Fröhlich interaction dominated by a single phonon mode in CsPbBr3

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, Jaime Gòmez Rivas, Paul M. Koenraad and Andrei Yu. Silov ()
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Claudiu M. Iaru: Eindhoven University of Technology
Annalisa Brodu: Utrecht University
Niels J. J. Hoof: Eindhoven University of Technology
Stan E. T. Huurne: Eindhoven University of Technology
Jonathan Buhot: University of Bristol
Federico Montanarella: Utrecht University
Sophia Buhbut: Utrecht University
Peter C. M. Christianen: Radboud University
Daniël Vanmaekelbergh: Utrecht University
Celso Mello Donega: Utrecht University
Jaime Gòmez Rivas: Eindhoven University of Technology
Paul M. Koenraad: Eindhoven University of Technology
Andrei Yu. Silov: Eindhoven University of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract The excellent optoelectronic performance of lead halide perovskites has generated great interest in their fundamental properties. The polar nature of the perovskite lattice means that electron-lattice coupling is governed by the Fröhlich interaction. Still, considerable ambiguity exists regarding the phonon modes that participate in this crucial mechanism. Here, we use multiphonon Raman scattering and THz time-domain spectroscopy to investigate Fröhlich coupling in CsPbBr3. We identify a longitudinal optical phonon mode that dominates the interaction, and surmise that this mode effectively defines exciton-phonon scattering in CsPbBr3, and possibly similar materials. It is additionally revealed that the observed strength of the Fröhlich interaction is significantly higher than the expected intrinsic value for CsPbBr3, and is likely enhanced by carrier localization in the colloidal perovskite nanocrystals. Our experiments also unearthed a dipole-related dielectric relaxation mechanism which may impact transport properties.

Date: 2021
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DOI: 10.1038/s41467-021-26192-0

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