Real‐Time Tuning Exciton‐Plasmon Coupling with Photosensitive Nanocavity

Abstract A novel method is proposed to directly characterize the exciton‐plasmon coupling in a photosensitive nanoparticle‐on‐mirror (NPoM) nanocavity. Under the illumination of UV light, the localized surface plasmon resonance (LSPR) peaks of the nanocavity can be continuously tuned over a wide range (≈65 nm), enabling precise determination of the energy dispersion relationship of plexcitons in the nanocavity. The results indicate that the energy of Rabi splitting can be actively tuned from 65 meV (weak coupling) to 170 meV (strong coupling) by adjusting the LSPR peak of a specific nanocavity (particle size L ≈55‐92 nm) to the exciton wavelength (the zero detuning). In addition, the criterion of strong coupling is optimized by introducing single‐particle absorption spectroscopy. The work offers an intuitive method for the strong coupling characterization in nanocavity, paving the way for the real‐time tuning of coupling strength over a wide range (100 meV) from weak to strong coupling regimes.