Room temperature ferromagnetism in pure ZnO thin films prepared by spin-coating method was observed. X-ray photoelectron spectroscopy and inductively coupled plasma-mass spectrometry showed no or extremely little presence of impurities, which were unlikely to be responsible for the large magnetization moment observed. In order to study the origin of ferromagnetism, ZnO thin films were rapidly annealed in N2 and O2 ambient in a repetitive way. Electrical and magnetic performance after each annealing was measured. It is found that ferromagnetism is diminished and re-appeared, in accordance with the decrease and increase of conductivity. Cathodoluminescence spectra show evidence of reversible variation of oxygen vacancy defect in the annealing process. These results provide strong evidence that oxygen vacancies play a significant role in inducing ferromagnetism in ZnO thin films.
The effect of intrinsic point defects on the electronic structure and absorption spectra of ZnO was investigated by first-principle calculation. Among the intrinsic point defects in ZnO, oxygen vacancies [Formula: see text] and interstitial zinc [Formula: see text] have the lower formation energy and the more stable structure under zinc(Zn)-rich condition, whereas zinc vacancies [Formula: see text] and interstitial oxygen [Formula: see text] have the lower formation energy and the more stable structure under oxygen(O)-rich condition. The band gap of [Formula: see text] becomes narrow and the absorption spectrum has a redshift. In the visible region, the photo-excited electron transition of [Formula: see text] is graded from the valence band top to the impurity level and then to the conduction band bottom, showing the redshift of absorption spectrum of [Formula: see text] and explaining the reason of [Formula: see text] forming a deep impurity levels in ZnO. Moreover, the impurity energy level of [Formula: see text] coincides with the Fermi level, indicating the significant trap effect and the slow recombination of electrons and holes, which are conducive to the design and preparation of novel ZnO photocatalysts. The band gap of [Formula: see text] and [Formula: see text] broadened and the absorption spectrum showed blueshift, explaining the different values of the ZnO band gap width.
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