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Communication Dans Un Congrès Année : 2022

Unusual anharmonicity and pseudospin-phonon dynamics in 3D halide perovskites

Résumé

3D halide perovskites used in light emitters and PV systems exhibit an unusual anharmonicity, which is not accounted for in nowadays descriptions of phonons and electron-phonon coupling. Therefore, the low frequency lattice vibrations and relaxations were 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 related to structural phase transitions. 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. 3D halide perovskites are therefore in a very unusual situation where anharmonicity prevails. It is leading to partial, extensive and ultraslow critical and stochatic dynamics connected to structural instabilities. The extensive disorder of the lattice at normal operation temperatures for devices is similar to premelting where only long-range acoustic normal modes survive.
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Dates et versions

hal-03949021 , version 1 (20-01-2023)

Identifiants

  • HAL Id : hal-03949021 , version 1

Citer

Jacky Even, Bernard Hehlen, Philippe Bourges, Benoit Rufflé, Antoine Létoublon, et al.. Unusual anharmonicity and pseudospin-phonon dynamics in 3D halide perovskites. International Conference on Emerging Light Emitting Materials (EMLEM 2022), Oct 2022, Limassol, Cyprus. ⟨hal-03949021⟩
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