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cted by copyright. All rights reserved.We report a new family of five-coordinate Lanthanide Single-Molecule Magnets (Ln SMMs) [Dy(Mes*O) 2 (THF) 2 X] (Mes*= 2,4,6-tri-tert-butylphenyl; X = Cl, 1 ; Br, 2 ; I, 3 ) with energy barriers to magnetic reversal amongst the highest reported for any SMM to date. The five-coordinate Dy(III) ions have distorted square pyramidal geometries, with halide anions on the apex, and two Mes*O ligands mutually trans- to each other, and the two THF molecules forming the second trans- pair. These geometrical

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