Multifunctional single-molecule magnets (SMMs) have sparked great interest, but chiral SMMs obtained via spontaneous resolution are rarely reported. We synthesized a series of chiral trinuclear hepta-coordinate lanthanide complexes [ZnLn] ( for Dy, for Tb, for Gd, and for DyY) using the achiral flexible ligand HL (2,2'-[1,2-ethanediylbis[(ethylimino)methylene]]bis[3,5-dimethylphenol]). The complexes crystallize in the chiral 6 group space, and two enantiomers of different chirality are spontaneously resolved. Three [Zn(L)Cl] anions utilize the two phenoxy oxygen atoms of each L to coordinate with three lanthanide ions, respectively, and the three hepta-coordinate lanthanide ions are arranged in a triangle. The chirality comes from the propeller arrangement of the peripheral three bidentate chelate L ligands like octahedral [M(AA)] (M = transition metal ions; AA = bidentate chelate ligands, e.g., 2,2'-bipyridine, 1,10-phenathroline, ethylenediamine, acac or oxalate). Complex exhibits an AC susceptibility signal and is frequency-dependent, which is typical of SMMs. Complex , doped with a large amount of diamagnetic Y(III) in Dy(III), exhibits = 48.3 K and τ = 4.4 × 10 s in experiments. Complex shows circularly polarized luminescence and apparent photoluminescence, typical of the f-f transitions of Tb(III).
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