Fröhlich interaction dominated by a single phonon mode in CsPbBr3

Claudiu M. Iaru; Annalisa Brodu; Niels J.J. van Hoof; Stan E.T. ter Huurne; Jonathan Buhot; Federico Montanarella; Sophia Buhbut; Peter C.M. Christianen; Daniël Vanmaekelbergh; Celso de Mello Donega; Jaime Gòmez Rivas; Paul M. Koenraad; Andrei Yu Silov

doi:10.1038/s41467-021-26192-0

Fröhlich interaction dominated by a single phonon mode in CsPbBr₃

Claudiu M. Iaru (Corresponding author), Annalisa Brodu, Niels J.J. van Hoof, Stan E.T. ter Huurne, Jonathan Buhot, Federico Montanarella, Sophia Buhbut, Peter C.M. Christianen, Daniël Vanmaekelbergh, Celso de Mello Donega, Jaime Gòmez Rivas, Paul M. Koenraad, Andrei Yu Silov (Corresponding author)

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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.

Original language	English
Article number	5844
Number of pages	8
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-26192-0
Publication status	Published - Dec 2021

Bibliographical note

Funding Information:
This work is part of the research program entitled “Designing Dirac Carriers in Semiconductor Superlattices” (DDC13), which is supported by the Foundation for Fundamental Research on Matter (FOM) which is part of the Netherlands Organization for Scientific Research (NWO).

Funding

This work is part of the research program entitled “Designing Dirac Carriers in Semiconductor Superlattices” (DDC13), which is supported by the Foundation for Fundamental Research on Matter (FOM) which is part of the Netherlands Organization for Scientific Research (NWO).

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Cite this

Iaru, C. M., Brodu, A., van Hoof, N. J. J., ter Huurne, S. E. T., Buhot, J., Montanarella, F., Buhbut, S., Christianen, P. C. M., Vanmaekelbergh, D., de Mello Donega, C., Rivas, J. G., Koenraad, P. M., & Silov, A. Y. (2021). Fröhlich interaction dominated by a single phonon mode in CsPbBr₃. Nature Communications, 12(1), Article 5844. https://doi.org/10.1038/s41467-021-26192-0

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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 Fr{\"o}hlich 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 Fr{\"o}hlich 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 Fr{\"o}hlich 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.",

author = "Iaru, {Claudiu M.} and Annalisa Brodu and {van Hoof}, {Niels J.J.} and {ter Huurne}, {Stan E.T.} and Jonathan Buhot and Federico Montanarella and Sophia Buhbut and Christianen, {Peter C.M.} and Dani{\"e}l Vanmaekelbergh and {de Mello Donega}, Celso and Rivas, {Jaime G{\`o}mez} and Koenraad, {Paul M.} and Silov, {Andrei Yu}",

note = "Funding Information: This work is part of the research program entitled “Designing Dirac Carriers in Semiconductor Superlattices” (DDC13), which is supported by the Foundation for Fundamental Research on Matter (FOM) which is part of the Netherlands Organization for Scientific Research (NWO). ",

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AU - de Mello Donega, Celso

AU - Rivas, Jaime Gòmez

AU - Koenraad, Paul M.

AU - Silov, Andrei Yu

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