Enhanced Spontaneous Emission through High‐k Modes in CsPbBr3 Perovskite Hyperbolic Metamaterials

Novel optical sources require fast decay rates, making hyperbolic metamaterials (HMMs) an increasingly attractive option. HMMs are well-known for their remarkable anisotropy, and leverage hyperbolic dispersion to enhance the decay rate of a fluorophore placed on top of them. This study tackles the complex task of embedding a fluorophore into an HMM, successfully overcoming challenges related to surface roughness, thickness imperfections, and layer washing effects. Specifically, CsPbBr3 perovskite nanocrystals (NCs)-based HMM are fabricated, by alternating silver/nanocrystals (Ag/NCs) layers. Through a systematic investigation of the photophysical response following the deposition of each bilayer, compelling evidence of the achievement of hyperbolic dispersion is provided. Specifically, the impact of "high-k" modes is isolated, which is distinctive to the HMM architecture. Therefore, the longstanding debate regarding the number of bilayers needed to achieve hyperbolic dispersion is conclusively resolved. The research demonstrates a nearly twofold increase in the decay rate and a threefold enhancement in photoluminescence intensity. These findings are further supported by theoretical Purcell factor calculations. This study marks a pioneering advancement in the field of bulk dye-embedded HMMs, laying the groundwork for the development of advanced optical sources such as "resonant gain HMMs".