Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

Realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently significant efforts have focused on exploring excitons in solids as a pathway to achieving nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light-matter interactions require large oscillator strength and short radiative lifetime of the excitons, which limits their interaction strength and nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses by exploiting the coupling between excitons and carriers in an atomically thin semiconductor of trilayer tungsten diselenide. By controlling the electric field and electrostatic doping of the trilayer, we observe the hybridization between intralayer and interlayer excitons along with the formation of Fermi polarons due to the interactions between excitons and free carriers. We find substantial optical nonlinearity can be achieved under both continuous wave and pulsed laser excitation, where the resonance of the hole-doped Fermi polaron blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the strong interactions between excitons and free charges with optically induced valley polarization. Our results establish that atomically thin heterostructures are a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics, and open avenues for exploring many-body physics in hybrid Fermionic-Bosonic systems.
Comment: 4 figures with SI