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Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites

Nature materials, 2019-04, Vol.18 (4), p.349-356 [Peer Reviewed Journal]

2019© The Author(s), under exclusive licence to Springer Nature Limited 2019 ;ISSN: 1476-1122 ;EISSN: 1476-4660 ;DOI: 10.1038/s41563-018-0262-7 ;PMID: 30643234

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  • Title:
    Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites
  • Author: Thouin, Félix ; Valverde-Chávez, David A ; Quarti, Claudio ; Cortecchia, Daniele ; Bargigia, Ilaria ; Beljonne, David ; Petrozza, Annamaria ; Silva, Carlos ; Srimath Kandada, Ajay Ram
  • Subjects: Chemical bonds ; Complexity ; Covalent bonds ; Crystal lattices ; Density functional theory ; Excitons ; Lattice vibration ; Organic semiconductors ; Perovskites ; Phonons ; Raman spectroscopy ; Semiconductor materials ; Softness
  • Is Part Of: Nature materials, 2019-04, Vol.18 (4), p.349-356
  • Description: Hybrid organic-inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency (≲50 cm ) optical phonons involving motion in the lead iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight into the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.
  • Publisher: England: Nature Publishing Group
  • Language: English
  • Identifier: ISSN: 1476-1122
    EISSN: 1476-4660
    DOI: 10.1038/s41563-018-0262-7
    PMID: 30643234
  • Source: ProQuest Central
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