Charge transport through biomolecular wires in a solvent: bridging molecular dynamics and model Hamiltonian approaches

Phys Rev Lett. 2009 May 22;102(20):208102. doi: 10.1103/PhysRevLett.102.208102. Epub 2009 May 22.

Abstract

We present a hybrid method based on a combination of classical molecular dynamics simulations, quantum-chemical calculations, and a model Hamiltonian approach to describe charge transport through biomolecular wires with variable lengths in presence of a solvent. The core of our approach consists in a mapping of the biomolecular electronic structure, as obtained from density-functional based tight-binding calculations of molecular structures along molecular dynamics trajectories, onto a low-dimensional model Hamiltonian including the coupling to a dissipative bosonic environment. The latter encodes fluctuation effects arising from the solvent and from the molecular conformational dynamics. We apply this approach to the case of pG-pC and pA-pT DNA oligomers as paradigmatic cases and show that the DNA conformational fluctuations are essential in determining and supporting charge transport.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Algorithms
  • Computer Simulation
  • DNA / chemistry*
  • Electricity*
  • Models, Chemical*
  • Nucleic Acid Conformation
  • Quantum Theory
  • Solvents / chemistry*

Substances

  • Solvents
  • DNA