The molecular structures and the spin ground-state of the iron(II/III) complexes Fe1, Fe2 and Fe3, which contain dianionic macrocyclic [N 4 ] ligands derived from substituted acetylacetaldehydes and 1,2-diamines, have been investigated by X-ray analysis and temperature-dependent susceptibility measurements, respectively. The iron (II) . The iron centre in Fe II 2 is nearly square-planar and shows a strong decrease of the magnetic moment below T Ϸ 250 K. This is probably due to an S = 0 to S = 1 spin-crossover or, more likely, to intermolecular