Time-dependent versus static quantum transport simulations beyond linear response

Abstract

To explore whether the density-functional theory–nonequilibrium Green’s function formalism (DFT-NEGF) provides a rigorous framework for quantum transport, we carried out time-dependent density-functional-theory (TDDFT) calculations of the transient current through two realistic molecular devices, a carbon chain and a benzenediol molecule between two aluminum electrodes. The TDDFT simulations for the steady-state current exactly reproduce the results of fully self-consistent DFT-NEGF calculations even beyond linear response. In contrast, sizable differences are found with respect to an equilibrium, non-self-consistent treatment, which are related here to differences in the Kohn-Sham and fully interacting susceptibilities of the device region. Moreover, earlier analytical conjectures on the equivalence of static and time-dependent approaches in the low-bias regime are confirmed with high numerical precision.