Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide
Abstract We are reporting on the use of a low‐coordinate YbIII amide with near‐ideal planar trigonal [Yb{N(SiMe3)2}3] (1) and on a bipyramidal trigonal derivative [Yb{N(SiMe2H)2}3 ⋅ (thf)2] (2) that constitute quintessential cases to investigate luminescent and magnetic properties otherwise usually...
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Wiley-VCH
2024-11-01
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| Online Access: | https://doi.org/10.1002/ceur.202400062 |
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| author | Dr. Nimisha Jain Dr. Félix Houard Rémi Marchal Marie Cordier Dr. Boris Le Guennic Dr. Yan Suffren Dr. Yann Sarazin Prof. Kevin Bernot |
| author_facet | Dr. Nimisha Jain Dr. Félix Houard Rémi Marchal Marie Cordier Dr. Boris Le Guennic Dr. Yan Suffren Dr. Yann Sarazin Prof. Kevin Bernot |
| author_sort | Dr. Nimisha Jain |
| collection | DOAJ |
| description | Abstract We are reporting on the use of a low‐coordinate YbIII amide with near‐ideal planar trigonal [Yb{N(SiMe3)2}3] (1) and on a bipyramidal trigonal derivative [Yb{N(SiMe2H)2}3 ⋅ (thf)2] (2) that constitute quintessential cases to investigate luminescent and magnetic properties otherwise usually blurred on less symmetrical compounds. These compounds represent the first experimental objects that allow for the confirmation of the recent conjecture about best‐performing SMM built on the archetypal prolate lanthanide ion. We have performed a combined theoretical, luminescent, and magnetic study on these molecules. For 1, a spectacular split of the 2F7/2 ground state of 1312 cm−1 is measured by low‐temperature near‐infra‐red luminescence as well as the calculated pure wavefunction composition of the low‐lying Kramers doublets, making this complex a textbook example of a prolate SMM. These results are corroborated by comparison with 2, that exhibits as expected a 50 % decrease of the ground state splitting compared to 1. Yet, we show that these remarkable features are insufficient to promote SMM behavior, and Orbach relaxation is unlikely to occur even on such an ideal low‐coordinate SMM without control of spin‐phonon coupling. |
| format | Article |
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| institution | OA Journals |
| issn | 2751-4765 |
| language | English |
| publishDate | 2024-11-01 |
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| spelling | doaj-art-ecee32b1873f4b81a94b4e557aecc27f2025-08-20T02:14:15ZengWiley-VCHChemistryEurope2751-47652024-11-0126n/an/a10.1002/ceur.202400062Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) AmideDr. Nimisha Jain0Dr. Félix Houard1Rémi Marchal2Marie Cordier3Dr. Boris Le Guennic4Dr. Yan Suffren5Dr. Yann Sarazin6Prof. Kevin Bernot7Univ Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEUniv Rennes INSA Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Université de Rennes Rennes FRANCEAbstract We are reporting on the use of a low‐coordinate YbIII amide with near‐ideal planar trigonal [Yb{N(SiMe3)2}3] (1) and on a bipyramidal trigonal derivative [Yb{N(SiMe2H)2}3 ⋅ (thf)2] (2) that constitute quintessential cases to investigate luminescent and magnetic properties otherwise usually blurred on less symmetrical compounds. These compounds represent the first experimental objects that allow for the confirmation of the recent conjecture about best‐performing SMM built on the archetypal prolate lanthanide ion. We have performed a combined theoretical, luminescent, and magnetic study on these molecules. For 1, a spectacular split of the 2F7/2 ground state of 1312 cm−1 is measured by low‐temperature near‐infra‐red luminescence as well as the calculated pure wavefunction composition of the low‐lying Kramers doublets, making this complex a textbook example of a prolate SMM. These results are corroborated by comparison with 2, that exhibits as expected a 50 % decrease of the ground state splitting compared to 1. Yet, we show that these remarkable features are insufficient to promote SMM behavior, and Orbach relaxation is unlikely to occur even on such an ideal low‐coordinate SMM without control of spin‐phonon coupling.https://doi.org/10.1002/ceur.202400062lanthanidesluminescenceprolatesingle-molecule magnetsytterbium(III) |
| spellingShingle | Dr. Nimisha Jain Dr. Félix Houard Rémi Marchal Marie Cordier Dr. Boris Le Guennic Dr. Yan Suffren Dr. Yann Sarazin Prof. Kevin Bernot Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide ChemistryEurope lanthanides luminescence prolate single-molecule magnets ytterbium(III) |
| title | Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide |
| title_full | Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide |
| title_fullStr | Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide |
| title_full_unstemmed | Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide |
| title_short | Luminescence and Single‐Molecule Magnet Properties in Ideal Symmetry Compounds: Example of a Near‐Planar Tricoordinate Ytterbium(III) Amide |
| title_sort | luminescence and single molecule magnet properties in ideal symmetry compounds example of a near planar tricoordinate ytterbium iii amide |
| topic | lanthanides luminescence prolate single-molecule magnets ytterbium(III) |
| url | https://doi.org/10.1002/ceur.202400062 |
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