Phonon anharmonicity, lifetimes and thermal transport in CH$_3$NH$_3$PbI$_3$ from many-body perturbation theory

Abstract

Lattice vibrations in CH$_3$NH$_3$PbI$_3$ are strongly interacting, with double well instabilities present at the Brillouin zone boundary. Analysis within a first-principles lattice dynamics framework reveals anharmonic potentials with short phonon quasi-particle lifetimes and mean-free paths. The phonon behaviour is distinct from the inorganic semiconductors GaAs and CdTe where three-phonon interaction strengths are three orders of magnitude smaller. The implications for the applications of hybrid halide perovskites arising from thermal conductivity, band-gap deformation, and charge-carrier scattering through electron-phonon coupling, are presented.