Manipulating Coherent Light–Matter Interaction: Continuous Transition between Strong Coupling and Weak Coupling in MoS2 Monolayer Coupled with Plasmonic Nanocavities

Strong interactions between surface plasmons in ultracompact nanocavities and excitons in 2D materials have attracted wide interests for its prospective realization of polariton devices at room temperature. Here, a continuous transition from weak coupling to strong coupling between excitons in molybdenum disulfide (MoS2) monolayer and highly localized plasmons in ultracompact nanoantenna is proposed. The nanoantenna is assembled by a silver nanocube positioned over a gold film and separated by a dielectric spacer layer. A 1570‐fold enhancement in the photoluminescence is observed at weak coupling regime in hybrid nanocavities with thick spacer layers. The interaction between excitons and plasmons is then directly prompted to strong coupling regime by shrinking down the thickness of spacer layer. Room temperature formation of polaritons with Rabi splitting up to 190 meV is observed with a fair polariton loss around 165 meV. Numerical calculations quantify the relation between coupling strength, local density of states, and spacer thickness, and reveal the transition between weak coupling and strong coupling in nanocavities. The findings in this work offer a guideline for feasible designs of plasmon–exciton interaction systems with gap plasmonic cavities.