Low-frequency Raman scattering in WSe$_2$-MoSe$_2$ heterobilayers: Evidence for atomic reconstruction

We investigate WSe$_2$-MoSe$_2$ heterobilayers with different twist angles $θ\pm δ$ between the two layers, by low-frequency Raman scattering. In sufficiently aligned samples with $θ=0^\circ$, or $θ=60^\circ$, and $δ\lesssim 3^\circ$, we observe an interlayer shear mode (ISM), which is a clear sign of a commensurate bilayer structure, i.e., the layers must undergo an atomic reconstruction to form R-type or H-type stacking orders. We find slightly different ISM energies of about 18~cm$^{-1}$ and 17~cm$^{-1}$ for H-type and R-type reconstructions, respectively, independent of the exact value of $θ\pm δ$. Our findings are corroborated by the fact that the ISM is not observed in samples with twist angles, which deviate by $δ> 3^\circ$ from $0^\circ$ or $60^\circ$. This is expected, since in such incommensurate structures, with the possibility of Moir$\acute{\text{e}}$-lattice formation, there is no restoring force for an ISM. Furthermore, we observe the ISM even in sufficiently aligned heterobilayers, which are encapsulated in hexagonal Boron nitride. This is particularly relevant for the characterization of high-quality heterostructure devices.

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