Electrically tunable ultrafast dynamics and interactions of hybrid excitons in a 2D semiconductor bilayer.

Abstract

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.