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arXiv · 1808.08130

Carrier Lifetimes and Polaronic Mass Enhancement in the Hybrid Halide Perovskite CH$_3$NH$_3$PbI$_3$ from Multiphonon Fröhlich Coupling

Martin Schlipf·Samuel Poncé·Feliciano Giustino
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Abstract

We elucidate the nature of the electron-phonon interaction in the archetypal hybrid perovskite CH$_3$NH$_3$PbI$_3$ 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.

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Martin Schlipf, Samuel Poncé, Feliciano Giustino. 2018-08-24. Carrier Lifetimes and Polaronic Mass Enhancement in the Hybrid Halide Perovskite CH$_3$NH$_3$PbI$_3$ from Multiphonon Fröhlich Coupling. https://doi.org/10.1103/physrevlett.121.086402

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