Tailoring MoS₂ Valley-Polarized Photoluminescence with Super Chiral Near-Field.

Abstract

Transition metal dichalcogenides with intrinsic spin-valley degrees of freedom hold great potentials for applications in spintronic and valleytronic devices. MoS₂ monolayer possesses two inequivalent valleys in the Brillouin zone, with each valley coupling selectively with circularly polarized photons. The degree of valley polarization (DVP) is a parameter to characterize the purity of valley-polarized photoluminescence (PL) of MoS₂ monolayer. Usually, the detected values of DVP in MoS₂ monolayer show achiral property under optical excitation of opposite helicities due to reciprocal phonon-assisted intervalley scattering process. Here, it is reported that valley-polarized PL of MoS₂ can be tailored through near-field interaction with plasmonic chiral metasurface. The resonant field of the chiral metasurface couples with valley-polarized excitons, and tailors the measured PL spectra in the far-field, resulting in observation of chiral DVP of MoS₂ -metasurface under opposite helicities excitations. Valley-contrast PL in the chiral heterostructure is also observed when illuminated by linearly polarized light. The manipulation of valley-polarized PL in 2D materials using chiral metasurface represents a viable route toward valley-polaritonic devices.