Spin-quenching in molecule-transition-metal-dichalcogenide heterostructure through inverse proximity effect
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arXiv
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| Auteurs principaux: | , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866909912219516928 |
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| author | Acharya, Swagata Pashov, Dimitar Lubert-Perquel, Daphne van Schilfgaarde, Mark Johnson, Justin C. |
| author_facet | Acharya, Swagata Pashov, Dimitar Lubert-Perquel, Daphne van Schilfgaarde, Mark Johnson, Justin C. |
| contents | A functional heterostructure is central to integrated circuitry in quantum photonics, optoelectronics, neuromorphic computing, spintronics, and straintronics. Recently, heterostructures combining 2D magnets and nonmagnetic transition metal dichalcogenides (TMDs) have been explored. In these, electron and hole wavefunctions are localized in 2D magnets but delocalized in TMDs. When combined, a proximity induced magnetic inter layer exciton can emerge, with energy differing by 20 to 30 meV from intra layer excitons and being two orders of magnitude darker, making it hard to detect and functionalize. Using a high fidelity ab initio many body diagrammatic approach, we show that functionality can be significantly enhanced in a transition metal molecule TMD interface. The molecular exciton exhibits charge transfer character and is extended, unlike the localized Frenkel excitation in 2D magnets. Moreover, the degree of localization and magnetic moment can be tuned by varying the molecular orientation relative to the TMD. This changes the proximity to the magnetic ion, altering screening and enabling a pathway to quench the ion's spin moment. This inverse proximity effect tunes the energies, spin states, and brightness of molecular and inter layer magnetic excitons, a mechanism absent in 2D magnet TMD systems. We also identify conditions under which the interlayer exciton becomes well separated and brighter than intra layer excitons, making it promising for protocols that probe and manipulate magnetic excitonic states. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2511_14968 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Spin-quenching in molecule-transition-metal-dichalcogenide heterostructure through inverse proximity effect Acharya, Swagata Pashov, Dimitar Lubert-Perquel, Daphne van Schilfgaarde, Mark Johnson, Justin C. Strongly Correlated Electrons Mesoscale and Nanoscale Physics Materials Science Soft Condensed Matter A functional heterostructure is central to integrated circuitry in quantum photonics, optoelectronics, neuromorphic computing, spintronics, and straintronics. Recently, heterostructures combining 2D magnets and nonmagnetic transition metal dichalcogenides (TMDs) have been explored. In these, electron and hole wavefunctions are localized in 2D magnets but delocalized in TMDs. When combined, a proximity induced magnetic inter layer exciton can emerge, with energy differing by 20 to 30 meV from intra layer excitons and being two orders of magnitude darker, making it hard to detect and functionalize. Using a high fidelity ab initio many body diagrammatic approach, we show that functionality can be significantly enhanced in a transition metal molecule TMD interface. The molecular exciton exhibits charge transfer character and is extended, unlike the localized Frenkel excitation in 2D magnets. Moreover, the degree of localization and magnetic moment can be tuned by varying the molecular orientation relative to the TMD. This changes the proximity to the magnetic ion, altering screening and enabling a pathway to quench the ion's spin moment. This inverse proximity effect tunes the energies, spin states, and brightness of molecular and inter layer magnetic excitons, a mechanism absent in 2D magnet TMD systems. We also identify conditions under which the interlayer exciton becomes well separated and brighter than intra layer excitons, making it promising for protocols that probe and manipulate magnetic excitonic states. |
| title | Spin-quenching in molecule-transition-metal-dichalcogenide heterostructure through inverse proximity effect |
| topic | Strongly Correlated Electrons Mesoscale and Nanoscale Physics Materials Science Soft Condensed Matter |
| url | https://arxiv.org/abs/2511.14968 |