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

TY - JOUR

T1 - Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems

AU - Zelovich, Tamar

AU - Hansen, Thorsten

AU - Liu, Fulai

AU - Neaton, Jeffrey B.

AU - Kronik, Leeor

AU - Hod, Oded

PY - 2017

Y1 - 2017

N2 - 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. 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.

AB - 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. 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.

U2 - 10.1063/1.4976731

DO - 10.1063/1.4976731

M3 - Journal article

AN - SCOPUS:85014487439

SN - 0021-9606

VL - 146

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

IS - 9

M1 - 092331

ER -