Polaritonic Bottleneck in Colloidal Quantum Dots

Kaiyue Peng*, Eran Rabani*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Controlling the relaxation dynamics of excitons is key to improving the efficiencies of semiconductor-based applications. Confined semiconductor nanocrystals (NCs) offer additional handles to control the properties of excitons, for example, by changing their size or shape, resulting in a mismatch between excitonic gaps and phonon frequencies. This has led to the hypothesis of a significant slowing-down of exciton relaxation in strongly confined NCs, but in practice due to increasing exciton-phonon coupling and rapid multiphonon relaxation channels, the exciton relaxation depends only weakly on the size or shape. Here, we focus on elucidating the nonradiative relaxation of excitons in NCs placed in an optical cavity. We find that multiphonon emission of carrier governs the decay, resulting in a polariton-induced phonon bottleneck with relaxation time scales that are slower by orders of magnitude compared to the cavity-free case, while the photon fraction plays a secondary role.

Original languageEnglish
Pages (from-to)10587-10593
Number of pages7
JournalNano Letters
Volume23
Issue number22
DOIs
StatePublished - 22 Nov 2023

Funding

FundersFunder number
NSF-BSF
National Science FoundationDMR2026741
Office of ScienceDEAC02- 05CH11231
National Energy Research Scientific Computing Center

    Keywords

    • Microcavity
    • Nanocrystals
    • Phonon Bottleneck
    • Polariton
    • Quantum Dots

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