Ultrastrong Coupling of Band-Nested Excitons in Few-Layer Molybdenum Disulphide

The 2D transition-metal dichalcogenides (2D TMDCs) are an intriguing platform for studying strong light–matter interactions because they combine the electronic properties of conventional semiconductors with the optical resonances found in organic systems. However, the coupling strengths demonstrated in strong exciton–polariton coupling in the 2D TMDCs remain much lower than those found in organic systems. In this paper, a new approach is taken by utilizing the large oscillator strength of the above-band gap C exciton in few-layer molybdenum disulphide (FL-MoS₂). A k-space Rabi splitting of 293 meV is shown when coupling FL-MoS₂ C excitons to surface plasmon polaritons at room temperature. This value is 11% of the uncoupled exciton energy (2.67 eV or 464 nm), ≈2× what is typically seen in the TMDCs, placing the system in the ultrastrong coupling regime. The results take a step toward finally achieving the efficient quantum coherent processes of ultrastrong coupling in a CMOS-compatible system—the 2D TMDCs—in the visible spectrum.