Role of molecular symmetry in the magnetic relaxation dynamics of five-coordinate Dy(iii) complexes†
Abstract
A new family of low-coordinate mononuclear DyIII single-molecule magnets [(TrapenTMS)Dy(LB)] (Trapen = tris(2-aminobenzyl)amine; TMS = SiMe3; LB = THF 1, pyridine 2, ONMe33) has been synthesized and structurally characterized by single crystal X-ray diffraction. The five-coordinate DyIII ions exhibit distorted triangular bipyramidal geometries, among the different neutral ligands LB on the apex and the same TrapenTMS ligand, making the pyramid base of the trigonal bipyramid. Magnetic data analysis reveals that 1–3 are characteristic of SMM behaviors without a dc field, accompanying an unambiguous quantum tunneling of magnetization. Under an extra dc field of 500 Oe, field-induced slow magnetic relaxation behaviors occur with Raman and/or QTM processes. Ab initio calculations were also performed to rationalize the observed discrepancy in the magnetic behaviors, and the result illustrates that the SMM behavior could be effectively manipulated by the axial symmetry of the triangular bipyramidal DyIII motifs.
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