A broadened classical master equation approach for treating electron-nuclear coupling in non-equilibrium transport

作者：Dou Wenjie^*; Schinabeck Christian; Thoss Michael; Subotnik Joseph E

来源：Journal of Chemical Physics, 2018, 148(10): 102317.

DOI：10.1063/1.4992784

We extend the broadened classical master equation (bCME) approach [W. Dou and J. E. Subotnik, J. Chem. Phys. 144, 024116 (2016)] to the case of two electrodes, such that we may now calculate non-equilibrium transport properties when molecules come near metal surfaces and there is both strong electron-nuclear and strong metal-molecule coupling. By comparing against a numerically exact solution, we show that the bCME usually works very well, provided that the temperature is high enough that a classical treatment of nuclear motion is valid. Finally, in the low temperature (quantum) regime, we suggest a means to incorporate broadening effects in the quantum master equation (QME). This bQME works well for fairly low temperatures. Published by AIP Publishing.

• 出版日期2018-3-14