Multimode vibrational effects in single-molecule conductance: A nonequilibrium Green’s function approach

The role of multimode vibrational dynamics in electron transport through single-molecule junctions is investigated. The study is based on a generic model, which describes charge transport through a single molecule that is attached to metal leads. To address vibrationally coupled electron transport, we employ a nonequilibrium Green's function approach that extends a method recently proposed by Galperin et al. [Phys. Rev. B 73, 045314 (2006)] to multiple vibrational modes. The methodology is applied to two systems: a generic model with two vibrational degrees of freedom and benzenedibutanethiolate covalently bound to gold electrodes. The results show that the coupling to multiple vibrational modes can have a significant effect on the conductance of a molecular junction. In particular, we demonstrate the effect of the electronically induced coupling between different vibrational modes and study nonequilibrium vibrational effects by calculating the current-induced excitation of the vibrational modes.