Nitrogen Pretreatment of Growth Substrates for Vacancy-Saturated MoS₂

Two-dimensional transition-metal dichalcogenides (2D TMDCs) are considered promising materials for optoelectronics due to their unique optical and electric properties. However, their potential has been limited by the occurrence of atomic vacancies during synthesis. While post-treatment processes have demonstrated the passivation of such vacancies, they increase process complexity and affect the TMDC's quality. We here introduce the concept of pretreatment as a facile and powerful route to solve the problem of vacancies in MoS₂. Low-temperature nitridation of the sapphire substrate prior to growth provides a nondestructive method to MoS₂ modification without introducing new processing steps or increasing the thermal budget. Spectroscopic characterization and atomic-resolution microscopy reveal the incorporation of nitrogen from the sapphire surface layer into chalcogen vacancies. The resulting MoS₂ with nitrogen-saturated defects shows a decrease in midgap states and more intrinsic doping as confirmed by ab initio calculations and optoelectronic measurements. The demonstrated pretreatment method opens up new routes toward future, high-performance 2D electronics, as evidenced by a 3-fold reduction in contact resistance and a 10-fold improved performance of 2D photodetectors.