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A mononuclear as well as dinuclear DyIII complexes of general formula [Dy(hmb)(NO3)2(DMF)2] (1) and [Dy2(hmt)(NO3)4(DMF)4]·DMF (2), where Hhmb: (N′-(2-hydroxy-3-methoxybenzylidene)benzohydrazide and H2hmt: (N1,N4)-N′1,N′4-bis(2-hydroxy-3-methoxybenzylidene)terephthalohydrazide were obtained using a synthetic strategy involving a polytopic Schiff base ligand. Single-crystal X-ray analysis reveals the DyIII ion is in a distorted pentagonal interpenetrating tetrahedral arrangement. The two symmetrical DyIII ions in complex 2 exhibit the same geometry and are well-isolated in the molecule by an hmt2− ligand. The direct current (dc) and alternating current (ac) magnetic measurements of the compounds were investigated. Complex 1 did not exhibit any ac signal whereas a frequency dependant signal was observed for 2 under zero dc field. When an optimum dc field was applied, clear frequency dependant signals were obtained for both complexes indicative of Single-Ion Magnet behaviour with relaxation barriers of Ueff = 34 and 42 K for 1 and 2, respectively.
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