Charge transport through biomolecular wires in a solvent: bridging molecular dynamics and model Hamiltonian approaches.
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.
Gutiérrez
R
R
Institute for Materials Science and Max Bergmann Center of Biomaterials, Dresden University of Technology, D-01062, Dresden, Germany.
Caetano
R A
RA
Woiczikowski
B P
BP
Kubar
T
T
Elstner
M
M
Cuniberti
G
G
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*
D012997:Solvents; D004247:DNA