Static and dynamic aspects of DNA charge transfer: a theoretical perspective

Phys Chem Chem Phys. 2005 Dec 21;7(24):4039-50. doi: 10.1039/b507454a. Epub 2005 Sep 1.

Abstract

In this work, we approach the impact of dynamic and static disorder on DNA charge transfer from a theoretical and numerical perspective. Disordered or defect geometries are either realized via molecular dynamics simulations using a classical force field or by experimentally determined DNA bulge structures. We apply a chemically specific, atomically resolved extended Su-Schrieffer-Heeger model to compute the energy parameters relevant to DNA charge transfer. For both models studied here, the effective donor-acceptor couplings--and hence the charge transfer rates--significantly depend upon the geometry. Dynamic disorder leads to a correlation time in this quantity of the order of 30 fs, and the transfer rates universally exhibit a broad, yet well-defined, exponential distribution. For DNA bulges, the angle characterizing the defect controls the charge transfer efficiency. The results are discussed and extensively compared to experimental findings and other calculations.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Base Sequence
  • DNA / chemistry*
  • Guanine / chemistry
  • Kinetics
  • Models, Chemical*
  • Molecular Sequence Data
  • Oxidation-Reduction
  • Static Electricity

Substances

  • Guanine
  • DNA