Hole Conductivity in Heterogeneous DNA Fragments

TL;DR

This paper models hole migration in heterogeneous DNA using a quantum statistical approach, revealing the environment's polarization as crucial and aligning well with experimental data on transfer rates and temperature effects.

Contribution

It introduces a new theoretical framework based on the Kubo formula and Bogoliubov hierarchy to analyze charge transfer in DNA, emphasizing environment polarization effects.

Findings

Environment polarization significantly influences hole transport.

Transfer rates align with experimental measurements.

Hopping mechanism dominates at physiological temperature.

Abstract

The characteristics of cation radical (hole) migration in heterogeneous DNA were investigated on the basis of Kubo formula, in which correlation functions were obtained from solutions of systems of Bogoliubov hierarchy. The cutting of Bogoliubov hierarchy was carried out by excepting correlations of the third and higher order. The obtained system of non-linear differential equations was investigated both analytically and numerically. The environment polarization, caused by interaction of holes with base pairs vibrations, was shown to play the key role in transport processes. The energy of the interaction can ten-fold exceed vibration energy. The transfer rate between adjacent DNA bases in one-dimensional case was shown to be almost independent of the nature and behavior of more distant pairs. The charge probability amplitude oscillates in the picosecond timescale. Nonetheless, the rates of hole transfer, obtained by averaging over these oscillations, turned out to be very close to the experimental data. The calculated dependence of the hole transfer rate between two guanine bases on the number of intervening adenine bases was also in good agreement with the experimental data. Besides, the temperature dependence of the transfer rate was investigated. Hopping mechanism was shown to make the main contribution to the hole transport process at 300 K.