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Title: 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.

Authors:
;  [1]
  1. Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104 (United States)
Publication Date:
OSTI Identifier:
22679016
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 145; Journal Issue: 5; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BOLTZMANN-VLASOV EQUATION; ELECTRONIC STRUCTURE; EXPERIMENTAL DATA; FOKKER-PLANCK EQUATION

Citation Formats

Dou, Wenjie, and Subotnik, Joseph E. A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states. United States: N. p., 2016. Web. doi:10.1063/1.4959604.
Dou, Wenjie, & Subotnik, Joseph E. A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states. United States. doi:10.1063/1.4959604.
Dou, Wenjie, and Subotnik, Joseph E. Sun . "A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states". United States. doi:10.1063/1.4959604.
@article{osti_22679016,
title = {A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states},
author = {Dou, Wenjie and Subotnik, Joseph E.},
abstractNote = {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.},
doi = {10.1063/1.4959604},
journal = {Journal of Chemical Physics},
number = 5,
volume = 145,
place = {United States},
year = {Sun Aug 07 00:00:00 EDT 2016},
month = {Sun Aug 07 00:00:00 EDT 2016}
}