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Hot carrier cooling mechanisms in halide perovskites

Author

Listed:
  • Jianhui Fu

    (Nanyang Technological University)

  • Qiang Xu

    (Nanyang Technological University)

  • Guifang Han

    (Energy Research Institute @NTU (ERI@N), Research Techno Plaza)

  • Bo Wu

    (Nanyang Technological University)

  • Cheng Hon Alfred Huan

    (Nanyang Technological University
    Institute of Materials Research and Engineering (IMRE))

  • Meng Lee Leek

    (Nanyang Technological University)

  • Tze Chien Sum

    (Nanyang Technological University)

Abstract

Halide perovskites exhibit unique slow hot-carrier cooling properties capable of unlocking disruptive perovskite photon–electron conversion technologies (e.g., high-efficiency hot-carrier photovoltaics, photo-catalysis, and photodetectors). Presently, the origins and mechanisms of this retardation remain highly contentious (e.g., large polarons, hot-phonon bottleneck, acoustical–optical phonon upconversion etc.). Here, we investigate the fluence-dependent hot-carrier dynamics in methylammonium lead triiodide using transient absorption spectroscopy, and correlate with theoretical modeling and first-principles calculations. At moderate carrier concentrations (around 1018 cm−3), carrier cooling is mediated by polar Fröhlich electron–phonon interactions through zone-center delayed longitudinal optical phonon emissions (i.e., with phonon lifetime τ LO around 0.6 ± 0.1 ps) induced by the hot-phonon bottleneck. The hot-phonon effect arises from the suppression of the Klemens relaxation pathway essential for longitudinal optical phonon decay. At high carrier concentrations (around 1019 cm−3), Auger heating further reduces the cooling rates. Our study unravels the intricate interplay between the hot-phonon bottleneck and Auger heating effects on carrier cooling, which will resolve the existing controversy.

Suggested Citation

  • Jianhui Fu & Qiang Xu & Guifang Han & Bo Wu & Cheng Hon Alfred Huan & Meng Lee Leek & Tze Chien Sum, 2017. "Hot carrier cooling mechanisms in halide perovskites," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-01360-3
    DOI: 10.1038/s41467-017-01360-3
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    Cited by:

    1. Junzhi Ye & Navendu Mondal & Ben P. Carwithen & Yunwei Zhang & Linjie Dai & Xiang-Bing Fan & Jian Mao & Zhiqiang Cui & Pratyush Ghosh & Clara Otero‐Martínez & Lars Turnhout & Yi-Teng Huang & Zhongzhen, 2024. "Extending the defect tolerance of halide perovskite nanocrystals to hot carrier cooling dynamics," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. 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.
    3. Yue Wang & Senyun Ye & Jia Wei Melvin Lim & David Giovanni & Minjun Feng & Jianhui Fu & Harish N S Krishnamoorthy & Qiannan Zhang & Qiang Xu & Rui Cai & Tze Chien Sum, 2023. "Carrier multiplication in perovskite solar cells with internal quantum efficiency exceeding 100%," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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