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Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites

Author

Listed:
  • Bo Wu

    (South China Normal University
    Nanyang Technological University)

  • Haifeng Yuan

    (KU Leuven)

  • Qiang Xu

    (Nanyang Technological University)

  • Julian A. Steele

    (KU Leuven)

  • David Giovanni

    (Nanyang Technological University)

  • Pascal Puech

    (University of Toulouse)

  • Jianhui Fu

    (Nanyang Technological University)

  • Yan Fong Ng

    (Nanyang Technological University
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza)

  • Nur Fadilah Jamaludin

    (Nanyang Technological University
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza)

  • Ankur Solanki

    (Nanyang Technological University)

  • Subodh Mhaisalkar

    (Nanyang Technological University
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza)

  • Nripan Mathews

    (Nanyang Technological University
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza)

  • Maarten B. J. Roeffaers

    (KU Leuven)

  • Michael Grätzel

    (Energy Research Institute @NTU (ERI@N), Research Techno Plaza
    Swiss Federal Institute of Technology)

  • Johan Hofkens

    (KU Leuven)

  • Tze Chien Sum

    (Nanyang Technological University)

Abstract

Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08326-7
    DOI: 10.1038/s41467-019-08326-7
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    Cited by:

    1. 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.

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