2025/06/06 by Tuovinen, R., Pavlyukh, Y. · 3 citations
#Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Quantum Physics (quant-ph)
paper · doi:10.48550/arxiv.2506.06129
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 (iGKBA), 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 iGKBA 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.