Metal Coordination Sphere Deformation Induced Highly Stokes‐Shifted, Ultra Broadband Emission in 2D Hybrid Lead‐Bromide Perovskites and Investigation of Its Origin

Published studies of layered (2D) (100)‐oriented hybrid lead‐bromide perovskites evidence a correlation between increased inter‐octahedral (Pb‐Br‐Pb) distortions and the appearance of broadband white light emission. However, the impact of distortions within their constituent [PbBr6]4− octahedra has...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2020-06, Vol.59 (27), p.10791-10796
Main Authors: Febriansyah, Benny, Borzda, Tetiana, Cortecchia, Daniele, Neutzner, Stefanie, Folpini, Giulia, Koh, Teck Ming, Li, Yongxin, Mathews, Nripan, Petrozza, Annamaria, England, Jason
Format: Article
Language:English
Subjects:
Broadband
Color centers
crystal engineering
Distortion
Emission analysis
Excitons
intra-octahedral distortion
Lead
lead-bromide perovskites
Light emission
Localization
Perovskites
Photoluminescence
Photons
photophysics
Room temperature
Temperature dependence
Time dependence
White light
white-light emission
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Summary:Published studies of layered (2D) (100)‐oriented hybrid lead‐bromide perovskites evidence a correlation between increased inter‐octahedral (Pb‐Br‐Pb) distortions and the appearance of broadband white light emission. However, the impact of distortions within their constituent [PbBr6]4− octahedra has yet to be assessed. Herein, we report two new (100)‐oriented 2D Pb‐Br perovskites, whose structures display unusually high intra‐octahedral distortions, whilst retaining minimal inter‐octahedral distortions. Using a combination of temperature‐dependent, power‐dependent and time‐resolved photoluminescence spectroscopic measurements, we show that increased intra‐octahedral distortion induces exciton localization processes and leads to formation of multiple photoinduced emissive colour centres. Ultimately, this leads to highly Stokes‐shifted, ultrabroad white light emission at room temperature. 2D perovskite white‐light emitters: Asymmetric pyridinium‐ and piperidinium‐based cations were used to template 2D hybrid lead‐bromide perovskites with unusually high intra‐octahedral distortions. This synthetic procedure leads to the formation of multiple photoinduced emissive colour centres, which ultimately results in highly Stokes‐shifted, ultrabroad white light emission.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201915708