Abstract
Two new cobalt(II) complexes with an unsymmetrical bidentate ligand, 2-(1,4,5,6-tetrahydropyrimidin-2-yl)-6-methoxyphenol (H2mthp), were synthesized and crystallographically characterized. Tetra- and hexa-coordinate mononuclear complexes were selectively obtained by adjusting the stoichiometry of the base. The coordination geometry of hexa-coordinated complex was severely distorted from an ideal octahedron, due to the NO5 coordination environment from the mixed coordination of one Hmthp− and two H2mthp ligands. Both complexes formed one-dimensional chain networks by hydrogen-bond and N-H···π interactions. Single-molecule magnet behavior was observed for the tetrahedral complex under zero magnetic field. The relatively short Co···Co distances induced non-zero intermolecular magnetic coupling, which split the ground ±Ms levels to suppress quantum-tunneling of magnetization. In the octahedral complex, by contrast, the distance was not short enough to induce the coupling. As a consequence, single-molecule magnetic behavior was observed for the octahedral complex only in the presence of an external static field.
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