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Understanding Short-Range Electron-Transfer Dynamics in Proteins.

Yangyi Lu1, Dongping Zhong1,2

  • 1Department of Physics, Department of Chemistry and Biochemistry, Programs of Biophysics, Chemical Physics, and Biochemistry , The Ohio State University , Columbus , Ohio 43210 , United States.

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Ultrafast electron transfer (ET) in biological systems is complex. Our study reveals that environmental fluctuations significantly impact ET dynamics, even with constant energy factors, offering new insights into protein ET mechanisms.

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Area of Science:

  • Biophysics
  • Physical Chemistry
  • Biochemistry

Background:

  • Short-range electron-transfer (ET) reactions in biological systems are ultrafast.
  • These reactions often exhibit nonexponential behaviors and rates comparable to environmental fluctuations.

Purpose of the Study:

  • To understand the nonequilibrium ET dynamics in biological systems.
  • To analyze the influence of environmental fluctuations on ET reaction rates and behaviors.

Main Methods:

  • Detailed theoretical analyses using the Sumi-Marcus model.
  • Application of the model to an ultrafast ET process in DNA repair by (6-4) photolyase.

Main Results:

  • ET dynamics are primarily governed by the relative timescales of the ET reaction and surrounding motions.
  • Diverse environmental fluctuations can lead to varied apparent ET dynamics, irrespective of constant driving force (ΔG°) and reorganization energy (λ).
  • Inner (λi) and outer (λo) reorganization energies and free energy (ΔG°) were determined for (6-4) photolyase mutants.

Conclusions:

  • Environmental fluctuations play a crucial role in shaping observed ET dynamics.
  • The study provides mechanical insights into ultrafast short-range ET reactions within proteins.
  • Understanding these dynamics is key for biological processes like DNA repair.