Valley-Selective Optical Stark Effect in Monolayer WS2

Abstract

Breaking space-time symmetries in two-dimensional crystals (2D) can dramatically influence their macroscopic electronic properties. Monolayer transition metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations [1–4], even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applications. While applying a magnetic field should in principle accomplish this task, experiments to date have observed no valley-selective energy level shifts in fields accessible in the laboratory. Here we show the first direct evidence of lifted valley degeneracy in the monolayer TMD WS2 [5]. By applying intense circularly polarized light, which breaks time-reversal symmetry, we demonstrate that the exciton level in each valley can be selectively tuned by as much as 18 meV via the optical Stark effect. These results offer a novel way to control valley degree of freedom and may provide a means to realize new valley-selective Floquet topological phases [6–8] in 2D TMDs.