Structural, optical, and electronic properties of room temperature ferromagnetic GaCuN film grown by hybrid physical-chemical vapor deposition

Abstract

Ferromagnetic Cu-doped GaN film was grown on a GaN-buffered sapphire (0001) substrate by a hybrid physical-chemical-vapor-deposition method (HPCVD). The GaCuN film (Cu: 3.6 at.%) has a highly c-axis-oriented hexagonal wurtzite crystal structure, which is similar to GaN buffer but without any secondary phases such as metallic Cu, CuxNy, and CuxGay compounds. Two weak near-band edge (NBE) emissions at 3.38 eV and donor-acceptor-pair (DAP) transition at 3.2 eV with a typical strong broad yellow emission were observed in photoluminescence spectra for GaN buffer. In contrast, the yellow emission was completely quenched in GaCuN film because Ga vacancies causing the observed yellow emission in undoped GaN were substituted by Cu atoms. In addition, GaCuN film exhibits a blue shift of NBE emission, which could be explained with the +2 oxidation state of Cu ions, replacing +3 Ga ions resulting in band gap increment. The valance sate of Cu in GaCuN film was also confirmed by x-ray photoelectron spectroscopy (XPS) analysis. The GaCuN film shows ferromagnetic ordering and possesses a residual magnetization of 0.12 emu/cm3 and a coercive field of 264 Oe at room temperature. The unpaired spins in Cu2+ ions (d9) are most likely to be responsible for the observed ferromagnetism in GaCuN.