Publication date: 15th May 2025
Polaritons, arising from the strong coupling between excitons and photons in optical microcavities, exhibit unique quantum properties that could potentially enable novel applications at the intersection of quantum information science and chemistry.[1],[2] Investigations of polariton dynamics in ultrafast time scales is crucial for understanding their coherence and population exchange mechanisms, neither of which is well understood.[3] Using ultrafast transient absorption spectroscopy, we investigated the time evolution of polaritonic states formed by CdSe nanoplatelets coupled to a Fabry-Pérot optical cavity. Angle-resolved reflectance measurement indicates a Rabi splitting energy ℏΩR ~70 meV; such a large energy splitting allows us to probe state selective excitation dependent dynamics. Direct excitation to the upper polariton (UP) state reveals a population relaxation time of 509 ± 31 fs, suggesting dark-state-mediated cooling from the UP to LP states. In contrast, above UP and direct excitation of LP states results in faster population growth (472 ± 14 and 399 ± 47 fs, respectively). These results provide insights into the fundamental processes in systems showing strong light-matter coupling, highlighting the evolution of state populations and the influence of dark states.
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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