Abstract
The enhancement of the photophysical response of fluorophores is a crucial factor for photonic and optoelectronic technologies that involve fluorophores as gain media. Recent advances in the development of an extreme light propagation regime, called epsilon-near-zero (ENZ), provide a promising approach in this respect. In this work, we design metal/dielectric nanocavities to be resonant with the absorption and emission bands of the employed fluorophores. Using CsPbBr3 perovskite nanocrystal films as light emitters, we study the spontaneous emission and decay rate enhancement induced by a specifically tailored double-epsilon-near-zero (double ENZ) structure. We experimentally demonstrate the existence of two ENZ wavelengths, by directly measuring their dielectric permittivity via ellipsometric analysis. The double ENZ nature of this plasmonic nanocavity has been exploited to achieve both surface plasmon enhanced absorption (SPEA) and surface plasmon coupled emission (SPCE), inducing a significant enhancement of both the spontaneous emission and the decay rate of the perovskite nanocrystal film that is placed on top of the nanocavity. Finally, we discuss the possibility of tailoring the two ENZ wavelengths of this structure within the visible spectrum simply by finely designing the thickness of the two dielectric layers, which enables resonance matching with a broad variety of dyes. Our device design is appealing for many practical applications, ranging from sensing to low threshold amplified spontaneous emission, since we achieve a strong PL enhancement with structures that allow for straightforward fluorophore deposition on a planar surface that keeps the fluorophores exposed and accessible.