On Approaching the Limit of Molecular Magnetic Anisotropy: A Near‐Perfect Pentagonal Bipyramidal Dysprosium(III) Single‐Molecule Magnet

We report a monometallic dysprosium complex, [Dy(OtBu)2(py)5][BPh4] (5), that shows the largest effective energy barrier to magnetic relaxation of Ueff=1815(1) K. The massive magnetic anisotropy is due to bis‐trans‐disposed tert‐butoxide ligands with weak equatorial pyridine donors, approaching proposed schemes for high‐temperature single‐molecule magnets (SMMs). The blocking temperature, TB , is 14 K, defined by zero‐field‐cooled magnetization experiments, and is the largest for any monometallic complex and equal with the current record for [Tb2N2{N(SiMe3)2}4(THF)2].