Valleytronics in transition metal dichalcogenides has been intensively investigated for potential applications in next-generation information storage, data processing, and signal transmission devices. Here a ferroelectric gating approach is engaged in achieving nonvolatile electrical tuning of the valley-excitonic properties of monolayer and bilayer WS2. The gating effects include carrier doping and ferroelectric coupling, which are further distinguished by comparing two geometries where the gate electrodes are in direct contact with or insulated from the WS2 crystal. The results show that the carrier doping from gate electrodes acts on WS2 through carrier screening, which only moderately alters the valley polarization. In contrast, the ferroelectric gating promotes electron-phonon interaction, introduces a strong surface polarization field, and controls the interfacial charge trapping/detrapping, causing a Stark shift in exciton energy and strongly enhancing room-temperature valley polarization. In bilayer WS2, the intralayer-interlayer exciton transition is further induced, contributing to even higher valley polarization. The ferroelectric coupling effect can still be maintained after the removal of gate voltage, showing its nonvolatile nature. The role of ferroelectricity is further verified by the anomalous temperature dependence in valley polarization. This work has revealed effective electrical control over valley excitons in semiconductors through interaction with ferroelectric materials. The reported high room-temperature valley polarization in WS2 will boost the development of valleytronics devices.
Keywords: excitons; ferroelectricity; photoluminescence; tungsten disulfide; valley polarization.