Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum and nonlinear optics. Polaritons, hybridized light-matter quasiparticles, are an appealing candidate to realize such nonlinearities. Here, we explore a class of peculiar polaritons, named plasmon-exciton polaritons (plexcitons), in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS₂), which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature. Specifically, comprehensive ultrafast pump-probe measurements reveal that plexciton nonlinearity is dominated by the saturation and higher-order excitation-induced dephasing interactions, rather than the well-known exchange interaction in traditional microcavity polaritons. Furthermore, we demonstrate this giant nonlinearity can be exploited to manipulate the ultrafast nonlinear absorption properties of the solid-state system. Our findings suggest that plexcitons are intrinsically strongly interacting, thereby pioneering new horizons for practical implementations such as energy-efficient ultrafast all-optical switching and information processing.