title: Solvent effects on charge spatial extent in DNA and implications for transfer.
abstract: To clarify the role played by water in facilitating long-range DNA charge transport, carefully designed, state-of-the-art, self-interaction corrected density-functional quantum mechanical and molecular mechanical (SIC-QM/MM) simulations are performed for the first time on two ionized adenine:thymine bridge models in explicit water solvent at finite temperature. For random solvent configurations, the charge is partially delocalized. However, a charge localization on different, well-separated adenines can be induced and is correlated with a restructuring of their first solvation shells. Thus, the importance of water in the mechanism of long-range charge transport is explicitly demonstrated, and the microscopic conditions for a charge localization are revealed.
authors.affiliation: Computational Science, Department of Chemistry and Applied Biosciences, ETH Zurich, US I Campus, Via Giuseppe Buffi 13, CH-6900 Lugano, Switzerland. ymantz@phys.chem.ethz.ch
authors.forename: Yves A
authors.initials: YA
authors.lastname: Mantz
authors.forename: Francesco Luigi
authors.initials: FL
authors.lastname: Gervasio
authors.forename: Teodoro
authors.initials: T
authors.lastname: Laino
authors.forename: Michele
authors.initials: M
authors.lastname: Parrinello
mesh_terms: D004247:DNA; D008958:Models, Molecular; D011789:Quantum Theory; D012997:Solvents; D013941:Thymine; D014867:Water
chemical_list: D012997:Solvents; D014867:Water; D004247:DNA; D013941:Thymine