Paramagnetism and antiferromagnetic interactions in single-phase Fe-implanted ZnO

As the intrinsic origin of the high temperature ferromagnetism often observed in wide-gap dilute magnetic semiconductors becomes increasingly debated, there is a growing need for comprehensive studies on the single-phase region of the phase diagram of these materials. Here we report on the magnetic and structural properties of Fe-doped ZnO prepared by ion implantation of ZnO single crystals. A detailed structural characterization shows that the Fe impurities substitute for Zn in ZnO in a wurtzite Zn$_{1−x}$Fe$_{x}$O phase which is coherent with the ZnO host. In addition, the density of beam-induced defects is progressively decreased by thermal annealing up to 900$^{\circ}$C, from highly disordered after implantation to highly crystalline upon subsequent annealing. Based on a detailed analysis of the magnetometry data, we demonstrate that isolated Fe impurities occupying Zn substitutional sites behave as localized paramagnetic moments down to 2$^{\circ}$K, irrespective of the Fe concentration and the density of beam-induced defects. With increasing local concentration of Zn-substitutional Fe, strong nearest-cation-neighbor antiferromagnetic interactions favor the antiparallel alignment of the Fe moments.