Large-Scale Mapping of Moiré Superlattices by Hyperspectral Raman Imaging

Moiré superlattices can induce correlated-electronic phases in twisted van der Waals materials: strongly correlated quantum phenomena emerge, such as superconductivity and the Mott-insulating state. However, moiré superlattices produced through artificial stacking can be quite inhomogeneous, which hampers the development of a clear correlation between the moiré period and the emerging electrical and optical properties. Here, it is demonstrated in twisted-bilayer transition-metal dichalcogenides that low-frequency Raman scattering can be utilized not only to detect atomic reconstruction, but also to map out the inhomogeneity of the moiré lattice over large areas. The method is established based on the finding that both the interlayer-breathing mode and moiré phonons are highly susceptible to the moiré period and provide characteristic fingerprints. Hyperspectral Raman imaging visualizes microscopic domains of a 5° twisted-bilayer sample with an effective twist-angle resolution of about 0.1°. This ambient methodology can be conveniently implemented to characterize and preselect high-quality areas of samples for subsequent device fabrication, and for transport and optical experiments.