Publication date: 15th May 2025
Exciton-polaritons are hybrid light-matter states arising from the strong coupling of electronic states of matter to the photonic states of an optical cavity, characterized by the realization of two new energy states split about the exciton. Polaritons offer as promising systems to employ quantum electrodynamics for a number of applications including quantum computing, room temperature Bose-Einstein condensation, and the alteration of chemical reactions. CdSe nanoplatelets (NPLs) have been investigated as the active material in such systems in-part due to the large oscillator strength of the bright heavy-hole excitonic transition. Recently, the nature of this oscillator strength has faced scrutiny, with measured values differing by several orders of magnitude [1-3]. Using experimentally measured room-temperature Rabi-splitting energies of exciton-polaritons generated from CdSe core-only NPLs, alongside theoretical simulations of cavity mode volume, we determine the heavy hole exciton oscillator strength for NPLs with a variety of lateral areas. Using this method, we also investigate exciton-polaritons formed from CdSe core, CdSe/CdS core-crown, and CdSe/CdS core-shell NPLs, and are able to extract oscillator strengths in each case from the magnitude of the coupling to the cavity. Photoluminescence lifetime measurements on core-crown and core-shell polariton samples revealed no difference in lifetime between the two samples in contrast to the thin films. Additionally, each sample showed a gradual lengthening of lifetime as energy is lowered from the upper to lower polariton states, indicating a lessening degree of phonon-mediated transfer to the dark states. These results provide insight and progress towards utilizing CdSe NPLs as the active medium in practical polaritonic devices.
Synthesis and characterization of CdSe NPLs was supported by the US Department of Energy (DOE) under Grant No. DE-SC0022171 and subsequently by National Science Foundation under Grant No. CHE-2304937. Spectroscopic measurements were supported by DOE under Grant No. DE-SC0022171.
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