IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v12y2021i1d10.1038_s41467-021-22934-2.html
   My bibliography  Save this article

Coherent vibrational dynamics reveals lattice anharmonicity in organic–inorganic halide perovskite nanocrystals

Author

Listed:
  • Tushar Debnath

    (Ludwig Maximilians-Universität (LMU))

  • Debalaya Sarker

    (Skolkovo Institute of Science and Technology)

  • He Huang

    (Ludwig Maximilians-Universität (LMU))

  • Zhong-Kang Han

    (Skolkovo Institute of Science and Technology)

  • Amrita Dey

    (Ludwig Maximilians-Universität (LMU))

  • Lakshminarayana Polavarapu

    (Ludwig Maximilians-Universität (LMU))

  • Sergey V. Levchenko

    (Skolkovo Institute of Science and Technology)

  • Jochen Feldmann

    (Ludwig Maximilians-Universität (LMU))

Abstract

The halide ions of organic-inorganic hybrid perovskites can strongly influence the interaction between the central organic moiety and the inorganic metal halide octahedral units and thus their lattice vibrations. Here, we report the halide-ion-dependent vibrational coherences in formamidinium lead halide (FAPbX3, X = Br, I) perovskite nanocrystals (PNCs) via the combination of femtosecond pump–probe spectroscopy and density functional theory calculations. We find that the FAPbX3 PNCs generate halide-dependent coherent vibronic wave packets upon above-bandgap non-resonant excitation. More importantly, we observe several higher harmonics of the fundamental modes for FAPbI3 PNCs as compared to FAPbBr3 PNCs. This is likely due to the weaker interaction between the central FA moiety and the inorganic cage for FAPbI3 PNCs, and thus the PbI64− unit can vibrate more freely. This weakening reveals the intrinsic anharmonicity in the Pb-I framework, and thus facilitating the energy transfer into overtone and combination bands. These findings not only unveil the superior stability of Br–based PNCs over I–based PNCs but are also important for a better understanding of their electronic and polaronic properties.

Suggested Citation

  • Tushar Debnath & Debalaya Sarker & He Huang & Zhong-Kang Han & Amrita Dey & Lakshminarayana Polavarapu & Sergey V. Levchenko & Jochen Feldmann, 2021. "Coherent vibrational dynamics reveals lattice anharmonicity in organic–inorganic halide perovskite nanocrystals," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-22934-2
    DOI: 10.1038/s41467-021-22934-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-021-22934-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-021-22934-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    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. Yannan Liu & Cheng-Hao Liu & Tushar Debnath & Yong Wang & Darius Pohl & Lucas V. Besteiro & Debora Motta Meira & Shengyun Huang & Fan Yang & Bernd Rellinghaus & Mohamed Chaker & Dmytro F. Perepichka &, 2023. "Silver nanoparticle enhanced metal-organic matrix with interface-engineering for efficient photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-22934-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.