Optical control of the valley Zeeman effect through many-exciton interactions

Charge carriers in two-dimensional transition metal dichalcogenides (TMDs), such as WSe₂, have their spin and valley-pseudospin locked into an optically addressable index that is proposed as a basis for future information processing^1,2. The manipulation of this spin-valley index, which carries a magnetic moment³, requires tuning its energy. This is typically achieved through an external magnetic field (B), which is practically cumbersome. However, the valley-contrasting optical Stark effect achieves valley control without B, but requires large incident powers^4,5. Thus, other efficient routes to control the spin-valley index are desirable. Here we show that many-body interactions among interlayer excitons (IXs) in a WSe₂/MoSe₂ heterobilayer (HBL) induce a steady-state valley Zeeman splitting that corresponds to B ≈ 6 T. This anomalous splitting, present at incident powers as low as microwatts, increases with power and is able to enhance, suppress or even flip the sign of a B-induced splitting. Moreover, the g-factor of valley Zeeman splitting can be tuned by ~30% with incident power. In addition to valleytronics, our results could prove helpful to achieve optical non-reciprocity using two-dimensional materials.