Modulation of Phonons and Excitons Due to Moiré Potentials in Twisted Bilayer of WSe₂/MoSe₂

The application of two-dimensional materials has been expanded by introducing the twisted bilayer (TBL) system. However, the landscape of the interlayer interaction in hetero-TBLs has not yet been fully understood, while that in homo-TBLs has been extensively studied, with the dependence on the twist angle between the constituent layers. Here, we present detailed analyses on the interlayer interaction that depends on the twist angle in WSe 2 /MoSe 2 hetero-TBL via Raman and photoluminescence studies combined with first-principles calculation. We observe interlayer vibrational modes, moiré phonons, and the interlayer excitonic states that evolve with the twist angle and identify different regimes with distinct characteristics of such features. Moreover, the interlayer excitons that appear strong in the hetero-TBLs with twist angles near 0° or 60° have different energies and photoluminescence excitation spectra for the two cases, which results from different electronic structures and carrier relaxation dynamics. These results would enable a better understanding of the interlayer interaction in hetero-TBLs.