Defect mediated ferromagnetism in Ni-doped ZnO nanocrystals evidenced by positron annihilation spectroscopy

Abstract

NiO/ZnO nanocomposites with NiO content of 4 at. % and 20 at. % were annealed up to 1200 °C to get Ni doped ZnO nanocrystals. Raman scattering spectra illustrate a broad and strong band at 500-600cm−1 in all nanocomposites after annealing above 700 °C, which suggests incorporation of Ni in the ZnO lattice. However, x-ray diffraction measurements show that NiO phase can be still observed in all nanocomposites after annealing, which indicates that Ni is partially doped into the ZnO structure. Positron annihilation measurements reveal large number of vacancy defects in the interface region of all nanocomposites, and they are gradually recovered with increasing annealing temperature up to 1000 °C. Room temperature ferromagnetism can be observed in the NiO/ZnO nanocomposites, which is stronger in the 20 at. % NiO/ZnO nanocomposites, and the magnetization decreases continuously with increasing annealing temperature. This indicates that the ferromagnetism at low annealing temperatures originates from the NiO nanograins, and they become antiferromanetic after subsequent higher temperature annealing which leads to the weakening of ferromagnetism. After annealing up to 1000 °C, the ferromagnetism in both the two samples becomes nearly invisible. The disappearance of ferromagnetism shows good coincidence with the recovery of vacancy defects in NiO/ZnO nanocomposites. It can be inferred that the ferromagnetism is mediated by vacancy defects which are distributed in the interface region.