Scalable Moiré Lattice with Oriented TMD Monolayers

Moiré lattice in artificially stacked monolayers of two-dimensional (2D) materials effectively modulates the electronic structures of materials, which is widely highlighted. Formation of the electronic Moiré superlattice promises the prospect of uniformity among different moiré cells across the lattice, enabling a new platform for novel properties, such as unconventional superconductivity, and scalable quantum emitters. Recently, epitaxial growth of the monolayer transition metal dichalcogenide (TMD) is achieved on the sapphire substrate by chemical vapor deposition (CVD) to realize scalable growth of highly-oriented monolayers. However, fabrication of the scalable Moiré lattice remains challenging due to the lack of essential manipulation of the well-aligned monolayers for clean interface quality and precise twisting angle control. Here, scalable and highly-oriented monolayers of TMD are realized on the sapphire substrates by using the customized CVD process. Controlled growth of the epitaxial monolayers is achieved by promoting the rotation of the nuclei-like domains in the initial growth stage, enabling aligned domains for further grain growth in the steady-state stage. A full coverage and distribution of the highly-oriented domains are verified by second-harmonic generation (SHG) microscopy. By developing the method for clean monolayer manipulation, hetero-stacked bilayer (epi-WS₂/epi-MoS₂) is fabricated with the specific angular alignment of the two major oriented monolayers at the edge direction of 0°/ ± 60°. On account of the optimization for scalable Moiré lattice with a high-quality interface, the observation of interlayer exciton at low temperature illustrates the feasibility of scalable Moiré superlattice based on the oriented monolayers.