A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions
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.
- Authors:
-
- Department of Chemistry and Kenneth S. Pitzer Center for Theoretical Chemistry, University of California, and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
- School of Physics and Astronomy, The Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv 69978 (Israel)
- Institute for Theoretical Physics and Interdisciplinary Center for Molecular Materials, Friedrich-Alexander-Universität Erlangen-Nürnberg, Staudtstr. 7/B2, 91058 Erlangen (Germany)
- School of Chemistry, The Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv 69978 (Israel)
- Publication Date:
- OSTI Identifier:
- 22253451
- Resource Type:
- Journal Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 10; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; CHARGE TRANSPORT; ELECTRIC POTENTIAL; HAMILTONIANS; QUANTIZATION
Citation Formats
Li, Bin, Miller, William H., Wilner, Eli Y., Thoss, Michael, and Rabani, Eran. A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions. United States: N. p., 2014.
Web. doi:10.1063/1.4867789.
Li, Bin, Miller, William H., Wilner, Eli Y., Thoss, Michael, & Rabani, Eran. A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions. United States. https://doi.org/10.1063/1.4867789
Li, Bin, Miller, William H., Wilner, Eli Y., Thoss, Michael, and Rabani, Eran. 2014.
"A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions". United States. https://doi.org/10.1063/1.4867789.
@article{osti_22253451,
title = {A quasi-classical mapping approach to vibrationally coupled electron transport in molecular junctions},
author = {Li, Bin and Miller, William H. and Wilner, Eli Y. and Thoss, Michael and Rabani, Eran},
abstractNote = {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.},
doi = {10.1063/1.4867789},
url = {https://www.osti.gov/biblio/22253451},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 10,
volume = 140,
place = {United States},
year = {Fri Mar 14 00:00:00 EDT 2014},
month = {Fri Mar 14 00:00:00 EDT 2014}
}