Quadrupolar Excitons in MoSe2 Bilayers

The quest for platforms to generate and control exotic excitonic states has greatly benefited from the advent of transition metal dichalcogenide (TMD) monolayers and their heterostructures. Among the unconventional excitonic states, quadrupolar excitons - a hybridized combination of two dipolar excitons with anti-aligned dipole moments - are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, we unambiguously demonstrate for the first time in natural MoSe₂ homobilayers the emergence of quadrupolar excitons, whose energy shifts quadratically in electric field. In contrast to, so far reported trilayer systems hosting quadrupolar excitons, MoSe₂ homobilayers have many advantages, a stronger interlayer hybridization, cleaner potential landscapes and inherent stability with respect to moir\'e potentials or post-stacking reconstruction. Our experimental observations are complemented by many-particle theory calculations offering microscopic insights in the formation of quadrupole excitons. Our results suggest TMD homobilayers as ideal platform for the engineering of excitonic states and their interaction with light and thus candidate for carrying out on-chip simulations.