Mixed‐Valence Nickel Bis(azamacrocycle) Compounds with Ghost‐Leg‐type Sheets

The fabrication of so‐called ghost‐leg sheets and their electronic properties is reported. This unique sheet structure is composed of one‐dimensional mixed‐valence nickel chains, which are linked with one another by bis(azamacrocycle) ligands. They are also topologically unique Ni^II/Ni^III mixed‐valence complexes, as confirmed by X‐ray and optical measurements. Moreover, their magnetic susceptibilities indicated two‐dimensional antiferromagnetic behavior following the Fisher 1D chain model with interchain interactions, where spins on Ni^III sites mutually interact antiferromagnetically in the sheets.