Magnetic Anisotropy from Trigonal Prismatic to Trigonal Antiprismatic Co(II) Complexes: Experimental Observation and Theoretical Prediction

A family of trigonal antiprismatic Co(II) complexes was synthesized, which exhibited field-induced Raman process dominated single-molecule magnet behavior. Despite the coordination environment of Co(II) being of similar symmetry, the four complexes exhibit distinct dynamic magnetic properties owing to their packing arrangements and dipole–dipole interactions. On the basis of computational results we have demonstrated that the gz and giso values follow a cosine relation with respect to the rotated angle φ (twist angle φ defined as the rotation angle of one coordination square away from the eclipse conformation to the other).