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Momentarily trapped exciton polaron in two-dimensional lead halide perovskites

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  • Weijian Tao

    (Zhejiang University)

  • Chi Zhang

    (Zhejiang University)

  • Qiaohui Zhou

    (Zhejiang University)

  • Yida Zhao

    (Zhejiang University)

  • Haiming Zhu

    (Zhejiang University)

Abstract

Two-dimensional (2D) lead halide perovskites with distinct excitonic feature have shown exciting potential for optoelectronic applications. Compared to their three-dimensional counterparts with large polaron character, how the interplay between long- and short- range exciton-phonon interaction due to polar and soft lattice define the excitons in 2D perovskites is yet to be revealed. Here, we seek to understand the nature of excitons in 2D CsPbBr3 perovskites by static and time-resolved spectroscopy which is further rationalized with Urbach-Martienssen rule. We show quantitatively an intermediate exciton-phonon coupling in 2D CsPbBr3 where exciton polarons are momentarily self-trapped by lattice vibrations. The 0.25 ps ultrafast interconversion between free and self-trapped exciton polaron with a barrier of ~ 34 meV gives rise to intrinsic asymmetric photoluminescence with a low energy tail at room temperature. This study reveals a complex and dynamic picture of exciton polarons in 2D perovskites and emphasizes the importance to regulate exciton-phonon coupling.

Suggested Citation

  • Weijian Tao & Chi Zhang & Qiaohui Zhou & Yida Zhao & Haiming Zhu, 2021. "Momentarily trapped exciton polaron in two-dimensional lead halide perovskites," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21721-3
    DOI: 10.1038/s41467-021-21721-3
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    Cited by:

    1. Tian Tian & Meifang Yang & Yuxuan Fang & Shuo Zhang & Yuxin Chen & Lianzhou Wang & Wu-Qiang Wu, 2023. "Large-area waterproof and durable perovskite luminescent textiles," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Songhao Guo & Willa Mihalyi-Koch & Yuhong Mao & Xinyu Li & Kejun Bu & Huilong Hong & Matthew P. Hautzinger & Hui Luo & Dong Wang & Jiazhen Gu & Yifan Zhang & Dongzhou Zhang & Qingyang Hu & Yang Ding &, 2024. "Exciton engineering of 2D Ruddlesden–Popper perovskites by synergistically tuning the intra and interlayer structures," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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