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Title: Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems

A parameter-free version of the recently developed driven Liouville-von Neumann equation [T. Zelovich et al., J. Chem. Theory Comput. 10(8), 2927-2941 (2014)] for electronic transport calculations in molecular junctions is presented. The single driving rate, appearing as a fitting parameter in the original methodology, is replaced by a set of state-dependent broadening factors applied to the different single-particle lead levels. These broadening factors are extracted explicitly from the self-energy of the corresponding electronic reservoir and are fully transferable to any junction incorporating the same lead model. Furthermore, the performance of the method is demonstrated via tight-binding and extended Hückel calculations of simple junction models. Our analytic considerations and numerical results indicate that the developed methodology constitutes a rigorous framework for the design of "black-box" algorithms to simulate electron dynamics in open quantum systems out of equilibrium.
Authors:
 [1] ; ORCiD logo [2] ;  [3] ;  [4] ;  [5] ;  [1]
  1. Tel Aviv Univ., Ramat Aviv (Israel). The Raymond and Beverly Sackler Faculty of Exact Sciences, The Sackler Center for Computation Molecular and Materials Science
  2. Copenhagen Univ. (Denmark). Dept. of Chemistry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division, Molecular Foundry
  4. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division, Molecular Foundry; Kavli Energy NanoSciences Inst., Berkeley, CA (United States)
  5. Weizmann Inst. of Science, Rehovot (Israel). Dept. of Materials and Interfaces
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS
OSTI Identifier:
1379766
Alternate Identifier(s):
OSTI ID: 1349534

Zelovich, Tamar, Hansen, Thorsten, Liu, Zhen-Fei, Neaton, Jeffrey B., Kronik, Leeor, and Hod, Oded. Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems. United States: N. p., Web. doi:10.1063/1.4976731.
Zelovich, Tamar, Hansen, Thorsten, Liu, Zhen-Fei, Neaton, Jeffrey B., Kronik, Leeor, & Hod, Oded. Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems. United States. doi:10.1063/1.4976731.
Zelovich, Tamar, Hansen, Thorsten, Liu, Zhen-Fei, Neaton, Jeffrey B., Kronik, Leeor, and Hod, Oded. 2017. "Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems". United States. doi:10.1063/1.4976731. https://www.osti.gov/servlets/purl/1379766.
@article{osti_1379766,
title = {Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems},
author = {Zelovich, Tamar and Hansen, Thorsten and Liu, Zhen-Fei and Neaton, Jeffrey B. and Kronik, Leeor and Hod, Oded},
abstractNote = {A parameter-free version of the recently developed driven Liouville-von Neumann equation [T. Zelovich et al., J. Chem. Theory Comput. 10(8), 2927-2941 (2014)] for electronic transport calculations in molecular junctions is presented. The single driving rate, appearing as a fitting parameter in the original methodology, is replaced by a set of state-dependent broadening factors applied to the different single-particle lead levels. These broadening factors are extracted explicitly from the self-energy of the corresponding electronic reservoir and are fully transferable to any junction incorporating the same lead model. Furthermore, the performance of the method is demonstrated via tight-binding and extended Hückel calculations of simple junction models. Our analytic considerations and numerical results indicate that the developed methodology constitutes a rigorous framework for the design of "black-box" algorithms to simulate electron dynamics in open quantum systems out of equilibrium.},
doi = {10.1063/1.4976731},
journal = {Journal of Chemical Physics},
number = 9,
volume = 146,
place = {United States},
year = {2017},
month = {3}
}