Efficient calculation of charge-transfer matrix elements for hole transfer in DNA.
We present a new computational strategy to evaluate the charge-transfer (CT) parameters for hole transfer in DNA. On the basis of a fragment-orbital approach, site energies and coupling integrals for a coarse-grained tight-binding description of the electronic structure of DNA are rapidly calculated using the approximative density functional method SCC-DFTB. The methodology is validated by extensive test calculations in comparison with DFT and ab initio reference data, demonstrating its high accuracy at low computational cost. Environmental effects are captured using a quantum mechanics-molecular mechanics (QM/MM) coupling scheme, and dynamical effects are included by evaluating the CT parameters along classical molecular dynamics simulations. This combined methodology allows for a realistic treatment of CT processes in DNA.
Department of Physical and Theoretical Chemistry, Technische Universität Braunschweig, Braunschweig, Germany.
Tomás
T
Kubar
P Benjamin
PB
Woiczikowski
Gianaurelio
G
Cuniberti
Marcus
M
Elstner
D003198:Computer Simulation; D004247:DNA / Q000737:chemistry*; D007477:Ions / Q000737:chemistry; D008958:Models, Molecular; D009690:Nucleic Acid Conformation
D007477:Ions; D004247:DNA