Molten glass-mediated conditional CVD growth of MoS₂ monolayers and effect of surface treatment on their optical properties

Abstract In the rapidly developing field of optoelectronics, the utilization of transition-metal dichalcogenides with adjustable band gaps holds great promise. MoS₂, in particular, has garnered considerable attention owing to its versatility. However, a persistent challenge is to establish a simple, reliable and scalable method for large-scale synthesis of continuous monolayer films. In this study, we report the growth of continuous large-area monolayer MoS₂ films using a glass-assisted chemical vapor deposition (CVD) process. High-quality monolayer films were achieved by precisely controlling carrier gas flow and sulfur vaporization with a customized CVD system. Additionally, we explored the impact of chemical treatment using lithium bistrifluoromethylsulfonylamine (Li-TFSI) salt on the optical properties of monolayer MoS₂ crystals. To investigate the evolution of excitonic characteristics, we conditionally grew monolayer MoS₂ flakes by controlling sulfur evaporation. We reported two scenarios on MoS₂ films and flakes based on substrate-related strain and defect density. Our findings revealed that high-quality monolayer MoS₂ films exhibited lower treatment efficiency due to substrate-induced surface strain. whereas defective monolayer MoS₂ flakes demonstrated a higher treatment sensitivity due to the p-doping effect. The Li-TFSI-induced changes in exciton density were elucidated through photoluminescence, Raman, and x-ray photoelectron spectroscopy results. Furthermore, we demonstrated treatment-related healing in flakes under variable laser excitation power. The advancements highlighted in our study carry significant implications for the scalable fabrication of diverse optoelectronic devices, potentially paving the way for widespread real-world applications.