LAUSR

Abstract Understanding the source of magnetism in Mn doped ZnO (ZnO:Mn) is an active area of research, made difficult experimentally by the challenge of controlling point vacancies in ZnO:Mn. Therefore, the stability and magnetic properties of ZnO:Mn with point vacancies were studied by first-principles calculations based on density functional theory (DFT). Formation energy and magnetic moment calculation results show that Mn prefers to cluster in ZnO:Mn. This clustering can become uniformly distributed through modifications by Zn vacancies (VZn) or O vacancies (Vo). Magnetic analysis shows that Mn dopant in Zn site (ZnO:MnZn) coupled with VZn or interstitial Mn (Mni) coupled with VO makes ZnO having long-range ordered ferromagnetism (FM) and an increased Curie temperature (Tc) above room-temperature. The ZnO:MnZn with VZn exhibits obvious half-metallic characteristics that are of essential benefit to the design and preparation of a new-type of spin-electron injection source dilute magnetic semiconductor. The magnetic sources of ZnO:MnZn with VZn and Mni-doped ZnO (ZnO:Mni) with VO arise from carrier-mediated magnetic interaction and the double exchange of Mn3d, O2p and Zn4s orbitals, consistent with the theories of average field approximation and the double exchange mechanism.