First principles study of magneto-optical properties of Fe-doped ZnO

Abstract Studies on optical band gaps and absorption spectra of Fe-doped ZnO have conflicting conclusions, such as contradictory redshifted and blueshifted spectra. To solve this contradiction, we constructed models of un-doped and Fe-doped ZnO using first-principles theory and optimized the geometry of the three models. Electronic structures and absorption spectra were also calculated using the GGA+ U method. Higher doping content of Fe resulted in larger volume of doped system, and higher total energy resulted in lower stability. Higher formation energy also led to more difficult doping. Meanwhile, the band gaps broadened and the absorption spectra exhibited an evident blue shift. The calculations were in good agreement with the experimental results. Given the unipolar structure of ZnO, four possible magnetic coupling configurations for Zn 14 Fe 2 O 16 were calculated to investigate the magnetic properties. Results suggest that Fe doping can improve ferromagnetism in the ZnO system and that ferromagnetic stabilization was mediated by p–d exchange interaction between Fe-3 d and O-2 p orbitals. Therefore, the doped system is expected to obtain high stability and high Curie temperature of diluted magnetic semiconductor material, which are useful as theoretical bases for the design and preparation of the Fe-doped ZnO system’s magneto-optical properties.