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Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites

Author

Listed:
  • Jianfeng Yang

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Xiaoming Wen

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
    Centre for Micro-Photonics, Swinburne University of Technology)

  • Hongze Xia

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Rui Sheng

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Qingshan Ma

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Jincheol Kim

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Patrick Tapping

    (The University of Adelaide)

  • Takaaki Harada

    (The University of Adelaide)

  • Tak W. Kee

    (The University of Adelaide)

  • Fuzhi Huang

    (State Key Lab of Advanced Technologies for Materials Synthesis and Processing, Wuhan University of Technology)

  • Yi-Bing Cheng

    (Monash University)

  • Martin Green

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Anita Ho-Baillie

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Shujuan Huang

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Santosh Shrestha

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Robert Patterson

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

  • Gavin Conibeer

    (Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales)

Abstract

The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) prolongs the cooling period of hot charge carriers, an effect that could be used in the next-generation photovoltaics devices. Using ultrafast optical characterization and first-principle calculations, four kinds of lead-halide perovskites (A=FA+/MA+/Cs+, X=I−/Br−) are compared in this study to reveal the carrier-phonon dynamics within. Here we show a stronger phonon bottleneck effect in hybrid perovskites than in their inorganic counterparts. Compared with the caesium-based system, a 10 times slower carrier-phonon relaxation rate is observed in FAPbI3. The up-conversion of low-energy phonons is proposed to be responsible for the bottleneck effect. The presence of organic cations introduces overlapping phonon branches and facilitates the up-transition of low-energy modes. The blocking of phonon propagation associated with an ultralow thermal conductivity of the material also increases the overall up-conversion efficiency. This result also suggests a new and general method for achieving long-lived hot carriers in materials.

Suggested Citation

  • Jianfeng Yang & Xiaoming Wen & Hongze Xia & Rui Sheng & Qingshan Ma & Jincheol Kim & Patrick Tapping & Takaaki Harada & Tak W. Kee & Fuzhi Huang & Yi-Bing Cheng & Martin Green & Anita Ho-Baillie & Shu, 2017. "Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14120
    DOI: 10.1038/ncomms14120
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    Cited by:

    1. Yu Wan & Zhe Cheng & Zhen Wang & Jiapeng Hu & Fang Zhong & Kangmin Leng & Mengchun Qiu & Kuai Yu & Li Wang & Antoni Rogalski & Qi Jie Wang & Jianbin Xu & Weida Hu & Qisheng Wang, 2025. "Spatial confined hot carrier dynamics for beyond unity quantum efficiency detection," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    2. Can Huang & Yingyin Mo & Ruiqi Gao & Rongchen Shen & Guijie Liang & Peng Zhang & Xin Li & Qihua Yang, 2026. "Polarized dislocation covalent organic frameworks ignite hot electrons to propel photocatalytic hydrogen generation," Nature Communications, Nature, vol. 17(1), pages 1-11, December.
    3. Daniele Catone & Giuseppe Ammirati & Patrick O’Keeffe & Faustino Martelli & Lorenzo Di Mario & Stefano Turchini & Alessandra Paladini & Francesco Toschi & Antonio Agresti & Sara Pescetelli & Aldo Di C, 2021. "Effects of Crystal Morphology on the Hot-Carrier Dynamics in Mixed-Cation Hybrid Lead Halide Perovskites," Energies, MDPI, vol. 14(3), pages 1-14, January.
    4. Jialin Li & Xun Ge & Junjian Mi & Hailu Wang & Jiachang Chen & Runzhi He & Fang Zhong & Mengwen Zhan & Cong Hu & Zhen Wang & Xiaohao Zhou & Xiangfan Xu & Zhuan Xu & Piotr Martyniuk & Antoni Rogalski &, 2025. "Flat-band quantum materials empowering self-adapted ultrabroadband detectors," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    5. Luyao Zheng & Amin Nozariasbmarz & Yuchen Hou & Jungjin Yoon & Wenjie Li & Yu Zhang & Haodong Wu & Dong Yang & Tao Ye & Mohan Sanghadasa & Ke Wang & Bed Poudel & Shashank Priya & Kai Wang, 2022. "A universal all-solid synthesis for high throughput production of halide perovskite," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    6. Qingzhao Hua & Zirui Liu & Sheng Wang & Mengyang Xia & Chenglin He & Liang Liu & Zheyuan Xu & Zilan Tang & Wenlong Jiang & Ying Jiang & Fan Cao & Xiaoxia Wang & Xuyong Yang & Anlian Pan, 2026. "Suppressing electron-phonon coupling in perovskite nanoplatelets for efficient pure-red light-emitting diodes with narrow spectral emission," Nature Communications, Nature, vol. 17(1), pages 1-10, December.

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