First organic radicals, now metal complexes: A successful extension to metal complexes of a well‐known organic radical approach to ferromagnetism is exemplified by the triplet ground‐state molecule containing two CuII centers connected by a double m‐phenylenediamide skeleton of the cyclophane type shown in the scheme.

Self-assembly of 1,4-phenylenebis(oxamate) and 4,4'-biphenylenebis(oxamate) ligands and Cu2+ ions gives two new dinuclear copper(II) metallacyclophanes where the two metal centers are connected by double para-substituted aromatic diamide bridges. Despite the relatively large intramolecular Cu-Cu distance of ca. 8 and 12 A for each complex, magnetic susceptibility measurements evidence strong to moderately strong intramolecular antiferromagnetic couplings (-J values of the order of 100 and 10 cm-1, respectively). Density functional theory calculations on these compounds and their homologues with linear oligo-p-phenylenediamide bridges predict a rather slow exponential decay of magnetic coupling with increasing intermetal distance (r values up to 25 A) along this novel series of dicopper metalla-amidocyclophanes.