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Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy

Author

Listed:
  • Johannes M. Richter

    (University of Cambridge)

  • Federico Branchi

    (Politecnico di Milano)

  • Franco Valduga de Almeida Camargo

    (Politecnico di Milano)

  • Baodan Zhao

    (University of Cambridge)

  • Richard H. Friend

    (University of Cambridge)

  • Giulio Cerullo

    (Politecnico di Milano)

  • Felix Deschler

    (University of Cambridge)

Abstract

In band-like semiconductors, charge carriers form a thermal energy distribution rapidly after optical excitation. In hybrid perovskites, the cooling of such thermal carrier distributions occurs on timescales of about 300 fs via carrier-phonon scattering. However, the initial build-up of the thermal distribution proved difficult to resolve with pump–probe techniques due to the requirement of high resolution, both in time and pump energy. Here, we use two-dimensional electronic spectroscopy with sub-10 fs resolution to directly observe the carrier interactions that lead to a thermal carrier distribution. We find that thermalization occurs dominantly via carrier-carrier scattering under the investigated fluences and report the dependence of carrier scattering rates on excess energy and carrier density. We extract characteristic carrier thermalization times from below 10 to 85 fs. These values allow for mobilities of 500 cm2 V−1 s−1 at carrier densities lower than 2 × 1019 cm−3 and limit the time for carrier extraction in hot carrier solar cells.

Suggested Citation

  • Johannes M. Richter & Federico Branchi & Franco Valduga de Almeida Camargo & Baodan Zhao & Richard H. Friend & Giulio Cerullo & Felix Deschler, 2017. "Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy," Nature Communications, Nature, vol. 8(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-00546-z
    DOI: 10.1038/s41467-017-00546-z
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    Cited by:

    1. Jongchul Lim & Manuel Kober-Czerny & Yen-Hung Lin & James M. Ball & Nobuya Sakai & Elisabeth A. Duijnstee & Min Ji Hong & John G. Labram & Bernard Wenger & Henry J. Snaith, 2022. "Long-range charge carrier mobility in metal halide perovskite thin-films and single crystals via transient photo-conductivity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. 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.
    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. Gang Wang & Tanghao Liu & Bingzhe Wang & Hao Gu & Qi Wei & Zhipeng Zhang & Jun He & Mingjie Li & Guichuan Xing, 2022. "Hot-carrier tunable abnormal nonlinear absorption conversion in quasi-2D perovskite," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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