Synthesis, Structure, and Magnetic Properties of Rare-Earth Bis(diazabutadiene) Diradical Complexes

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Abstract
New kinds of diradical rare-earth metal complexes supported by diazabutadiene (DAD) ligands, [(DAD)2LnN(TMS)2] (1; Ln = Dy, Lu; TMS = SiMe3), were synthesized and studied. They showed a new [radical–Ln–radical] alignment with distorted square-pyramidal geometry. Structural and density functional theory analysis illustrated the radical anionic nature of the ligands. Magnetic studies revealed antiferromagnetic coupling of the two radicals in 1-Lu. 1-Dy showed typical single-molecule-magnet (SMM) behavior with an effective energy barrier of 231 K, which is much higher than those of similar radical-containing SMMs. Magnetostructural analysis suggests that the anionic [N(TMS)2]− group plays a vital role in the SMM property. This study provides a new platform for further improving the performance of radical–Ln SMMs.
Funding Information
  • National Natural Science Foundation of China (21725201, 21801037, 21890721)