Inducing feature-rich electronic and magnetic properties in PtSe2 monolayer via doping with TMXn clusters (TM = Mn and Fe; X = N and P; n=3 and 6): A first-principles study

In this work, doping with TMXn n (TM = Mn and Fe; X = N and P, n = 3 and 6) clusters is proposed to modify the electronic and magnetic properties of PtSe2 2 monolayer. Pristine PtSe2 2 monolayer is a non-magnetic two-dimensional (2D) semiconductor material with indirect band gap of 1.40(2.01) eV obtained from PBE (HSE06)-based calculations. PtSe3-type 3-type multivacancies lead to the monolayer magnetization with total magnetic moment of 0.54 mu B , where Pt and Se atoms around defect sites produce mainly the system magnetism. In contrast, no magnetism is induced by PtSe6-type 6-type multivacancies. The substitutional incorporation of TMXn n clusters magnetizes significantly PtSe2 2 monolayer, where both TM and X atoms originate mainly the magnetic properties. Depending on the spin orientation in the clusters, total magnetic moments between 0.00 and 8.00 mu B B are obtained. All the doped D TMX n systems exhibit strong spin polarization around the Fermi level, which is derived mainly from the outermost TM-3d, d , N-2p, p , and P-3p p orbitals. Consequently, either half-metallicity or magnetic semiconductor behavior can be induced, depending on the nature of TMXn n cluster. Further, the Bader analysis indicates that TMNn n clusters act as charge gainers due to the more electronegative nature of N atoms in comparison with Se atoms, meanwhile TMPn n clusters transfer charge to the host PtSe2 2 monolayer. Our study may introduce the cluster doping in PtSe2 2 monolayer as efficient method to create new highly spin-polarized 2D materials towards spintronic applications.