title: Charge-transfer excited states in aqueous DNA: Insights from many-body Green's function theory.
abstract: Charge-transfer (CT) excited states play an important role in the excited-state dynamics of DNA in aqueous solution. However, there is still much controversy on their energies. By ab initio many-body Green's function theory, together with classical molecular dynamics simulations, we confirm the existence of CT states at the lower energy side of the optical absorption maximum in aqueous DNA as observed in experiments. We find that the hydration shell can exert strong effects (∼1  eV) on both the electronic structure and CT states of DNA molecules through dipole electric fields. In this case, the solvent cannot be simply regarded as a macroscopic screening medium as usual. The influence of base stacking and base pairing on the CT states is also discussed.
authors.affiliation: School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, People's Republic of China.
authors.forename: Huabing
authors.initials: H
authors.lastname: Yin
authors.affiliation: School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, People's Republic of China.
authors.forename: Yuchen
authors.initials: Y
authors.lastname: Ma
authors.affiliation: School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, People's Republic of China.
authors.forename: Jinglin
authors.initials: J
authors.lastname: Mu
authors.affiliation: School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, People's Republic of China.
authors.forename: Chengbu
authors.initials: C
authors.lastname: Liu
authors.affiliation: Institut für Festkörpertheorie, Universität Münster, 48149 Münster, Germany.
authors.forename: Michael
authors.initials: M
authors.lastname: Rohlfing
mesh_terms: D004247:DNA / Q000737:chemistry*; D008956:Models, Chemical; D008958:Models, Molecular; D056004:Molecular Dynamics Simulation; D055095:Optics and Photonics / Q000379:methods; D013057:Spectrum Analysis; D014867:Water / Q000737:chemistry*
chemical_list: D014867:Water; D004247:DNA