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A hydroxide-bridged centrosymmetric Dy III dimer with each Dy III being five-coordinated has been synthesized using bulky hindered phenolate ligands. Magnetic studies revealed that this compound exhibits a slow magnetic relaxation of a single-ion origin together with a step-like magnetic hysteresis of the magnetic coupled cluster. The thermal relaxation barrier of magnetization is 721 K in the absence of a static magnetic field, while the intramolecular magnetic interaction is very large among reported 4f-only dimers. CASSCF calculations with a larger active space were performed to understand the electronic structure of the compound. The thermal relaxation regime and the quantum tunneling regime are well separated, representing a good model to study the relaxation mechanism of SMMs with intramolecular Dy-Dy magnetic interactions.

chemical science

Hydroxide-bridged five-coordinate Dy<sup>III</sup> single-molecule magnet exhibiting the record thermal relaxation barrier of magnetization among lanthanide-only dimers

Hydroxide-bridged five-coordinate DyIII single-molecule magnet exhibiting the record thermal relaxation barrier of magnetization among lanthanide-only dimers

Hydroxide-bridged five-coordinate Dy^III single-molecule magnet exhibiting the record thermal relaxation barrier of magnetization among lanthanide-only dimers