Work

Thermoelectric Energy Conversion in Molecular Junctions Out of Equilibrium

Year: 2025

Type: article

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 timescales. In this work, we present a nonequilibrium Green’s function formalism, within the recently developed iterated generalized Kadanoff-Baym ansatz ( i 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 i 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.

Source: PRX Energy

DOI: 10.1103/rj3h-8z3g

Authors: R. Tuovinen, Y. Pavlyukh

Institutions: University of Jyväskylä, Wrocław University of Science and Technology

Language: English

Topic: Molecular Junctions and Nanostructures

Subfield: Electrical and Electronic Engineering

Field: Engineering

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: diamond

Funders: Jane ja Aatos Erkon Säätiö, China Scholarship Council