A trivalent 4f complex with two bis-silylamide ligands displaying slow magnetic relaxation
Errulat, Dylan; Harriman, Katie L. M.; Gálico, Diogo A.; Kitos, Alexandros A.; Mansikkamäki, Akseli; Murugesu, Muralee (2023-05-25)
Springer
25.05.2023
Errulat, D., Harriman, K.L.M., Gálico, D.A. et al. A trivalent 4f complex with two bis-silylamide ligands displaying slow magnetic relaxation. Nat. Chem. 15, 1100–1107 (2023). https://doi.org/10.1038/s41557-023-01208-y
https://rightsstatements.org/vocab/InC/1.0/
© 2023, The Author(s), under exclusive licence to Springer Nature Limited. This version of the article has been accepted for publication, after peer review (when applicable) and is subject to Springer Nature’s AM terms of use, but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1038/s41557-023-01208-y
https://rightsstatements.org/vocab/InC/1.0/
© 2023, The Author(s), under exclusive licence to Springer Nature Limited. This version of the article has been accepted for publication, after peer review (when applicable) and is subject to Springer Nature’s AM terms of use, but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1038/s41557-023-01208-y
https://rightsstatements.org/vocab/InC/1.0/
Julkaisun pysyvä osoite on
https://urn.fi/URN:NBN:fi:oulu-202401031038
https://urn.fi/URN:NBN:fi:oulu-202401031038
Tiivistelmä
Abstract
The best-performing single-molecule magnets (SMMs) have historically relied on pseudoaxial ligands delocalized across several coordinated atoms. This coordination environment has been found to elicit strong magnetic anisotropy, but lanthanide-based SMMs with low coordination numbers have remained synthetically elusive species. Here we report a cationic 4f complex bearing only two bis-silylamide ligands, Yb(III)[{N(SiMePh2)2}2][Al{OC(CF3)3}4], which exhibits slow relaxation of its magnetization. The combination of the bulky silylamide ligands and weakly coordinating [Al{OC(CF3)3}4]− anion provides a sterically hindered environment that suitably stabilizes the pseudotrigonal geometry necessary to elicit strong ground-state magnetic anisotropy. The resolution of the mJ states by luminescence spectroscopy is supported by ab initio calculations, which show a large ground-state splitting of approximately 1,850 cm−1. These results provide a facile route to access a bis-silylamido Yb(III) complex, and further underline the desirability of axially coordinated ligands with well-localized charges for high-performing SMMs.
The best-performing single-molecule magnets (SMMs) have historically relied on pseudoaxial ligands delocalized across several coordinated atoms. This coordination environment has been found to elicit strong magnetic anisotropy, but lanthanide-based SMMs with low coordination numbers have remained synthetically elusive species. Here we report a cationic 4f complex bearing only two bis-silylamide ligands, Yb(III)[{N(SiMePh2)2}2][Al{OC(CF3)3}4], which exhibits slow relaxation of its magnetization. The combination of the bulky silylamide ligands and weakly coordinating [Al{OC(CF3)3}4]− anion provides a sterically hindered environment that suitably stabilizes the pseudotrigonal geometry necessary to elicit strong ground-state magnetic anisotropy. The resolution of the mJ states by luminescence spectroscopy is supported by ab initio calculations, which show a large ground-state splitting of approximately 1,850 cm−1. These results provide a facile route to access a bis-silylamido Yb(III) complex, and further underline the desirability of axially coordinated ligands with well-localized charges for high-performing SMMs.
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