Excitonic Complexes and Emerging Interlayer Electron–Phonon Coupling in BN Encapsulated Monolayer Semiconductor Alloy: WS_0.6Se_1.4

Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. Although WS₂ and WSe₂ are known for their excellent valley polarization due to the strong spin–orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS_2xSe_2(1–x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN encapsulated monolayer WS_0.6Se_1.4 inherits the superior optical properties of tungsten-based TMDs, including a trion splitting of ∼6 meV and valley polarization as high as ∼60%. In particular, we demonstrate for the first time the emerging and gate-tunable interlayer electron–phonon coupling in the BN/WS_0.6Se_1.4/BN van der Waals heterostructure, which renders the otherwise optically silent Raman modes visible. In addition, the emerging Raman signals can be drastically enhanced by the resonant coupling to the 2s state of the monolayer WS_0.6Se_1.4 A exciton. The BN/WS_2xSe_2(1–x)/BN van der Waals heterostructure with a tunable bandgap thus provides an exciting platform for exploring the valley degree of freedom and emerging excitonic physics in two-dimension.