Strong-interaction-driven quadrupolar-to-dipolar exciton transitions in a trilayer moiré superlattice

The additional layer degree of freedom in trilayer moiré superlattices of transition metal dichalcogenides enables the emergence of novel excitonic species, such as quadrupolar excitons, which exhibit unique excitonic interactions and hold promise for realizing intriguing excitonic phases and their quantum phase transitions. Concurrently, the presence of strong electronic correlations in moiré superlattices, as exemplified by the observations of Mott insulators and generalized Wigner crystals, offers a direct route to manipulate these new excitonic states and the resulting collective excitonic phases. Here we demonstrate that strong exciton–exciton and electron–exciton interactions, both stemming from robust electron correlations, can be harnessed to controllably drive transitions between quadrupolar and dipolar excitons. This is achieved by tuning either the exciton density or electrostatic doping in a trilayer semiconducting moiré superlattice. Our findings not only advance the fundamental understanding of quadrupolar excitons but also usher in new avenues for exploring and engineering many-body quantum phenomena through novel correlated excitons in semiconducting moiré systems.