Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits
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arXiv
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| Autori principali: | , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| _version_ | 1866929375827460096 |
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| author | Poh, Yong Rui Morozov, Dmitry Kazmierczak, Nathanael P. Hadt, Ryan G. Groenhof, Gerrit Yuen-Zhou, Joel |
| author_facet | Poh, Yong Rui Morozov, Dmitry Kazmierczak, Nathanael P. Hadt, Ryan G. Groenhof, Gerrit Yuen-Zhou, Joel |
| contents | High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. Optical addressability of molecular electron spins has also been proposed in first-row transition metal complexes via optically-detected magnetic resonance (ODMR) mechanisms analogous to the diamond-NV colour centre. However, significantly less progress has been made on the front of metal-free molecules, which can deliver lower costs and milder environmental impacts. At present, most luminescent open-shell organic molecules are $π$-diradicals, but such systems often suffer from poor ground-state open-shell characters necessary to realise a stable ground-state molecular qubit. In this work, we use alternancy symmetry to selectively minimise radical-radical interactions in the ground state, generating $π$-systems with high diradical characters. We call them m-dimers, referencing the need to covalently link two benzylic radicals at their meta carbon atoms for the desired symmetry. Through a detailed electronic structure analysis, we find that the excited states of alternant hydrocarbon m-diradicals contain important symmetries that can be used to construct ODMR mechanisms leading to ground-state spin polarisation. The molecular parameters are set in the context of a tris(2,4,6-trichlorophenyl)methyl (TTM) radical dimer covalently tethered at the meta position, demonstrating the feasibility of alternant m-diradicals as molecular colour centres. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2403_09102 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits Poh, Yong Rui Morozov, Dmitry Kazmierczak, Nathanael P. Hadt, Ryan G. Groenhof, Gerrit Yuen-Zhou, Joel Chemical Physics Materials Science Quantum Physics High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. Optical addressability of molecular electron spins has also been proposed in first-row transition metal complexes via optically-detected magnetic resonance (ODMR) mechanisms analogous to the diamond-NV colour centre. However, significantly less progress has been made on the front of metal-free molecules, which can deliver lower costs and milder environmental impacts. At present, most luminescent open-shell organic molecules are $π$-diradicals, but such systems often suffer from poor ground-state open-shell characters necessary to realise a stable ground-state molecular qubit. In this work, we use alternancy symmetry to selectively minimise radical-radical interactions in the ground state, generating $π$-systems with high diradical characters. We call them m-dimers, referencing the need to covalently link two benzylic radicals at their meta carbon atoms for the desired symmetry. Through a detailed electronic structure analysis, we find that the excited states of alternant hydrocarbon m-diradicals contain important symmetries that can be used to construct ODMR mechanisms leading to ground-state spin polarisation. The molecular parameters are set in the context of a tris(2,4,6-trichlorophenyl)methyl (TTM) radical dimer covalently tethered at the meta position, demonstrating the feasibility of alternant m-diradicals as molecular colour centres. |
| title | Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits |
| topic | Chemical Physics Materials Science Quantum Physics |
| url | https://arxiv.org/abs/2403.09102 |