Cavity Controlled Upconversion in CdSe Nanoplatelet Polaritons.

Abstract

Exciton-polaritons provide a versatile platform for investigating quantum electrodynamics effects in chemical systems, such as polariton-altered chemical reactivity. However, using polaritons in chemical contexts will require a better understanding of their photophysical properties under ambient conditions, where chemistry is typically performed. Here, we used cavity quality factor to control strong light-matter interactions and in particular the excited state dynamics of colloidal CdSe nanoplatelets (NPLs) coupled to a Fabry-Pérot optical cavity. With increasing cavity quality factor, we observe significant population of the upper polariton (UP) state, exemplified by the rare observation of substantial UP photoluminescence (PL). Excitation of the lower polariton (LP) states results in upconverted PL emission from the UP branch due to efficient exchange of population between the LP, UP and the reservoir of dark states present in collectively coupled polaritonic systems. In addition, we measure time scales for polariton dynamics ∼100 ps, implying great potential for NPL based polariton systems to affect photochemical reaction rates. State-of-the-art quantum dynamical simulations show outstanding quantitative agreement with experiments, and thus provide important insight into polariton photophysical dynamics of collectively coupled nanocrystal-based systems. These findings represent a significant step toward the development of practical polariton photochemistry platforms.