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 g z 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).