Concentration Phase Separation of Substitution‐Doped Atoms in TMDCs Monolayer

Abstract The density and spatial distribution of substituted dopants affect the transition metal dichalcogenides (TMDCs) materials properties. Previous studies have demonstrated that the density of dopants in TMDCs increases with the amount of doping, and the phenomenon of doping concentration difference between the nucleation center and the edge is observed, but the spatial distribution law of doping atoms has not been carefully studied. Here, it is demonstrated that the spatial distribution of dopants changes at high doping concentrations. The spontaneous formation of an interface with a steep doping concentration change is named concentration phase separation (CPS). The difference in the spatial distribution of dopants on both sides of the interface can be identified by an optical microscope. This is consistent with the results of spectral analysis and microstructure characterization of scanning transmission electron microscope. According to the calculation results of density functional theory, the chemical potential has two relatively stable energies as the doping concentration increases, which leads to the spontaneous formation of CPS. Understanding the abnormal phenomena is important for the design of TMDCs devices. This work has great significance in the establishment and improvement of the doping theory and the design of the doping process for 2D materials.