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| Main Authors: | , , , , , |
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| Format: | Preprint |
| Published: |
2022
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2301.00282 |
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| _version_ | 1866909899835834368 |
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| author | Gandus, G. Jayaraj, A. Passerone, D. Stadler, R. Luisier, M. Valli, A. |
| author_facet | Gandus, G. Jayaraj, A. Passerone, D. Stadler, R. Luisier, M. Valli, A. |
| contents | Strongly correlated physics arises from electron-electron scattering within partially filled orbitals. Organic molecules in open-shell configurations are therefore good candidates to exhibit many-body effects. We focus on electron transport in a two-terminal single-molecule junction setup, in which the molecular bridge consists of an organic radical with a molecular orbital hosting a single unpaired electron (SOMO). We perform beyond state-of-the-art numerical simulations combining an ab-initio description of the chemical environment, with quantum field-theoretical techniques that account for many-body effects. The key observation is that the SOMO resonance is prone to splitting and we identify a giant electronic scattering rate as the driving many-body mechanism, akin to that of the Mott metal-to-insulator transition. By comparing linear and cyclic radicals, we show that the spatial distribution of the SOMO and its projection on the molecular backbone have dramatic consequences for the transport properties of the junction. We argue that the phenomenon and the underlying microscopic mechanism apply to a broad family of open-shell molecular systems, and can explain puzzling experimental observations such as suppressed conductance in radical junctions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2301_00282 |
| institution | arXiv |
| publishDate | 2022 |
| record_format | arxiv |
| spellingShingle | Strongly correlated physics in organic open-shell quantum systems Gandus, G. Jayaraj, A. Passerone, D. Stadler, R. Luisier, M. Valli, A. Strongly Correlated Electrons Mesoscale and Nanoscale Physics Strongly correlated physics arises from electron-electron scattering within partially filled orbitals. Organic molecules in open-shell configurations are therefore good candidates to exhibit many-body effects. We focus on electron transport in a two-terminal single-molecule junction setup, in which the molecular bridge consists of an organic radical with a molecular orbital hosting a single unpaired electron (SOMO). We perform beyond state-of-the-art numerical simulations combining an ab-initio description of the chemical environment, with quantum field-theoretical techniques that account for many-body effects. The key observation is that the SOMO resonance is prone to splitting and we identify a giant electronic scattering rate as the driving many-body mechanism, akin to that of the Mott metal-to-insulator transition. By comparing linear and cyclic radicals, we show that the spatial distribution of the SOMO and its projection on the molecular backbone have dramatic consequences for the transport properties of the junction. We argue that the phenomenon and the underlying microscopic mechanism apply to a broad family of open-shell molecular systems, and can explain puzzling experimental observations such as suppressed conductance in radical junctions. |
| title | Strongly correlated physics in organic open-shell quantum systems |
| topic | Strongly Correlated Electrons Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2301.00282 |