Pressure Dependence of Intra- and Interlayer Excitons in 2H-MoS₂ Bilayers

The optical and electronic properties of multilayer transition metal dichalcogenides differ significantly from their monolayer counterparts due to interlayer interactions. The separation of individual layers can be tuned in a controlled way by applying pressure. Here, we use a diamond anvil cell to compress bilayers of 2H-MoS₂ in the gigapascal range. By measuring optical transmission spectra, we find that increasing pressure leads to a decrease in the energy splitting between the A and the interlayer exciton. Comparing our experimental findings with ab initio calculations, we conclude that the observed changes are not due to the commonly assumed hydrostatic compression. This effect is attributed to the MoS₂ bilayer adhering to the diamond, which reduces the in-plane compression. Moreover, we demonstrate that the distinct real-space distributions and resulting contributions from the valence band account for the different pressure dependencies of the inter- and intralayer excitons in compressed MoS₂ bilayers.