Unexpected strong magnetism of Cu doped single-layer MoS₂ and its origin

The magnetism of the 3d transition-metal (TM) doped single-layer (1L) MoS2, where the Mo atom is partially replaced by the 3d TM atom, is investigated using the first-principles density functional calculations. In a series of 3d TM doped 1L-MoS2's, the induced spin polarizations are negligible for Sc, Ti, and Cr dopings, while the induced spin polarizations are confirmed for V, Mn, Fe, Co, Ni, Cu, and Zn dopings and the systems become magnetic. Especially, the Cu doped system shows unexpectedly strong magnetism although Cu is nonmagnetic in its bulk state. The driving force is found to be a strong hybridization between Cu 3d states and 3p states of neighboring S, which results in an extreme unbalanced spin-population in the spin-split impurity bands near the Fermi level. Finally, we also discuss further issues of the Cu induced magnetism of 1L-MoS2 such as investigation of additional charge states, the Cu doping at the S site instead of the Mo site, and the Cu adatom on the layer (i.e., 1L-MoS2).