Synergistic Effect of Chiral Metasurface and Hot Carrier Injection Enabling Manipulation of Valley Polarization of WSe2 at Room Temperature

Abstract The unique band structure of monolayer transition metal dichalcogenides (TMDC) provides an important platform for spintronic and valleytronic devices. Various approaches, such as in‐plane electric field and out‐of‐plane magnetic field, have been proposed to actively control the valley polarization. In this work, we propose a synergistic effect involving chiral near‐field interactions and hot carrier injection to actively control the valley polarization emission of WSe2 at room temperature (RT). The degree of valley polarization is enhanced from near zero (for pure WSe2) to 20% under non‐resonant optical excitation (532 nm) when monolayer WSe2 is coupled with the chiral near field of plasmonic metasurface. More importantly, the application of near‐infrared light (wavelength of 970 to 1600 nm) illumination further enhances the valley polarization from 20% to 30%, which is attributed to plasmonic‐induced hot carrier injection from the metasurface to WSe2. The synergistic effect of the chiral near field and infrared light pumping offers another strategy to manipulate the valley polarization emission in monolayer TMDs at room temperature, paving the way for future applications of opto‐valleytronic/spintronic devices based on these 2D materials.