Agarwalla Bijay Kumar, Segal Dvira
Chemical Physics Theory Group, Department of Chemistry, and Centre for Quantum Information and Quantum Control, University of Toronto, 80 Saint George St., Toronto, Ontario M5S 3H6, Canada.
J Chem Phys. 2016 Feb 21;144(7):074102. doi: 10.1063/1.4941582.
We present consistent results for molecular conduction using two central-complementary approaches: the non-equilibrium Green's function technique and the quantum master equation method. Our model describes electronic conduction in a donor-acceptor junction in which electron transfer is coupled to nuclear motion, modeled by a harmonic vibrational mode. This primary mode is further coupled to secondary phonon modes, a thermal bath. Assuming weak electron-phonon coupling but an arbitrary large molecule-metal hybridization, we compute several non-equilibrium transport quantities: the mean phonon number of the primary mode, charge current statistics. We further present scaling relations for the cumulants valid in the large voltage regime. Our analysis illustrates that the non-equilibrium Green's function technique and the quantum master equation method can be worked out consistently, when taking into account corresponding scattering processes.
非平衡格林函数技术和量子主方程方法。我们的模型描述了供体-受体结中的电子传导,其中电子转移与核运动耦合,核运动由简谐振动模式建模。这个主要模式进一步与次级声子模式(一个热库)耦合。假设电子-声子耦合较弱但分子-金属杂化任意大,我们计算了几个非平衡输运量:主要模式的平均声子数、电荷电流统计量。我们还给出了在大电压 regime 中有效的累积量的标度关系。我们的分析表明,当考虑相应的散射过程时,非平衡格林函数技术和量子主方程方法可以一致地得出结果。