Parameter Free Driven Liouville-von Neumann Approach for Time-Dependent Electronic Transport Simulations in Open Quantum Systems

Parameter Free Driven Liouville-von Neumann Approach for Time-Dependent Electronic Transport Simulations in Open Quantum Systems Parameter Free Driven Liouville-von Neumann Approach for Time-Dependent Electronic Transport Simulations in Open Quantum Systems

Tamar Zelovich¹, Thorsten Hansen², Zhen-Fei Liu^3,4,5, Jeffrey B. Neaton^3,4,5,6, Leeor Kronik⁷, and Oded Hod¹

1) Department of Physical Chemistry, School of Chemistry, The Raymond and Beverly Sackler Faculty of Exact Sciences and The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv 6997801, Israel
2) Department of Chemistry, Copenhagen University, Universitetsparken 5, DK-2100, Copenhagen, Denmark
3) Department of Physics, University of California, Berkeley, Berkeley, California 94720-7300, USA
4) Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
5) Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
6) Kavli Energy NanoSciences Institute at Berkeley, Berkeley, California 94720, USA
7) Department of Materials and Interfaces, Weizmann Institute of Science, Rehovoth 76100, Israel

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.

	Download the paper in PDF format
	Download supporting information in PDF format