A broadened classical master equation approach for treating electron-nuclear coupling in non-equilibrium transport
Abstract
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Nov 20, 2017
- Source ID
- 10.1063/1.4992784
Entities
People
- Christian Schinabeck
- Joseph E Subotnik
- Michael Thoss
- Wenjie Dou
Organizations
- Air Force Office of Scientific Research
- Friedrich-Alexander-Universität Erlangen-Nürnberg
- German Research Foundation
- University of Freiburg
- University of Pennsylvania