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Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence
Molecular entities with doublet or triplet ground states find increasing interest as potential molecular quantum bits (qubits). Complexes with higher multiplicity might even function as qudits and serve to encode further quantum bits. Vanadium(II) ions in octahedral ligand fields with quartet ground...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10107508/ https://www.ncbi.nlm.nih.gov/pubmed/36345821 http://dx.doi.org/10.1002/chem.202202898 |
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author | Dorn, Matthias Hunger, David Förster, Christoph Naumann, Robert van Slageren, Joris Heinze, Katja |
author_facet | Dorn, Matthias Hunger, David Förster, Christoph Naumann, Robert van Slageren, Joris Heinze, Katja |
author_sort | Dorn, Matthias |
collection | PubMed |
description | Molecular entities with doublet or triplet ground states find increasing interest as potential molecular quantum bits (qubits). Complexes with higher multiplicity might even function as qudits and serve to encode further quantum bits. Vanadium(II) ions in octahedral ligand fields with quartet ground states and small zero‐field splittings qualify as qubits with optical read out thanks to potentially luminescent spin‐flip states. We identified two V(2+) complexes [V(ddpd)(2)](2+) with the strong field ligand N,N’‐dimethyl‐N,N’‐dipyridine‐2‐yl‐pyridine‐2,6‐diamine (ddpd) in two isomeric forms (cis‐fac and mer) as suitable candidates. The energy gaps between the two lowest Kramers doublets amount to 0.2 and 0.5 cm(−1) allowing pulsed EPR experiments at conventional Q‐band frequencies (35 GHz). Both isomers possess spin‐lattice relaxation times T (1) of around 300 μs and a phase memory time T (M) of around 1 μs at 5 K. Furthermore, the mer isomer displays slow magnetic relaxation in an applied field of 400 mT. While the vanadium(III) complexes [V(ddpd)(2)](3+) are emissive in the near‐IR‐II region, the [V(ddpd)(2)](2+) complexes are non‐luminescent due to metal‐to‐ligand charge transfer admixture to the spin‐flip states. |
format | Online Article Text |
id | pubmed-10107508 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-101075082023-04-18 Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence Dorn, Matthias Hunger, David Förster, Christoph Naumann, Robert van Slageren, Joris Heinze, Katja Chemistry Research Articles Molecular entities with doublet or triplet ground states find increasing interest as potential molecular quantum bits (qubits). Complexes with higher multiplicity might even function as qudits and serve to encode further quantum bits. Vanadium(II) ions in octahedral ligand fields with quartet ground states and small zero‐field splittings qualify as qubits with optical read out thanks to potentially luminescent spin‐flip states. We identified two V(2+) complexes [V(ddpd)(2)](2+) with the strong field ligand N,N’‐dimethyl‐N,N’‐dipyridine‐2‐yl‐pyridine‐2,6‐diamine (ddpd) in two isomeric forms (cis‐fac and mer) as suitable candidates. The energy gaps between the two lowest Kramers doublets amount to 0.2 and 0.5 cm(−1) allowing pulsed EPR experiments at conventional Q‐band frequencies (35 GHz). Both isomers possess spin‐lattice relaxation times T (1) of around 300 μs and a phase memory time T (M) of around 1 μs at 5 K. Furthermore, the mer isomer displays slow magnetic relaxation in an applied field of 400 mT. While the vanadium(III) complexes [V(ddpd)(2)](3+) are emissive in the near‐IR‐II region, the [V(ddpd)(2)](2+) complexes are non‐luminescent due to metal‐to‐ligand charge transfer admixture to the spin‐flip states. John Wiley and Sons Inc. 2022-12-21 2023-02-10 /pmc/articles/PMC10107508/ /pubmed/36345821 http://dx.doi.org/10.1002/chem.202202898 Text en © 2022 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH https://creativecommons.org/licenses/by-nc/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc/4.0/ (https://creativecommons.org/licenses/by-nc/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes. |
spellingShingle | Research Articles Dorn, Matthias Hunger, David Förster, Christoph Naumann, Robert van Slageren, Joris Heinze, Katja Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title | Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title_full | Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title_fullStr | Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title_full_unstemmed | Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title_short | Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence |
title_sort | towards luminescent vanadium(ii) complexes with slow magnetic relaxation and quantum coherence |
topic | Research Articles |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10107508/ https://www.ncbi.nlm.nih.gov/pubmed/36345821 http://dx.doi.org/10.1002/chem.202202898 |
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