Pseudospin-phonon dynamics in lead halide hybrid perovskites
jacky even a, bernard hehlen b, philippe bourges c, benoit rufflé b, claudine katan d, antoine letoublon a
a Univ Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, F-35000 Rennes, France
b Laboratoire Charles Coulomb, UMR 5221, Université de Montpellier, 34095 Montpellier, France
c Laboratoire Léon Brillouin, CEA-CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette, France
d Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) - UMR 6226, F-35000 Rennes, France
Proceedings of Online Conference on Atomic-level Characterisation of Hybrid Perovskites (HPATOM2)
Online, Spain, 2022 February 2nd - 3rd
Organizers: Michael Hope and Eve Mozur
Invited Speaker, jacky even, presentation 001
DOI: https://doi.org/10.29363/nanoge.hpatom.2022.001
Publication date: 30th October 2021

The low frequency lattice vibrations and relaxations are investigated in single crystals of the four 3D hybrid organolead perovskites, MAPbBr3, FAPbBr3, MAPbI3, and FAPbI3, at the Brillouin zone center using Raman and Brillouin scattering and at the zone boundary using inelastic neutron scattering. The temperature dependence of the PbX6 lattice modes in the four compounds can be renormalized into universal curves and no soft vibration is observed excluding a displacive-like transitional dynamics. The reorientational (pseudospin) motions of the molecular cations exhibit a seemingly order-disorder character recalling that of plastic crystals, but attributed to a secondary order-parameter. At ultra-low frequency, a quasi-elastic component evidenced by Brillouin scattering and associated to the unresolved central peak observed in neutron scattering, is attributed to center of mass anharmonic motions and rattling of the molecular cations in the perovskite cavities. 

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