Magnetism and magnetocrystalline anisotropy in vacancy doped and (non)metal adsorbed single-layer PtSe2

Abstract

The single-layer (1L) transition-metal dichalcogenides (TMDs) have attracted great attentions over the past years. However, most of previous work focus on the Mo(W) TMDs and the pristine 1L-TMDs are often diamagnetic. Recent experimental progress has sparked renewed interest in Pt(Pd) TMDs. Here, using first-principles calculations, we study the functionalization of the newly synthesized 1L-PtSe2 through adatom adsorption and vacancy defect creation. It is found the 1L-PtSe2 with Pt vacancy (VPt) has large magnetocrystalline anisotropy energy (30.4meV/VPt), which is comparable with that of IrCo dimer adsorbed graphene. Except for the magnetism induced by the magnetic Fe(Co) adatom, the metal-free magnetism is introduced by the B(F) adatom, and the 1L-PtSe2 shows stronger adsorption capability to nonmetal atoms (H, B, C, N, F) than that of the 1L-MoS2(1L-MoSe2). In contrast to the case of 1L-MoS2(1L-MoSe2), significant reconstructions of surfaces are found for the H, B, C and N adsorbed 1L-PtSe2. Moreover, the semiconducting behaviors and spintronic features are modified: Fe(N) adatom causes n(p)-type doping, F adsorbed 1L-PtSe2 becomes bipolar semiconductor.