Published May 7, 2021 | Version v1
Dataset Open

Carrier lifetimes and polaronic mass enhancement in the hybrid halide perovskite CH₃NH₃PbI₃ from multiphonon Fröhlich coupling

  • 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

* Contact person

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.

Files

File preview

files_description.md

All files

Files (13.9 MiB)

Name Size
md5:eb914b911e7073310320aa6c380cdb34
220 Bytes Preview Download
md5:8b36455da5fe8cb55bf65f8c373ea2a8
1.1 KiB Preview Download
md5:3497b3156cda1564c25a6ddbd1b29aa8
13.9 MiB Download

References

Journal reference
M. Schlipf, S. Poncé, and F. Giustino, Phys. Rev. Lett. 121, 086402 (2018), doi: 10.1103/PhysRevLett.121.086402