A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions

Language
en
Document Type
Article
Issue Date
2014-04-07
Issue Year
2014
Authors
Li, Bin
Wilner, Eli Y.
Thoss, Michael
Rabani, Eran
Miller, William H.
Editor
Abstract

We develop a classical mapping approach suitable to describe vibrationally coupled charge transport in molecular junctions based on the Cartesian mapping for many-electron systems [B. Li and W. H. Miller, J. Chem. Phys.137, 154107 (2012)]. To properly describe vibrational quantum effects in the transport characteristics, we introduce a simple transformation rewriting the Hamiltonian in terms of occupation numbers and use a binning function to facilitate quantization. The approach provides accurate results for the nonequilibrium Holstein model for a range of bias voltages, vibrational frequencies, and temperatures. It also captures the hallmarks of vibrational quantum effects apparent in step-like structure in the current-voltage characteristics at low temperatures as well as the phenomenon of Franck-Condon blockade.

Journal Title
The Journal of Chemical Physics
Volume
140
Issue
10
Citation
The Journal of Chemical Physics 140 104110 (2014): 07.04.2014 <http://scitation.aip.org/content/aip/journal/jcp/140/10/10.1063/1.4867789>
DOI
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