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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.

We report about the investigation of twisted MoSe2 homo- and MoSe2–WSe2 heterobilayers by means of low-frequency Raman spectroscopy (LFRS) and low-temperature micro photoluminescence (µPL). In room-temperature LFRS experiments on both, twisted MoSe2 homobilayers and twisted MoSe2–WSe2 heterobilayers, we observe moiré phonons, i.e. folded acoustic phonon modes due to the moiré superlattice. In the heterobilayers, we can identify moiré phonons of both materials, MoSe2 and WSe2. While the twist angles for the homobilayers are relatively precisely known from the applied tear-and-stack preparation method, the twist angles of the heterobilayers have to be determined via second-harmonic-generation microscopy on monolayer regions of the samples, which has significant uncertainties. We show that by the moiré phonons of the heterobilayers, the relative twist angles can be determined on a local scale with much higher precision. We apply our technique for the investigation of a large area H-type (twist angle θ = 60∘ + δ) MoSe2–WSe2 heterobilayer. These investigations show that spatial regions, which can be identified to be atomically reconstructed (i.e. δ = 0∘) by the observation of an interlayer shear mode in LFRS experiments, exhibit a strong, momentum-allowed interlayer-exciton signal in low-temperature µPL. On the contrary, regions, where moiré phonons are observed, i.e. which can be identified to be rigidly twisted by a misalignment angle in the range of 5 ° ≲ | δ | ≲ 6 ° , exhibit no significant interlayer-exciton signals.

We report about the investigation of twisted MoSe2 homo- and MoSe2–WSe2 heterobilayers by means of low-frequency Raman spectroscopy (LFRS) and low-temperature micro photoluminescence (µPL). In room-temperature LFRS experiments on both, twisted MoSe2 homobilayers and twisted MoSe2–WSe2 heterobilayers, we observe moiré phonons, i.e. folded acoustic phonon modes due to the moiré superlattice. In the heterobilayers, we can identify moiré phonons of both materials, MoSe2 and WSe2. While the twist angles for the homobilayers are relatively precisely known from the applied tear-and-stack preparation method, the twist angles of the heterobilayers have to be determined via second-harmonic-generation microscopy on monolayer regions of the samples, which has significant uncertainties. We show that by the moiré phonons of the heterobilayers, the relative twist angles can be determined on a local scale with much higher precision. We apply our technique for the investigation of a large area H-type (twist angle θ = 60∘ + δ) MoSe2–WSe2 heterobilayer. These investigations show that spatial regions, which can be identified to be atomically reconstructed (i.e. δ = 0∘) by the observation of an interlayer shear mode in LFRS experiments, exhibit a strong, momentum-allowed interlayer-exciton signal in low-temperature µPL. On the contrary, regions, where moiré phonons are observed, i.e. which can be identified to be rigidly twisted by a misalignment angle in the range of 5°≲|δ|≲6° , exhibit no significant interlayer-exciton signals.