Enhancement of the hole-induced d0-ferromagnetism in ZnO through compensated donor–acceptor complexes: a first-principles study

Abstract

The presence of spontaneous magnetization in transparent conducting oxides with sufficient holes is an intrinsic property of the wide-band-gap semiconductors. In this paper, to enhance the hole-induced d0-ferromagnetism of transparent conducting oxides, we choose ZnO as a prototype material and study the hole-induced d0-ferromagnetism in ZnO by first-principles methods. Our calculations show that the hole-induced d0-ferromagnetism is limited by the spontaneous formation of intrinsic cation vacancies or extrinsic acceptor doping. To solve this problem, we propose an effective passivated codoping approach to reduce the formation energies of the acceptors by doping the host with passive donor–acceptor complexes. It is demonstrated that the formation energies and polarization energies of VZn or NO in ZnO can be reduced significantly by doping GaZn+NO complexes, while leaving the magnetic moment in these supercells almost unchanged, which finally improve hole-induced d0-ferromagnetism in the host. In principle, the suggested approach to enhance the hole-induced d0-ferromagnetism can also be applied to other transparent conducting oxides.