A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states
Abstract
We present a very general form of electronic friction as present when a molecule with multiple orbitals hybridizes with a metal electrode. To develop this picture of friction, we embed the quantum-classical Liouville equation (QCLE) within a classical master equation (CME). Thus, this article extends our previous work analyzing the case of one electronic level, as we may now treat the case of multiple levels and many electronic molecular states. We show that, in the adiabatic limit, where electron transitions are much faster than nuclear motion, the QCLE-CME reduces to a Fokker-Planck equation, such that nuclei feel an average force as well as friction and a random force—as caused by their interaction with the metallic electrons. Finally, we show numerically and analytically that our frictional results agree with other published results calculated using non-equilibrium Green’s functions. Numerical recipes for solving this QCLE-CME will be provided in a subsequent paper.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Aug 01, 2016
- Source ID
- 10.1063/1.4959604
Entities
People
- Joseph E Subotnik
- Wenjie Dou
Organizations
- Air Force Office of Scientific Research
- University of Pennsylvania