Lawrence Berkeley National Laboratory
Parameter-free driven Liouville-von Neumann approach for time-dependent electronic transport simulations in open quantum systems
- Author(s): Zelovich, T
- Hansen, T
- Liu, ZF
- Neaton, JB
- Kronik, L
- Hod, O
- et al.
Published Web Locationhttps://doi.org/10.1063/1.4976731
© 2017 Author(s). 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.