Abstract
AbstractAbstraction of a chloride ligand from the dysprosium metallocene [(Cpttt)2DyCl] (1Dy Cpttt=1,2,4‐tri(tert‐butyl)cyclopentadienide) by the triethylsilylium cation produces the first base‐free rare‐earth metallocenium cation [(Cpttt)2Dy]+ (2Dy) as a salt of the non‐coordinating [B(C6F5)4]− anion. Magnetic measurements reveal that [2Dy][B(C6F5)4] is an SMM with a record anisotropy barrier up to 1277 cm−1 (1837 K) in zero field and a record magnetic blocking temperature of 60 K, including hysteresis with coercivity. The exceptional magnetic axiality of 2Dy is further highlighted by computational studies, which reveal this system to be the first lanthanide SMM in which all low‐lying Kramers doublets correspond to a well‐defined MJ value, with no significant mixing even in the higher doublets.
Highlights
The drive to combine the macroscopic properties of bulk magnetic materials with the quantum effects observed in molecule-based materials has led to an explosion of interest in single-molecule magnets (SMMs).[1]
A transformative breakthrough came with the report of slow magnetic relaxation in a D4d-symmetric monometallic terbium phthalocyanine SMM,[7] with many derivatives of these systems showing enhanced properties such as larger effective energy barriers to reversal of the magnetization as a result of simple modifications to the ligand periphery.[8]
Our contributions have focused on cyclopentadienylligated dysprosium SMMs of the type [(Cp)2Dy(E)]n (n = 2, 3) with various Cp ligands and a wide variety of heteroatom donor ligands, including systems with E = N, P, As, Sb, S and Se donors.[10]
Summary
The drive to combine the macroscopic properties of bulk magnetic materials with the quantum effects observed in molecule-based materials has led to an explosion of interest in single-molecule magnets (SMMs).[1].
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