title: Charge transport through biomolecular wires in a solvent: bridging molecular dynamics and model Hamiltonian approaches.
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.
authors.affiliation: Institute for Materials Science and Max Bergmann Center of Biomaterials, Dresden University of Technology, D-01062, Dresden, Germany.
authors.forename: R
authors.initials: R
authors.lastname: Gutiérrez
authors.forename: R A
authors.initials: RA
authors.lastname: Caetano
authors.forename: B P
authors.initials: BP
authors.lastname: Woiczikowski
authors.forename: T
authors.initials: T
authors.lastname: Kubar
authors.forename: M
authors.initials: M
authors.lastname: Elstner
authors.forename: G
authors.initials: G
authors.lastname: Cuniberti
mesh_terms: D000465:Algorithms; D003198:Computer Simulation; D004247:DNA / Q000737:chemistry*; D004560:Electricity; D008956:Models, Chemical; D009690:Nucleic Acid Conformation; D011789:Quantum Theory; D012997:Solvents / Q000737:chemistry*
chemical_list: D012997:Solvents; D004247:DNA