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Title: Modulation of electron transfer kinetics by protein conformational fluctuations during early-stage photosynthesis

Abstract

The kinetics of electron transfer during the early stages of the photosynthetic reaction cycle has recently been shown in transient absorption experiments carried out by Wang et al. [Science 316, 747 (2007)] to be strongly influenced by fluctuations in the conformation of the surrounding protein. A model of electron transfer rates in polar solvents developed by Sumi and Marcus using a reaction-diffusion formalism [J. Chem. Phys. 84, 4894 (1986)] was found to be successful in fitting the experimental absorption curves over a roughly 200 ps time interval. The fits were achieved using an empirically determined time-dependent function that described protein conformational relaxation. In the present paper, a microscopic model of this function is suggested, and it is shown that the function can be identified with the dynamic autocorrelation function of intersegment distance fluctuations that occur in a harmonic potential of mean force under the action of fractional Gaussian noise.

Authors:
;  [1]
  1. Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012 (India)
Publication Date:
OSTI Identifier:
21024304
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 127; Journal Issue: 14; Other Information: DOI: 10.1063/1.2783845; (c) 2007 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION; BIOPHYSICS; ELECTRON TRANSFER; HARMONIC POTENTIAL; MOLECULAR STRUCTURE; PHOTOSYNTHESIS; PROTEINS; REACTION KINETICS; TIME DEPENDENCE

Citation Formats

Chaudhury, Srabanti, and Cherayil, Binny J. Modulation of electron transfer kinetics by protein conformational fluctuations during early-stage photosynthesis. United States: N. p., 2007. Web. doi:10.1063/1.2783845.
Chaudhury, Srabanti, & Cherayil, Binny J. Modulation of electron transfer kinetics by protein conformational fluctuations during early-stage photosynthesis. United States. https://doi.org/10.1063/1.2783845
Chaudhury, Srabanti, and Cherayil, Binny J. 2007. "Modulation of electron transfer kinetics by protein conformational fluctuations during early-stage photosynthesis". United States. https://doi.org/10.1063/1.2783845.
@article{osti_21024304,
title = {Modulation of electron transfer kinetics by protein conformational fluctuations during early-stage photosynthesis},
author = {Chaudhury, Srabanti and Cherayil, Binny J},
abstractNote = {The kinetics of electron transfer during the early stages of the photosynthetic reaction cycle has recently been shown in transient absorption experiments carried out by Wang et al. [Science 316, 747 (2007)] to be strongly influenced by fluctuations in the conformation of the surrounding protein. A model of electron transfer rates in polar solvents developed by Sumi and Marcus using a reaction-diffusion formalism [J. Chem. Phys. 84, 4894 (1986)] was found to be successful in fitting the experimental absorption curves over a roughly 200 ps time interval. The fits were achieved using an empirically determined time-dependent function that described protein conformational relaxation. In the present paper, a microscopic model of this function is suggested, and it is shown that the function can be identified with the dynamic autocorrelation function of intersegment distance fluctuations that occur in a harmonic potential of mean force under the action of fractional Gaussian noise.},
doi = {10.1063/1.2783845},
url = {https://www.osti.gov/biblio/21024304}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 14,
volume = 127,
place = {United States},
year = {Sun Oct 14 00:00:00 EDT 2007},
month = {Sun Oct 14 00:00:00 EDT 2007}
}