Biexcitonic optical Stark effects in monolayer molybdenum diselenide

Floquet states, where a periodic optical field coherently drives electrons in solids 1 – 3 , can enable novel quantum states of matter 4 – 6 . A prominent approach to realize Floquet states is based on the optical Stark effect. Previous studies on the optical Stark effect often treated the excited state in solids as free quasi-particles 3 , 7 – 12 . However, exciton–exciton interactions can be sizeably enhanced in low-dimensional systems and may lead to light–matter interactions that are qualitatively different from those in the non-interacting picture. Here we use monolayer molybdenum diselenide (MoSe 2 ) as a model system to demonstrate that the driving optical field can couple a hierarchy of excitonic states, and the many-body inter-valley biexciton state plays a dominant role in the optical Stark effect. Specifically, the exciton–biexciton coupling in monolayer MoSe 2 breaks down the valley selection rules based on the non-interacting exciton picture. The photon-dressed excitonic states exhibit an energy redshift, splitting or blueshift as the driving photon frequency varies below the exciton transition. We determine a binding energy of 21 meV for the inter-valley biexciton and a transition dipole moment of 9.3 debye for the exciton–biexciton transition. Our study reveals the crucial role of many-body effects in coherent light–matter interaction in atomically thin two-dimensional materials.