Giant Valley-Polarized Rydberg Excitons in Monolayer WSe₂Revealed by Magneto-photocurrent Spectroscopy

A strong Coulomb interaction could lead to a strongly bound exciton with high-order excited states, similar to the Rydberg atom. The interaction of giant Rydberg excitons can be engineered for a correlated ordered exciton array with a Rydberg blockade, which is promising for realizing quantum simulation. Monolayer transition metal dichalcogenides, with their greatly enhanced Coulomb interaction, are an ideal platform to host the Rydberg excitons in two dimensions. Here, we employ helicity-resolved magneto-photocurrent spectroscopy to identify Rydberg exciton states up to 11s in monolayer WSe2. Notably, the radius of the Rydberg exciton at 11s can be as large as 214 nm, orders of magnitude larger than the 1s exciton. The giant valley-polarized Rydberg exciton not only provides an exciting platform to study the strong exciton-exciton interaction and nonlinear exciton response but also allows the investigation of the different interplay between the Coulomb interaction and Landau quantization, tunable from a low- to high-magnetic-field limit.