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Manipulating the ferromagnetism of diluted magnetic semiconductors by tuning the valence state of doped ions is found to be achievable in Mn‐doped NiO. First‐principles calculations predict that the interactions between substitutional Mn3+ ions in NiO are ferromagnetic, while the Mn2+–Mn2+ interactions are antiferromagnetic. This scenario is experimentally supported by a great enhancement of saturation...
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