Thermoelectric energy conversion in molecular junctions out of equilibrium
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arXiv
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| Hauptverfasser: | , |
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| Format: | Preprint |
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2025
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| author | Tuovinen, R. Pavlyukh, Y. |
| author_facet | Tuovinen, R. Pavlyukh, Y. |
| contents | 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 ($i$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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2506_06129 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Thermoelectric energy conversion in molecular junctions out of equilibrium Tuovinen, R. Pavlyukh, Y. Mesoscale and Nanoscale Physics Chemical Physics Quantum Physics 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 ($i$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. |
| title | Thermoelectric energy conversion in molecular junctions out of equilibrium |
| topic | Mesoscale and Nanoscale Physics Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2506.06129 |