Paramagnetic, monoanionic and square-planar nickel bisdithiolene complexes are best described as having delocalized class-III mixed-valent radical anionic ligands coordinated to a closed shell low-spin d8 central metal, based on combined structural and spectroscopic studies given in several publications. They can be described by the resonance structures [NiII(L2−)(L−.)]− ↔ [NiII(L−.)(L2−)]−. In our formulation we have not differentiated the ligand “L”, which can carry the charges 2− or 1−. and vice versa.
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