Strong Light–Matter Interaction and Spontaneous Emission Reshaping via Pseudo‐Cavity Modes

Abstract Strong light–matter interaction is usually achieved by embedding a gain medium in a high‐quality (Q)‐factor cavity made with thick external mirrors. The high reflectivity of the mirrors poses, therefore, a trade‐off between pump radiation coupling efficiency and high Q‐factor, thus preventing the use of optical cavities in photonic contexts where the photosensitive element necessitates to be readily accessible. Here, this long‐standing problem is overcome by engineering “Pseudo‐Cavity Modes” (PCM) in a Metal/Dielectric Open Cavity (MDOC) system that has been commonly thought to be incapable to show resonances. The MDOC system lets the embedded fluorophore exposed to radiation, opening to strong light/matter interaction. To prove this: i) exciton/PCM strong coupling regime, with 160 meV Rabi splitting, ii) photoluminescence enhancement by more than 7 times, and iii) polarized and angle‐dependent spontaneous emission are experimentally and theoretically demonstrated. The proposed system holds great potential envisioning scenarios like cavity‐enhanced photovoltaics, surface‐enhanced Raman scattering, open‐cavity lasers, photoluminescence steering and polarization.