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Statistics and kinetics of single-molecule electron transfer dynamics in complex environments: a simulation model

Luciana C Paula¹, Jin Wang, Vitor B P Leite

¹Departamento de Física, Instituto de Biociências Letras e Ciências Exatas, Universidade Estadual Paulista, São José do Rio Preto, São Paulo 15054-000, Brazil.

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Summary

Environmental dynamics significantly impact electron transfer reactions. Analyzing first-passage time statistics reveals complex kinetics, with temperature and observation window size being crucial factors.

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Area of Science:

Physical Chemistry
Chemical Physics
Biophysical Chemistry

Background:

Environmental dynamics in complex systems like biomolecules and polar solvents are critical for electron transfer (ET) reactions.
The kinetics of ET reactions are governed by complex, multidimensional energy landscapes.

Purpose of the Study:

To reveal the dynamics of ET reactions controlled by their environments.
To quantify the statistics of first-passage time (FPT) and associated ratios under realistic experimental conditions.

Main Methods:

Analysis of mean and high-order statistics of FPT.
Consideration of finite observation time windows in experimental setups.

Main Results:

At high temperatures, exponential kinetics and multiple kinetic paths are observed.
At and below intermediate temperatures, nonexponential kinetics emerge, indicating local traps on the energy landscape.
Very low temperatures also exhibit nonexponential kinetics.

Conclusions:

The size of the observation time window is critical for accurately characterizing ET kinetics.
Sufficiently large observation windows are necessary to capture rare statistical fluctuations and define characteristic times.