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Diffusion effect on the decay of time-resolved photoluminescence under low illumination in lead halide perovskites

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Abstract

Time-resolved photoluminescence (TRPL) has been extensively used to measure the carrier lifetime in lead halide perovskites. The TRPL curves of perovskite materials are usually fitted with a multi-exponential function, instead of a single exponential one. This was considered to be a result of the surface and the bulk recombination or the additional radiative recombination caused by the high excited carrier density. Here, a new model considering the diffusion and the trap-assisted recombination of carriers is proposed to explain the TRPL curves. The expressions of the TRPL curves and the transient absorption (TA) dynamic curves are theoretically derived, demonstrating that the TRPL curve is an infinite exponential series, regardless of the presence of surface recombination or not. Our newly developed highly sensitive nanosecond TA and TRPL were employed to measure the carrier dynamics of the same sample under low illumination in the linear response region of TA, thereby experimentally verifying our model. These results suggest that the decay of the TRPL is not only a consequence of the carrier recombination but also the carrier diffusion. TRPL cannot provide a direct measurement of the carrier lifetime, whereas TA spectroscopy can. Furthermore, the surface and the bulk recombination can be resolved and the average diffusion coefficient \((\overline D)\) can also be correctly obtained by combining TRPL and TA measurements. We also propose an approximate method for calculating the carrier lifetime and diffusion coefficient of high-quality perovskite films. Our model provides not only a new interpretation of the dynamics of the PL decay but also a deep insight into the carrier dynamics in the nanosecond time scale under working condition of perovskites solar cells.

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Author notes

  1. These authors contribute equally to this work.

Authors and Affiliations

  1. Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China

    Huang Li, **ngan Wang & Xueming Yang

  2. Institute of Materials, China Academy of Engineering Physics, Jiangyou, 621908, China

    Haipeng Di & Yiying Zhao

  3. Bei**g Academy of Quantum Information Sciences, Bei**g, 100193, China

    Huang Li, Ming Lu, An-An Liu, Nanlin Wang & Bohan Li

  4. International Center for Quantum Materials, School of Physics, Peking University, Bei**g, 100871, China

    Nanlin Wang

  5. State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Huang Li, Zefeng Ren & Xueming Yang

Authors
  1. Huang Li
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  2. Haipeng Di
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  10. Bohan Li
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Corresponding authors

Correspondence to Yiying Zhao or Bohan Li.

Additional information

This work was supported by the National Natural Science Foundation of China (Grant No. 11888101), National Key Research and Development Program of China (Grant No. 2022YFA1403901), Sichuan Science and Technology Program (Grant Nos. 2021JDTD0021, and 2022ZYD0015), and Innovation Funds from China Academy of Engineering Physics (Grant No. CX20210037).

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The supporting information is available online at http://phys.scichina.com and https://springer.longhoe.net. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Li, H., Di, H., Wang, X. et al. Diffusion effect on the decay of time-resolved photoluminescence under low illumination in lead halide perovskites. Sci. China Phys. Mech. Astron. 66, 287311 (2023). https://doi.org/10.1007/s11433-023-2108-1

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  • DOI: https://doi.org/10.1007/s11433-023-2108-1

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