Ground and excited state exciton polarons in monolayer MoSe₂

The versatile experimentally accessible exciton species in monolayer transition metal dichalcogenide semiconductors offer an interesting platform for investigating the interaction between two-particle bound states and a Fermi sea of charges. Using hexagonal boron nitride encapsulated monolayer MoSe2, we study the impact of charge density tuning on the A and B series of exciton Rydberg states, including A:1s, A:2s, B:1s, and B:2s. The doping dependence of the A:2s state provides an opportunity to examine such interactions with greatly reduced exciton binding energy and more spatially diffuse structures, and we found that the impact of the Fermi sea becomes much more dramatic compared to the A:1s state. Using photoluminescence upconversion, we verify that the B:2s exciton state displays similar behavior when interacting with the Fermi sea despite being well above the bare bandgap in energy. Photoluminescence and reflection spectra of the A:1s state show clear evidence that the interaction of the exciton with a Fermi sea is best described by the exciton–polaron model, rather than a trion model. Our experimental results demonstrate that overall features of charge interaction are quite generic and highly robust, offering key insights into the dressed many-body states in a Fermi sea.