Rydberg polaritons in ReS2 crystals

Abstract: Rhenium disulfide (ReS2) belongs to group-VII transition metal dichalcogenide (TMDs) with attractive properties such as exceptionally high refractive index and significant oscillator strength, large in-plane birefringence, and good chemical stability. Unlike most other TMDs, the peculiar optical properties of ReS2 persist from bulk to the monolayer, making this material potentially suitable for applications in optical devices. In this work, we demonstrate with unprecedented clarity the strong coupling between cavity modes and excited states, which results in a strong polariton interaction, showing the interest of such materials as a solid-state counterpart of Rydberg atomic systems. Moreover, we definitively clarify the nature of important spectral features, shedding light on some controversial aspects or incomplete interpretations and demonstrating that their origin is due to the interesting combination of the very high refractive index and the large oscillator strength expressed by these TMDs.