Twist Angle-Dependent Phonon Hybridization in WSe₂/WSe₂ Homobilayer

The emerging moiré superstructure of twisted transition metal dichalcogenides (TMDs) leads to various correlated electronic and optical properties compared to those of twisted bilayer graphene. In such a versatile architecture, phonons can also be renormalized and evolve due to atomic reconstruction, which, in turn, depends on the twist angle. However, observing this reconstruction and its relationship to phonon behavior with conventional, cost-effective imaging methods remains challenging. Here, we used noninvasive Raman spectroscopy on twisted WSe₂/WSe₂ (t-WSe₂) homobilayers to examine the evolution of phonon modes due to interlayer coupling and atomic reconstruction. Unlike in the natural bilayer (NB), ∼0° as well as ∼60° t-WSe₂ samples, the nearly degenerate A_1g/E_2g mode in the twisted samples (1-7°) split into a doublet in addition to the nondegenerate B_2g mode, and the maximum splitting is observed around 2-3°. Our detailed theoretical calculations qualitatively capture the splitting and its dependence as a function of the twist angle and highlight the role of the moiré potential in phonon hybridization. Additionally, we found that around the 2° twist angle, the anharmonic phonon-phonon interaction is higher than the natural bilayer and decreases for larger twist angles. Interestingly, we observed anomalous Raman frequency softening and line-width increase with the decreasing temperature below 50 K, pointing to the combined effect of enhanced electron-phonon coupling and cubic anharmonic interactions in moiré superlattice.