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Efficient up-conversion in CsPbBr3 nanocrystals via phonon-driven exciton-polaron formation

Author

Listed:
  • Abdullah S. Abbas

    (Berkeley
    The University of Chicago)

  • Beiye C. Li

    (The University of Chicago
    The University of Chicago
    The University of Chicago)

  • Richard D. Schaller

    (Northwestern University
    Argonne National Laboratory)

  • Vitali B. Prakapenka

    (The University of Chicago)

  • Stella Chariton

    (The University of Chicago)

  • Daqian Bian

    (The University of Chicago
    The University of Chicago)

  • Gregory S. Engel

    (The University of Chicago
    The University of Chicago
    The University of Chicago
    The University of Chicago)

  • A. Paul Alivisatos

    (Berkeley
    The University of Chicago
    The University of Chicago
    The University of Chicago)

Abstract

Lead halide perovskite nanocrystals demonstrate efficient up-conversion, although the precise mechanism remains a subject of active research. This study utilizes steady-state and time-resolved spectroscopy methods to unravel the mechanism driving the up-conversion process in CsPbBr3 nanocrystals. Employing above- and below-gap photoluminescence measurements, we extract a distinct phonon mode with an energy of ~7 meV and identify the Pb-Br-Pb bending mode as the phonon involved in the up-conversion process. This result was corroborated by Raman spectroscopy. We confirm an up-conversion efficiency reaching up to 75%. Transient absorption measurements under conditions of sub-gap excitation also unexpectedly reveal coherent phonons for the subset of nanocrystals undergoing up-conversion. This coherence implies that the up-conversion and subsequent relaxation is accompanied by a synchronized and phased lattice motion. This study reveals that efficient up-conversion in CsPbBr3 nanocrystals is powered by a unique interplay between the soft lattice structure, phonons, and excited states dynamics.

Suggested Citation

  • Abdullah S. Abbas & Beiye C. Li & Richard D. Schaller & Vitali B. Prakapenka & Stella Chariton & Daqian Bian & Gregory S. Engel & A. Paul Alivisatos, 2025. "Efficient up-conversion in CsPbBr3 nanocrystals via phonon-driven exciton-polaron formation," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60992-y
    DOI: 10.1038/s41467-025-60992-y
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    References listed on IDEAS

    as
    1. Zikang Ye & Xing Lin & Na Wang & Jianhai Zhou & Meiyi Zhu & Haiyan Qin & Xiaogang Peng, 2021. "Phonon-assisted up-conversion photoluminescence of quantum dots," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Jun Zhang & Dehui Li & Renjie Chen & Qihua Xiong, 2013. "Laser cooling of a semiconductor by 40 kelvin," Nature, Nature, vol. 493(7433), pages 504-508, January.
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    1. Zikang Ye & Xing Lin & Na Wang & Jianhai Zhou & Meiyi Zhu & Haiyan Qin & Xiaogang Peng, 2021. "Phonon-assisted up-conversion photoluminescence of quantum dots," Nature Communications, Nature, vol. 12(1), pages 1-9, December.

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