Enhancement of Room-Temperature Photoluminescence and Valley Polarization of Monolayer and Bilayer WS₂ via Chiral Plasmonic Coupling

Transition-metal dichalcogenides with intrinsic spin-valley degree of freedom have enabled great potentials for valleytronic and optoelectronic applications. However, the degree of valley polarization is usually low under nonresonant excitation at room temperature due to the phonon-assisted intervalley scattering. Here, achiral and chiral Au arrays are designed to enhance the optical response and valley polarization in monolayer and bilayer WS2. A considerable band edge emission with 7 times increment is realized under the resonant coupling with Au dimer-prism arrays. Valley polarization enhancement is quantitatively predicted by the inherent mechanisms from elevated electromagnetic field intensity and radiation efficiency and further realized in polarized photoluminescence. A tunable valley polarization up to 30.0% is achieved in bilayer WS2 under a nonresonant excitation at room temperature. All of these results provide a promising route toward the development of room-temperature valley-dependent optoelectronic devices.