Pressure Tuning of Layer-hybridized Excitons in Trilayer WSe2

We demonstrate dynamic pressure tuning (0-6.6 GPa) of layer-hybridized excitons in AB-stacked trilayer WSe₂ via diamond-anvil-cell-integrated reflectance spectroscopy. Pressure-controlled interlayer coupling manifests in enhanced energy-level anti-crossings and oscillator strength redistribution, with Stark shift analysis revealing a characteristic dipole moment reduction of 11%. Notably, the hybridization strength between the intra- and interlayer excitons triples from ~10 meV to above ~30 meV, exhibiting a near-linear scaling of 3.5±0.2 meV/GPa. Spectral density simulations resolve four distinct components, i.e., intralayer ground/excited and interlayer ground/excited excitons, with their relative weights transitioning from one component dominant to strongly hybridized at higher pressures. Our findings highlight the potential for controlling excitonic properties and engineering novel optoelectronic devices through interlayer compression.