It has been known for a long time that the magnetic exchange interaction between copper and gadolinium ions is always ferromagnetic. Very recently, three exceptions to this general trend were revealed. They involve complexes associating a gadolinium(III) ion with a copper(II) ion or with radicals of the nitroxide or semiquinone types. We want to show that this trend is more general than expected, for such a behavior can also be observed in heterobinuclear vanadyl‐gadolinium complexes.

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