Fröhlich interaction dominated by a single phonon mode in CsPbBr3

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 th...

Full description

Saved in:
Bibliographic Details
Published in:Nature communications 2021-10, Vol.12 (1), p.5844-5844, Article 5844
Main Authors: Iaru, Claudiu M., Brodu, Annalisa, van Hoof, Niels J. J., ter Huurne, Stan E. T., Buhot, Jonathan, Montanarella, Federico, Buhbut, Sophia, Christianen, Peter C. M., Vanmaekelbergh, Daniël, de Mello Donega, Celso, Rivas, Jaime Gòmez, Koenraad, Paul M., Silov, Andrei Yu
Format: Article
Language:English
Subjects:
140/125
140/133
147/143
639/301/119/995
639/925/357/354
Coupling
Dielectric relaxation
Dipoles
Electron phonon interactions
Electrons
Excitons
Humanities and Social Sciences
Lattice vibration
Lead compounds
Localization
Metal halides
multidisciplinary
Nanocrystals
Optical properties
Optoelectronics
Perovskites
Phonons
Raman spectra
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
Time domain analysis
Transport properties
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary: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 CsPbBr 3 . We identify a longitudinal optical phonon mode that dominates the interaction, and surmise that this mode effectively defines exciton-phonon scattering in CsPbBr 3 , 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 CsPbBr 3 , 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. Electron-phonon interaction is essential for understanding electronic and optical properties of lead halide perovskites. Here, using multiphonon Raman scattering and THz time-domain spectroscopy, the authors characterize the full phonon spectrum of CsPbBr 3 and identify a single phonon mode that dominates electron-phonon scattering.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-021-26192-0