Monolayer MoS₂ with S vacancy defects doped with Group V non-metallic elements (N, P, As): a first-principles study

This study systematically investigated the effects of single S-atom vacancy defects and composite defects (vacancy combined with doping) on the properties of MoS₂ using density functional theory. The results revealed that N-doped S-vacancy MoS₂ has the smallest composite defect formation energy, indicating its highest stability. Doping maintained the direct band gap characteristic, with shifts in the valence band top. The Fermi level slightly shifted down in N- and P-doped systems, with N-doped MoS₂ showing a larger increase in valence band top energy. Doping also significantly altered the density of states at the Fermi level and weakened the dielectric properties of MoS₂. The maximum dielectric peaks of doped systems appeared near 2.7 eV with reduced intensities and red-shifted energies. Optical properties were significantly changed, with decreased reflectance, narrower reflectance spectra, and blue-shifted absorption spectra. These findings suggest that introducing composite defects can effectively reduce the forbidden bandwidth of MoS₂, enhancing electrical conductivity. This research provides theoretical guidance for novel material design and offers insights into composite defect behavior in other two-dimensional materials.

The Materials-Studio CASTEP module was used to calculate density functional theory (DFT). A plane wave ultrasoft pseudopotential is used to optimize the crystal structure, and the generalized gradient approximation (GGA) in the form of Perdew-Burke-Ernzerhof (PBE) is used to characterize the exchange correlation energy. After the convergence test, the truncation energy and dot settings were finally selected to be 450 eV and 3 × 3 × 1, respectively, the convergence accuracy was set to 1.0e-5eV/atom, and the convergence criterion for the interatomic interaction force was 0.02 eV/Å. The parameters were all at or better than the accuracy settings. The vacuum layer between the layers was set to 18 Å to avoid interactions caused by the periodic calculation method.