Martin Schlipf^1*, Samuel Poncé^1*, Feliciano Giustino^1,2*

1 Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, United Kingdom

2 Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14853, USA

* Corresponding authors emails: martin.schlipf@gmail.com, samuel.pon@gmail.com, feliciano.giustino@materials.ox.ac.uk

DOI10.24435/materialscloud:wg-d5 [version v1]

Publication date: May 07, 2021

How to cite this record

Martin Schlipf, Samuel Poncé, Feliciano Giustino, Carrier lifetimes and polaronic mass enhancement in the hybrid halide perovskite CH₃NH₃PbI₃ from multiphonon Fröhlich coupling, Materials Cloud Archive 2021.71 (2021), doi: 10.24435/materialscloud:wg-d5.

Description

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.

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Keywords

Electron-phonon coupling First-principles calculations Semiconductors Perovskite CH3NH3PbI3 PRACE