A series of films deposited under different oxygen partial pressures and annealed under different atmospheres were prepared to investigate the role of oxygen vacancies in tuning magnetic properties of Co-doped SnO2 films. The inclusive Co in SnO2 is in the 2+ state and substitutes for the Sn4+ site. Intrinsic room temperature ferromagnetism is observed in all films, which is not carrier mediated, but coexists with the dielectric behavior. A maximum magnetic moment of 2.37 μB∕Co is achieved by vacuum annealing due to the increase and diffusion of oxygen vacancies rather than the improvement of crystallinity of the film, and the magnetic moment decreases considerably after air annealing or increasing the oxygen partial pressure during deposition. The changes of oxygen vacancy concentration and distribution are indirectly demonstrated by the relative shifts of Co 2p3∕2 peaks in XPS spectra. The band gap of Co-doped SnO2 film is larger than that of pure SnO2 film, suggesting the influence of inclusive Co on the electronic states, and further blueshift after annealing is also visible. The F-center model is modified to explain the ferromagnetism in insulating Co-doped SnO2 films.
Sn 1 − x Co x O 2 films have been fabricated to study the local structure of Co dopant and the mediation effects of donor defects (oxygen vacancies and Sn interstitials) on magnetic properties. Compared to as-grown film, the ferromagnetism is evidently enhanced after annealing in vacuum at 400 °C due to the increase in oxygen vacancies. While annealing at higher temperature, the ferromagnetism declines because of the domination of decrease in Sn interstitials over increase in oxygen vacancies in the films. The incorporation of Co dopant as well as the presence of oxygen vacancies and Sn interstitials is verified using x-ray absorption fine structure spectroscopy. The variations in the concentration of defects as a function of annealing temperature are obtained by positron annihilation spectroscopy technique. Additionally, the changes in structure and ferromagnetism after annealing in different atmospheres further demonstrate the crucial roles of oxygen vacancies and Sn interstitials in tuning ferromagnetism.
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