Correlatively Dependent Lattice and Electronic Structural Evolutions in Compressed Monolayer Tungsten Disulfide

Transition-metal dichalcogenides (TMDs) are promising materials for optoelectronic devices. Their lattice and electronic structural evolutions under high strain conditions and their relations remain open questions. We exert pressure on WS₂ monolayers on different substrates, namely, Si/SiO₂ substrate and diamond anvil surface up to ∼25 GPa. Structural distortions in various degree are disclosed based on the emergence of Raman-inactive B mode. Splits of out-of-plane B and A₁′ modes are only observed on Si/SiO₂ substrate due to extra strain imported from volume decrease in Si and corrugation of SiO₂ surface, and its photoluminescence (PL) quenches quickly because of decreased K–K transition by conspicuous distortion of Brillouin zone. While diamond anvil surface provides better hydrostatic environment, combined analysis of PL and absorption proves that pressure effectively tunes PL emission energy and enhances Coulomb interactions. Knowledge of these distinct pressure tunable characteristics of monolayer WS₂ improves further understanding of structural and optical properties of TMDs.