Thermoelectric energy conversion in molecular junctions out of equilibrium
arXiv:2506.06129 · doi:10.1103/rj3h-8z3g
Abstract
Understanding time-resolved quantum transport is crucial for developing next-generation quantum technologies, particularly in nano- and molecular junctions subjected to time-dependent perturbations. Traditional steady-state approaches to quantum transport are not designed to capture the transient dynamics necessary for controlling electronic behavior at ultrafast time scales. In this work, we present a non-equilibrium Green's function formalism, within the recently-developed iterated generalized Kadanoff-Baym ansatz (GKBA), to study thermoelectric quantum transport beyond the wide-band limit approximation (WBLA). We employ the Meir-Wingreen formula for both charge and energy currents and analyze the transition from Lorentzian line-width functions to the WBLA, identifying unphysical divergences in the latter. Our results highlight the importance of finite-bandwidth effects and demonstrate the efficiency of the GKBA approach in modeling time-resolved thermoelectric transport, also providing benchmark comparisons against the full Kadanoff-Baym theory. We exemplify the developed theory in the calculation of time-resolved thermopower and thermoelectric energy conversion efficiency in a cyclobutadiene molecular junction.
Main: 15 pages, 9 figures. Supplemental Material: 5 pages, 2 figures
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