Effects of Transition Metal (TM = V, Cr, Mn, Fe, Co, and Ni) Elements on Magnetic Mechanism of LiZnP with Decoupled Charge and Spin Doping

The electronic structure and magnetism of a series of 111-type diluted magnetic semiconductors Li(Zn,TM)P (TM = V, Cr, Mn, Fe, Co, and Ni) are investigated on the basis of density functional theory. Our results indicate that V-, Cr-, Mn-, and Fe-doped LiZnP are magnetic while Co- and Ni-doped LiZnP systems show no magnetisms. But all TM-doped LiZnP systems prefer antiferromagnetic behavior by magnetic coupling calculations. In contrast, V/Li- and Cr/Li-codoped LiZnP prefer ferromagnetic ordering, and Mn/Li-, Fe/Li- and Co/Li-codoped LiZnP display antiferromagnetic spin ordering. Hence, Li dopant is very vital for the ferromagnetic formation of Li(Zn,TM)P materials. It is revealed that the magnetic moments come mainly from the TM 3d orbitals. The ferromagnetic coupling between the TM atoms is explained by through-bond spin polarization. Our work demonstrates that the magnetic properties of Li(Zn,TM)P can be mediated by doping different TM atoms. These results may provide theoretical guidance for further experimental research on DMS.