Nucleation and Growth of Monolayer MoS₂ at Multisteps of MoO₂ Crystals by Sulfurization

Two-dimensional (2D) materials and their heterostructures are promising for next-generation optoelectronics, spintronics, valleytronics, and electronics. Despite recent progress in various growth studies of 2D materials, mechanical exfoliation of flakes is still the most common method to obtain high-quality 2D materials because precisely controlling material growth and synthesizing a single domain during the growth process of 2D materials, for the desired shape and quality, is challenging. Here, we report the nucleation and growth behaviors of monolayer MoS₂ by sulfurizing a faceted monoclinic MoO₂ crystal. The MoS₂ layers nucleated at the thickness steps of the MoO₂ crystal and grew epitaxially with crystalline correlation to the MoO₂ surface. The epitaxially grown MoS₂ layer expands outwardly on the SiO₂ substrate, resulting in a monolayer single-crystal film, despite multiple nucleations of MoS₂ layers on the MoO₂ surface owing to several thickness steps. Although the photoluminescence of MoS₂ is quenched owing to efficient charge transfer between MoS₂ and metallic MoO₂, the MoS₂ stretched out to the SiO₂ substrate shows a high carrier mobility of (15 cm² V^-1 s^-1), indicating that a high-quality monolayer MoS₂ film can be grown using the MoO₂ crystal as a seed and precursor. Our work shows a method to grow high-quality MoS₂ using a faceted MoO₂ crystal and provides a deeper understanding of the nucleation and growth of 2D materials on a step-like surface.