Two New Dy ₃ Triangles with Trinuclear Circular Helicates and Their Single-Molecule Magnet Behavior

Self-assembly of polydentate Schiff base 2,6-diformyl-4-methylphenol di(benzoy1hydrazone) (H(3)L), with dysprosium thiocyanate and sodium azide, affords two novel trinuclear triangular circular helicate dysprosium(III) complexes, [Dy(3)(μ(3)-OCH(3))(2)(HL)(3)(SCN)]·4CH(3)OH·2CH(3)CN·2H(2)O (1) or [Dy(3)(μ(3)-N(3))(μ(3)-OH)(H(2)L)(3)(SCN)(3)](SCN)·3CH(3)OH·H(2)O (2), depending on the presence or absence of base. Single-crystal X-ray analyses show that two μ(3)-methoxy oxygens cap the Dy(3) triangle in complex 1 and that one μ(3)-OH and one μ(3)-N(3)(-) cap the Dy(3) triangle of complex 2, representing the first example of a μ(3)-N(3)(-)-capped lanthanide complex reported to date. Ac susceptibility measurements reveal that multiple relaxation processes and the onset of slow magnetization relaxation occur for complex 1 and 2, respectively. Theoretical calculations are required to elucidate the underlying mechanism; however, the different magnetic anisotropy of the respective structures, which is dictated by the coordination environment of Dy(III) ions and structural parameters of the triangles, is mostly responsible for the distinctive relaxation dynamics observed.