Well-Hidden Grain Boundary in the Monolayer MoS₂ Formed by a Two-Dimensional Core-Shell Growth Mode

Guided by the hexagonal lattice symmetry, triangles and hexagons are the most basic morphological units for two-dimensional (2D) transition metal dichalcogenides (TMDs) synthesized by chemical vapor deposition (CVD). Also, it is widely acknowledged that these units start from the single nucleation site and then grow epitaxially. Accordingly, the triangular monolayer (ML) samples are generally considered as single crystals. Here, we report a 2D core-shell growth mode in the CVD process for ML-MoS₂, which leads to one kind of "pseudo" single-crystal triangles containing triangular outline grain boundaries (TO-GBs). It is difficult to be optically distinguished from the "true" single-crystal triangles. The weakening of Raman peaks and the remarkable enhancement of photoluminescence (PL) are found at the built-in TO-GBs, which could be useful for high-performance optoelectronics. In addition, the electrical measurements indicate that the TO-GBs are conductive. Furthermore, TO-GBs and the common grain boundaries (CO-GBs) can coexist in a single flake, whereas their optical visibility and optical modifications (Raman and PL) are quite different. This work is helpful in further understanding the growth mechanism of 2D TMD materials and may also play a significant role in related nanodevices.