One- and two-electron oxidized CuII complexes of Schiff base ligands with para-substituted phenolate moieties were synthesized and characterized. The crystal structure of the one-electron oxidized methylthio-substituted complex [Cu(MeS-salen)]SbCl6 revealed the intermolecular π-π stacking interaction of the two phenolate moieties with those of the neighboring complex cations to form the one-dimensional chain. Such a π-π stacking interaction could not be detected in the two-electron oxidized complex [Cu(MeS-salen)](SbCl6)2 and the oxidized methoxy-substituted complexes [Cu(MeO-salen)](SbF6)n (n=1, 2). Magnetic study of [Cu(MeO-salen)]SbF6 showed a weak antiferromagnetic interaction between the CuII ion and phenoxyl radical unpaired electron spins, while [Cu(MeS-salen)]SbCl6 showed a ferromagnetism. Both of the two-electron oxidized complexes exhibited a relatively strong magnetic interaction between the two radical electrons, while the signs of the electron spins are different.
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