Pressure-Enhanced Interlayer Coupling and Hybridized Excitons in Twisted MoS₂ Moiré Quasicrystals

Moiré quasicrystals, characterized by broken translational symmetry, emerge in van der Waals (vdW) bilayers twisted 30°, resulting in unique interlayer coupling. Despite their intriguing properties, the modulation of interlayer interactions and its impact on the electronic and phononic behavior of moiré quasicrystals remain underexplored. Here, we synthesize 30° twisted MoS₂ bilayers and employ diamond anvil cell (DAC) technology to dynamically tune their moiré phonons and excitons. Enhanced interlayer coupling under pressure strengthens the moiré potential, shifting the moiré phonon away from pristine Raman modes. Furthermore, the broken translational symmetry in moiré quasicrystals facilitates intervalley coupling via Umklapp scattering, leading to hybridized interlayer excitons. These hybridized excitons induce a nonmonotonic shift in the photoluminescence peak under pressure, due to the mixing of intralayer and interlayer exciton states. Our findings offer new insights into the physics of moiré quasicrystals and demonstrate high-pressure modulation as a powerful tool for probing and controlling their physical properties.