Highly versatile tetradentate N2S2 ligands bind to numerous transition metals and, as the Cys-X-Cys motif in proteins, play important roles in metalloenzymes such as Acetyl CoA Synthase and Nitrile Hydratase. We have contributed to extensive studies of M(N2S2) using various metals such as nickel, palladium, and iron with di- and tetraanionic N2S2 donor ligands, and are currently examg. such sites with paramagnetic ions such as [V≡O]2+ and Mn2+. With its d1 electronic configuration, [V≡O]2...