The origins of ferromagnetism in Co-doped ZnO single crystalline films: From bound magnetic polaron to free carrier-mediated exchange interaction

High-quality Co-doped ZnO single crystalline films with a wide range of carrier concentration and good reproducibility have been grown by molecular beam epitaxy. After the systematic studies of the magnetic and transport properties of the films, we suggest that there are two distinct ferromagnetic mechanisms in different conductivity regimes. In the insulating regime, carriers tend to be localized, favoring the formation of bound magnetic polarons, which leads to ferromagnetism. In the metallic regime, however, most carriers are weakly localized and the free carrier-mediated exchange is dominant. Our experimental observations are well consistent with the recent theoretical description of magnetism in Co-doped ZnO and helpful for understanding the ferromagnetic mechanism in oxide-based diluted magnetic semiconductors.