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Disentangling the effects of structure and lone-pair electrons in the lattice dynamics of halide perovskites

Author

Listed:
  • Sebastián Caicedo-Dávila

    (Technical University of Munich)

  • Adi Cohen

    (Weizmann Institute of Science)

  • Silvia G. Motti

    (University of Oxford
    University of Southampton)

  • Masahiko Isobe

    (Max Planck Institute for Solid State Research)

  • Kyle M. McCall

    (ETH Zurich
    EMPA - Swiss National Laboratories for Materials and Technology
    University of Texas at Dallas)

  • Manuel Grumet

    (Technical University of Munich)

  • Maksym V. Kovalenko

    (ETH Zurich
    EMPA - Swiss National Laboratories for Materials and Technology)

  • Omer Yaffe

    (Weizmann Institute of Science)

  • Laura M. Herz

    (University of Oxford
    Technical University of Munich)

  • Douglas H. Fabini

    (Max Planck Institute for Solid State Research
    Massachusetts Institute of Technology)

  • David A. Egger

    (Technical University of Munich)

Abstract

Halide perovskites show great optoelectronic performance, but their favorable properties are paired with unusually strong anharmonicity. It was proposed that this combination derives from the ns2 electron configuration of octahedral cations and associated pseudo-Jahn–Teller effect. We show that such cations are not a prerequisite for the strong anharmonicity and low-energy lattice dynamics encountered in these materials. We combine X-ray diffraction, infrared and Raman spectroscopies, and molecular dynamics to contrast the lattice dynamics of CsSrBr3 with those of CsPbBr3, two compounds that are structurally similar but with the former lacking ns2 cations with the propensity to form electron lone pairs. We exploit low-frequency diffusive Raman scattering, nominally symmetry-forbidden in the cubic phase, as a fingerprint of anharmonicity and reveal that low-frequency tilting occurs irrespective of octahedral cation electron configuration. This highlights the role of structure in perovskite lattice dynamics, providing design rules for the emerging class of soft perovskite semiconductors.

Suggested Citation

  • Sebastián Caicedo-Dávila & Adi Cohen & Silvia G. Motti & Masahiko Isobe & Kyle M. McCall & Manuel Grumet & Maksym V. Kovalenko & Omer Yaffe & Laura M. Herz & Douglas H. Fabini & David A. Egger, 2024. "Disentangling the effects of structure and lone-pair electrons in the lattice dynamics of halide perovskites," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48581-x
    DOI: 10.1038/s41467-024-48581-x
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    References listed on IDEAS

    as
    1. Bo Wu & Haifeng Yuan & Qiang Xu & Julian A. Steele & David Giovanni & Pascal Puech & Jianhui Fu & Yan Fong Ng & Nur Fadilah Jamaludin & Ankur Solanki & Subodh Mhaisalkar & Nripan Mathews & Maarten B. , 2019. "Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Christian Gehrmann & David A. Egger, 2019. "Dynamic shortening of disorder potentials in anharmonic halide perovskites," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. Bo Wu & Haifeng Yuan & Qiang Xu & Julian A. Steele & David Giovanni & Pascal Puech & Jianhui Fu & Yan Fong Ng & Nur Fadilah Jamaludin & Ankur Solanki & Subodh Mhaisalkar & Nripan Mathews & Maarten B. , 2019. "Author Correction: Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites," Nature Communications, Nature, vol. 10(1), pages 1-1, December.
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