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. 2023 Aug;15(8):1100-1107.
doi: 10.1038/s41557-023-01208-y. Epub 2023 May 25.

A trivalent 4f complex with two bis-silylamide ligands displaying slow magnetic relaxation

Dylan Errulat  1 , Katie L M Harriman  1 , Diogo A Gálico  1 , Alexandros A Kitos  1 , Akseli Mansikkamäki  2 , Muralee Murugesu  3
Affiliations

A trivalent 4f complex with two bis-silylamide ligands displaying slow magnetic relaxation

Dylan Errulat et al. Nat Chem. 2023 Aug.

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.

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