Lanthanide‐Based Molecular Magnetic Semiconductors

Magnetic semiconductors, with integrated properties of ferromagnets and semiconductors, are significant for developing next‐generation spintronic devices. Herein two atomically precise clusters of dysprosium(III) tellurides, formulated respectively as [Na2(15‐crown‐5)3(py)][(η5‐Cp*Dy)5(Te)6](py)4 (Dy5Te6, Cp* = pentamethylcyclopentadienyl; py = pyridine) and [K(2,2,2‐cryptand)]2[(η5‐Cp*Dy)6(Te3)(Te2)2(Te)3] (Dy6Te10), are reported. Crystallographic studies revealed the presence of multifarious tellurido ligands within the polyhedral cluster cores. Spectroscopic and magnetic studies showed that both clusters are single‐molecule magnets exhibiting slow magnetic relaxation behaviors at low temperatures and semiconductors with optical bandgaps comparable to benchmark semiconductors. These clusters represent probably the first lanthanide‐based molecular magnetic semiconductors.