Carrier Lifetimes and Polaronic Mass Enhancement in the Hybrid Halide Perovskite CH3NH3PbI3 from Multiphonon Fröhlich Coupling

We elucidate the nature of the electron-phonon interaction in the archetypal hybrid perovskite CH3NH3PbI3 using ab initio many-body calculations and an exactly solvable model. We demonstrate that electrons and holes near the band edges primarily interact with three distinct groups of longitudinal-op...

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Bibliographic Details
Published in:Physical review letters 2018-08, Vol.121 (8), p.086402
Main Authors: Schlipf, Martin, Poncé, Samuel, Giustino, Feliciano
Format: Article
Language:English
Subjects:
Electron phonon interactions
Libration
Many body problem
Perovskites
Phonons
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Summary:We elucidate the nature of the electron-phonon interaction in the archetypal hybrid perovskite CH3NH3PbI3 using ab initio many-body calculations and an exactly solvable model. We demonstrate that electrons and holes near the band edges primarily interact with three distinct groups of longitudinal-optical vibrations, in order of importance: the stretching of the Pb-I bond, the bending of the Pb-I-Pb bonds, and the libration of the organic cations. These polar phonons induce ultrafast intraband carrier relaxation over timescales of 6–30 fs and yield polaron effective masses 28% heavier than the bare band masses. These findings allow us to rationalize previous experimental observations and provide a key to understanding carrier dynamics in halide perovskites.
ISSN:0031-9007
1079-7114
DOI:10.1103/PhysRevLett.121.086402