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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4976731· OSTI ID:1379766
 [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
+ Show Author Affiliations

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1379766
Alternate ID(s):
OSTI ID: 1349534
Journal Information:
Journal of Chemical Physics, Vol. 146, Issue 9; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 37 works
Citation information provided by
Web of Science

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Cited By (11)

Simulation of Many-Electron Systems That Exchange Matter with the Environment: Simulation of Many-Electron Systems That Exchange Matter with the Environment journal August 2018
Preface: Special Topic on Frontiers in Molecular Scale Electronics journal March 2017
Communication: Relaxation-limited electronic currents in extended reservoir simulations journal October 2017
Communication: Master equations for electron transport: The limits of the Markovian limit journal October 2017
Emergence of Landauer transport from quantum dynamics: A model Hamiltonian approach journal April 2018
Dynamical simulation of electron transfer processes in self-assembled monolayers at metal surfaces using a density matrix approach journal March 2018
Non-equilibrium Green’s function transport theory for molecular junctions with general molecule-lead coupling and temperatures journal December 2018
Communication: Gibbs phenomenon and the emergence of the steady-state in quantum transport journal December 2018
Lead geometry and transport statistics in molecular junctions journal June 2019
Multiscale approach to electron transport dynamics journal August 2019
Preface: Special Topic on Frontiers in Molecular Scale Electronics text January 2017

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