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Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites

Author

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  • Yinsheng Guo

    (Columbia University)

  • Omer Yaffe

    (Weizmann Institute of Science)

  • Trevor D. Hull

    (Columbia University)

  • Jonathan S. Owen

    (Columbia University)

  • David R. Reichman

    (Columbia University)

  • Louis E. Brus

    (Columbia University)

Abstract

Lead-halide perovskites have emerged as promising materials for photovoltaic and optoelectronic applications. Their significantly anharmonic lattice motion, in contrast to conventional harmonic semiconductors, presents a conceptual challenge in understanding the genesis of their exceptional optoelectronic properties. Here we report a strongly temperature dependent luminescence Stokes shift in the electronic spectra of both hybrid and inorganic lead-bromide perovskite single crystals. This behavior stands in stark contrast to that exhibited by more conventional crystalline semiconductors. We correlate the electronic spectra with the anti-Stokes and Stokes Raman vibrational spectra. Dielectric solvation theories, originally developed for excited molecules dissolved in polar liquids, reproduce our experimental observations. Our approach, which invokes a classical Debye-like relaxation process, captures the dielectric response originating from the incipient anharmonicity of the LO phonon at about 20 meV (160 cm−1) in the lead-bromide framework. We reconcile this liquid-like model incorporating thermally-activated dielectric solvation with more standard solid-state theories of the emission Stokes shift in crystalline semiconductors.

Suggested Citation

  • Yinsheng Guo & Omer Yaffe & Trevor D. Hull & Jonathan S. Owen & David R. Reichman & Louis E. Brus, 2019. "Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09057-5
    DOI: 10.1038/s41467-019-09057-5
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    Cited by:

    1. Claudiu M. Iaru & Annalisa Brodu & Niels J. J. Hoof & Stan E. T. Huurne & Jonathan Buhot & Federico Montanarella & Sophia Buhbut & Peter C. M. Christianen & Daniël Vanmaekelbergh & Celso Mello Donega , 2021. "Fröhlich interaction dominated by a single phonon mode in CsPbBr3," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    2. Hongzhi Zhou & Qingjie Feng & Cheng Sun & Yahui Li & Weijian Tao & Wei Tang & Linjun Li & Enzheng Shi & Guangjun Nan & Haiming Zhu, 2024. "Robust excitonic light emission in 2D tin halide perovskites by weak excited state polaronic effect," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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