Single-Molecule Magnet Behavior with a Single Metal Center Enhanced through Peripheral Ligand Modifications

Bis(imino)pyridine pincer ligands in conjunction with two isothiocyanate ligands have been used to prepare two mononuclear Co(II) complexes. Both complexes have a distorted square-pyramidal geometry with the Co(II) centers lying above the basal plane. This leads to significant spin–orbit coupling for the d<sup>7</sup> Co(II) ions and consequently to slow relaxation of the magnetization that is characteristic of Single-Molecule Magnet (SMM) behavior.