Moiré excitons in generalized Wigner crystals

Moiré superlattices of transition-metal dichalcogenide bilayers host strong Coulomb interactions residing in narrow electron bands, leading to correlated insulating states at fractional carrier doping densities, known as generalized Wigner crystals. In excited states, the formation of moiré excitons can be fundamentally shaped by the Wigner-crystal ground states, manifesting an intricate interplay between electronic and excitonic correlations. However, the microscopic description of these Wigner crystalline excitons (WCEs) remains elusive, largely subject to speculations, and is further needed for the understanding of exotic excitonic phases (e.g., exciton insulators and exciton density waves) and their unique properties (e.g., anomalous exciton diffusion). Here, using first-principles many-body <i>GW</i>-Bethe-Salpeter equation calculations, we directly reveal the internal structures of WCEs in angle-aligned MoSe₂/MoS₂ moiré heterostructure at hole fillings of 1/3 and 2/3. Our results uncover the propagation of correlation effects from the ground state to excited states, shaping the real-space characteristics of WCEs. The strong two-particle excitonic correlations dominate over the kinetic energy of free electron-hole pairs, in analog to the strong single-particle correlations of flat bands. We propose that such unusual excited-state correlation effects of WCEs can be experimentally probed by photocurrent tunneling microscopy (PTM). Our work provides a microscopic understanding of strongly correlated WCEs, suggesting them as a highly tunable mixed boson-fermion platform to study many-body interactions and phenomena.