Monolayer MoS2 has emerged as one of the most promising candidate materials for future semiconductor devices because of its fascinating physical properties and optoelectronic performance. Recently, the utilization of alkali metal compounds as promoters in CVD growth has been demonstrated to be a facile strategy for growing monolayer MoS2 and other 2D TMDs with large domain sizes. In this work, we systematically investigated the residues derived from alkali metal compounds and the spontaneous n-doping effect on monolayer MoS2 in alkali metal compound-promoted CVD growth. When using NaOH and other alkali metal compounds as promoters, it is found that the Raman peak of the A1g mode red shifted with a broadening width and the PL intensity of the A peak decreased with a red shift, which was attributed to the spontaneous n-doping effect during growth. Moreover, the growth using varying amounts of NaOH promoter suggests that the n-doping level could be controlled by the amount of promoter. X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary-ion mass spectroscopy (TOF-SIMS) showed the existence of cation-derived residues in the form of a Na-O cluster physiosorbed on top of monolayer MoS2, which was also confirmed by the transfer experiment. The NaOH treatment experiment and density functional theory (DFT) calculations demonstrate that sodium hydroxide clusters, which could be converted from a combination of Na-O clusters and water vapor, could produce an n-doping effect on monolayer MoS2. This study provides a facile route to controllably grow monolayer 2D materials with a desired doping level without further treatment.
Keywords: CVD growth; alkali metal compounds; density functional theory; monolayer molybdenum disulfide; spontaneous n-doping.