TY - JOUR
T1 - Fröhlich interaction dominated by a single phonon mode in CsPbBr3
AU - Iaru, Claudiu M.
AU - Brodu, Annalisa
AU - van Hoof, Niels J.J.
AU - ter Huurne, Stan E.T.
AU - Buhot, Jonathan
AU - Montanarella, Federico
AU - Buhbut, Sophia
AU - Christianen, Peter C.M.
AU - Vanmaekelbergh, Daniël
AU - de Mello Donega, Celso
AU - Rivas, Jaime Gòmez
AU - Koenraad, Paul M.
AU - Silov, Andrei Yu
N1 - 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).
PY - 2021/12
Y1 - 2021/12
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85116475028&partnerID=8YFLogxK
U2 - 10.1038/s41467-021-26192-0
DO - 10.1038/s41467-021-26192-0
M3 - Article
C2 - 34615880
AN - SCOPUS:85116475028
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 5844
ER -