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• W4366083979 abstract "The recent discovery of metal-metal bonding and valence delocalization in the dilanthanide complexes (CpiPr5)2Ln2I3 (CpiPr5 = pentaisopropylcyclopentadienyl; Ln = Y, Gd, Tb, Dy) opened up the prospect of harnessing the 4fn5dz21 electron configurations of non-traditional divalent lanthanide ions to access molecules with novel bonding motifs and magnetism. Here, we report the trinuclear mixed-valence clusters (CpiPr5)3Ln3H3I2 (1-Ln, Ln = Y, Gd), which were synthesized via potassium graphite reduction of the trivalent clusters (CpiPr5)3Ln3H3I3. Structural, computational, and spectroscopic analyses support valence delocalization in 1-Ln resulting from a three-center, one-electron σ bond formed from the 4dz2 and 5dz2 orbitals on Y and Gd, respectively. Dc magnetic susceptibility data obtained for 1-Gd reveal that valence delocalization engenders strong parallel alignment of the σ-bonding electron and the 4f electrons of each gadolinium center to afford a high-spin ground state of S = 11. Notably, this represents the first clear instance of metal-metal bonding in a molecular trilanthanide complex, and the large spin-spin exchange constant of J = 168(1) cm-1 determined for 1-Gd is only the second largest coupling constant characterized to date for a molecular lanthanide compound." @default.
• W4366083979 created "2023-04-19" @default.
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• W4366083979 date "2023-04-17" @default.
• W4366083979 modified "2023-10-01" @default.
• W4366083979 title "A Trinuclear Gadolinium Cluster with a Three-Center One-Electron Bond and an <i>S</i> = 11 Ground State" @default.
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• W4366083979 doi "https://doi.org/10.1021/jacs.3c00182" @default.
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