Large emission enhancement and emergence of strong coupling with plasmons in nanoassemblies: Role of quantum interactions and finite emitter size

Abstract

The Purcell effect has been the basis for several decades in understanding enhancement of photonic efficiency and decay rates of emitters through their coupling to cavity modes and metal nanostructures. However, it is not clear whether this regime of radiative enhancements can be extended to ultra-small nanoparticle sizes or inter-particle distances. Here we report large radiative enhancements of quantum dot assemblies with extremely small metal nanoparticles and emitter-particle separations R of a few nanometers, where Purcell effect would lead to either no enhancements or quenching. We invoke a new regime of radiative enhancements to explain the experimental data and also correctly predict the emergence of strong coupling below certain, R, as observed in experiments. In addition we show that the widely used point emitter approximations diverge from actual observations in case of finite size emitters at such small separations.