Abstract
In this work, defect engineering and doping are proposed to effectively functionalize a germanium sulfide (GeS) mononolayer. With a buckled hexagonal structure, the good dynamical and thermal stability of the GeS monolayer is confirmed. PBE(HSE06)-based calculations assert the indirect gap semiconductor nature of this two-dimensional (2D) material with a relatively large band gap of 2.48(3.28) eV. The creation of a single Ge vacancy magnetizes the monolayer with a total magnetic moment of 1.99 μ(B), creating a the feature-rich half-metallic nature. Va(S) vacancy, Va(GeS) divacancy, S(Ge) and Ge(S) antisites preserve the non-magnetic nature; however, they induce considerable band gap reduction of the order 47.98%, 89.11%, 29.84%, and 62.5%, respectively. By doping with transition metals (TMs), large total magnetic moments of 3.00, 4.00, and 5.00 μ(B) are obtained with V, Cr-Fe, and Mn impurities, respectively. The 3d orbital of TM dopants mainly regulates the electronic and magnetic properties, which induces either the half-metallic or diluted magnetic semiconductor nature. It is found that the doping site plays a determinant role in the case of doping with VA-group atoms (P and As). The GeS monolayer can be metallized by doping the Ge sublattice, meanwhile both spin states exhibit semiconductor character with strong spin polarization upon doping the S sublattice to obtain a diluted magnetic semiconductor nature with a total magnetic moment of 1.00 μ(B). In these cases, the magnetism originates mainly from P and As impurities. The obtained results suggest an efficient approach to functionalize the GeS monolayer for optoelectronic and spintronic applications.