Controlling the strong light-matter coupling in metal-dielectric optical resonators using spin-crossover molecules

Abstract

We report the observation of (ultra)strong light-matter coupling, in the UV spectral region, between optical modes of a metal/dielectric bilayer nanocavity and the electronic excitations of spin-crossover (SCO) molecules. By thermally switching the SCO molecules between their low-spin and high-spin states, we demonstrate the possibility of fine-tuning the light-molecule hybridization strength, allowing a reversible switching between strong- (with Rabi splitting values of up to 550 meV) and weak-coupling regimes within a single photonic resonator. As a result, we show that spin-crossover molecular compounds constitute a novel, promising class of active nanomaterials in the context of tuneable and reconfigurable polaritonic devices.