Room-Temperature Strong Coupling of CdSe Nanoplatelets and Plasmonic Hole Arrays

Abstract

Exciton polaritons are hybrid light-matter quasiparticles that can serve as coherent light sources. Motivated by applications, room-temperature realization of polaritons requires narrow, excitonic transitions with large transition dipoles. Such transitions must then be strongly coupled to an electromagnetic mode confined in a small volume. While much work has explored polaritons in organic materials, semiconductor nanocrystals present an alternative excitonic system with enhanced photostability and spectral tunability. In particular, quasi-two-dimensional nanocrystals known as nanoplatelets (NPLs) exhibit intense, spectrally narrow excitonic transitions useful for polariton formation. Here, we place CdSe NPLs on silver hole arrays to demonstrate exciton-plasmon polaritons at room temperature. Angle-resolved reflection spectra reveal Rabi splittings up to 149 meV for the polariton states. We observe bright, polarized emission arising from the lowest polariton state. Furthermore, we assess the dependence of the Rabi splitting on the hole-array pitch and the number N of NPLs. While the pitch determines the in-plane momentum for which strong coupling is observed, it does not affect the size of the splitting. The Rabi splitting first increases with NPL film thickness before eventually saturating. Instead of the commonly used N dependence, we develop an analytical expression that includes the transverse confinement of the plasmon modes to describe the measured Rabi splitting as a function of NPL film thickness.