case

Effect of friction on electron transfer: The two reaction coordinate case

10.1063/1.451952

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

Electron transfer is a very important reaction in many biological processes such as photosynthesis and oxidative phosphorylation. In many of these reactions, most of the interesting dynamics can be included by using two reaction coordinates: one fast (local high frequency vibration modes) and one slow (outersphere modes such as solvent polarization). We report a model to describe this problem, which uses path integral techniques to calculate electron transfer rates, and also to obtain the Fokker–Planck equations associated with this model. Different limiting cases lead to qualitatively different results such as exponential or nonexponential time decay for the donor survival probability. Conditions for the validity of the adiabatic or the nonadiabatic limits will be discussed. Application of this model to real systems is proposed, in particular for a porphyrin rigidly linked to a quinone, which is a very interesting model compound for primary events of photosynthesis. This model can also be used for other multicoordinate biological reactions such as ligand binding to heme proteins. Also, in the concluding part of Sec. III, we discuss the important limit where the fast vibronic mode is much faster than all the other nuclear modes coupled to the problem. In this limit the fast mode ‘‘renormalizes’’ the electronic matrix element, and this considerably simplifies the treatment of the problem, reducing it to coupling only to the slow modes.

Bibliography

Onuchic, J. N. (1987). Effect of friction on electron transfer: The two reaction coordinate case. The Journal of Chemical Physics, 86(7), 3925â3943.

Authors 1

José Nelson Onuchic (first)

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Dates

Type	When
Created	23 years, 1 month ago (July 26, 2002, 9:10 a.m.)
Deposited	1 year, 6 months ago (Feb. 10, 2024, 12:52 a.m.)
Indexed	1 year, 3 months ago (May 13, 2024, 9:49 a.m.)
Issued	38 years, 4 months ago (April 1, 1987)
Published	38 years, 4 months ago (April 1, 1987)
Published Print	38 years, 4 months ago (April 1, 1987)

Funders 0

None

BibTeX

@article{Onuchic_1987, title={Effect of friction on electron transfer: The two reaction coordinate case}, volume={86}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.451952}, DOI={10.1063/1.451952}, number={7}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Onuchic, José Nelson}, year={1987}, month=apr, pages={3925–3943} }

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