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Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite

Author

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  • Myeongkee Park

    (University of California
    Dong-A University)

  • Amanda J. Neukirch

    (Los Alamos National Laboratory)

  • Sebastian E. Reyes-Lillo

    (Universidad Andres Bello
    University of California
    Lawrence Berkeley National Laboratory)

  • Minliang Lai

    (University of California)

  • Scott R. Ellis

    (University of California)

  • Daniel Dietze

    (Osram Opto Semiconductors GmbH)

  • Jeffrey B. Neaton

    (University of California
    Lawrence Berkeley National Laboratory
    Kavli Energy NanoSciences Institute at Berkeley)

  • Peidong Yang

    (University of California
    Kavli Energy NanoSciences Institute at Berkeley
    University of California
    Lawrence Berkeley National Laboratory)

  • Sergei Tretiak

    (Los Alamos National Laboratory)

  • Richard A. Mathies

    (University of California)

Abstract

Hybrid organic–inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb–I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, ~43, and ~75 cm−1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I–Pb–I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI64− geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.

Suggested Citation

  • Myeongkee Park & Amanda J. Neukirch & Sebastian E. Reyes-Lillo & Minliang Lai & Scott R. Ellis & Daniel Dietze & Jeffrey B. Neaton & Peidong Yang & Sergei Tretiak & Richard A. Mathies, 2018. "Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04946-7
    DOI: 10.1038/s41467-018-04946-7
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    Cited by:

    1. Xuan Trung Nguyen & Katrin Winte & Daniel Timmer & Yevgeny Rakita & Davide Raffaele Ceratti & Sigalit Aharon & Muhammad Sufyan Ramzan & Caterina Cocchi & Michael Lorke & Frank Jahnke & David Cahen & C, 2023. "Phonon-driven intra-exciton Rabi oscillations in CsPbBr3 halide perovskites," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Claudiu M. Iaru & Annalisa Brodu & Niels J. J. Hoof & Stan E. T. Huurne & Jonathan Buhot & Federico Montanarella & Sophia Buhbut & Peter C. M. Christianen & Daniël Vanmaekelbergh & Celso Mello Donega , 2021. "Fröhlich interaction dominated by a single phonon mode in CsPbBr3," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    3. Xingyu Yue & Chunwei Wang & Bo Zhang & Zeyu Zhang & Zhuang Xiong & Xinzhi Zu & Zhengzheng Liu & Zhiping Hu & George Omololu Odunmbaku & Yujie Zheng & Kuan Sun & Juan Du, 2023. "Real-time observation of the buildup of polaron in α-FAPbI3," Nature Communications, Nature, vol. 14(1), pages 1-6, December.

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