Beyond-Grain-Boundary Growth of Twisted Bilayer MoS2

with a twist angle of 3.4°, Moiré superlattices with a periodicity of 5.45 nm were observed. Systematic Raman and photoluminescence (PL) studies revealed significant twist-angle-dependent effects on the phonon and exciton properties. This unique growth behavior is attributed to edge structure modifications induced by an increased sulfur chemical potential. These results demonstrate an approach to synthesizing high-quality twisted 2D materials, contributing to progress in twistronics and quantum device applications.