Charge Transport through Biomolecular Wires in a Solvent: Bridging Molecular Dynamics and Model Hamiltonian Approaches

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

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.

Details

Original languageEnglish
Article number208102
Number of pages4
JournalPhysical review letters
Volume102
Issue number20
Publication statusPublished - 22 May 2009
Peer-reviewedYes

External IDs

Scopus 66049155393
WOS 000266309000070
PubMed 19519078
ORCID /0000-0001-8121-8041/work/166324460

Keywords

Keywords

  • Single dna-molecules, Tight-binding method, Hole transfer, Electrical-transport, Migration, Poly(da)-poly(dt), Poly(dg)-poly(dc), Fluctuations, Simulations, Environment

Library keywords