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-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.

Identifier
Source https://archive.materialscloud.org/record/2021.71
Metadata Access https://archive.materialscloud.org/xml?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:847
Provenance
Creator Schlipf, Martin; Poncé, Samuel; Giustino, Feliciano
Publisher Materials Cloud
Publication Year 2021
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type Dataset
Discipline Materials Science and Engineering