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We have investigated the relation between local structure, valence and carrier type with magnetism in the Zn-Co-O system. Thin films ranging from wurtzite Zn 1−x Co x O (Co:ZnO) to ZnCo 2 O 4  spinel were grown on  c -sapphire substrates. On the one hand, the unprecedented doping of x = 0.6 Co in ZnO enables to study the structural and magnetic properties well-above the coalescence limit. On the other hand, the ZnCo 2 O 4  spinel provides a  p -type environment. We find a strong correlation between local structure, valence and carrier type throughout the Zn-Co-O system. In contrast to earlier publications neither 60% Co:ZnO nor ZnCo 2 O 4  exhibit any sign of ferromagnetic order despite of the high concentration of magnetic ions and a  p -type carrier background. Instead, antiferromagnetic exchange is found to be the predominant magnetic interaction in the Zn-Co-O system.

Magnetic interactions in the Zn-Co-O system: tuning local structure, valence and carrier type from extremely Co doped ZnO to ZnCo2O4