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

DOI

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
DOI https://doi.org/10.24435/materialscloud:wg-d5
Related Identifier https://doi.org/10.1103/PhysRevLett.121.086402
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:h6-eg
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:847
Provenance
Creator Schlipf, Martin; Poncé, Samuel; Giustino, Feliciano
Publisher Materials Cloud
Contributor Schlipf, Martin; Poncé, Samuel; Giustino, Feliciano
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 info:eu-repo/semantics/other
Format application/gzip; text/markdown
Discipline Materials Science and Engineering