title: The mechanism of slow hot-hole cooling in lead-iodide perovskite: first-principles calculation on carrier lifetime from electron-phonon interaction.
abstract: We report on an analysis of hot-carrier lifetimes from electron-phonon interaction in lead iodide perovskites using first-principles calculations. Our calculations show that the holes in CsPbI3 have very long lifetimes in the valence band region situated 0.6 eV below the top of the valence band. On the other hand, no long lifetime is predicted in PbI3(-). These different results reflect the different electronic density of states (DOSs) in the valence bands, that is, a small DOS for the former structure while a sharp DOS peak for the latter structure. We propose a reduction of the relaxation paths in the small valence DOS as being the origin of the slow hot-hole cooling. Analyzing the generalized Eliashberg functions, we predict that different perovskite A-site cations do not have an impact on the carrier decay mechanism. The similarity between the DOS structures of CsPbI3 and CH3NH3PbI3 enables us to extend the description of the decay mechanism of fully inorganic CsPbI3 to its organic-inorganic counterpart, CH3NH3PbI3.
authors: †Department of Chemical System Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.|‡CREST-JST, 7 Gobancho, Chiyoda-ku, Tokyo 102-0076, Japan.
authors: Hiroki
authors: H
authors: Kawai
authors: †Department of Chemical System Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.|‡CREST-JST, 7 Gobancho, Chiyoda-ku, Tokyo 102-0076, Japan.
authors: Giacomo
authors: G
authors: Giorgi
authors: §Istituto di Struttura della Materia of the National Research Council and European Theoretical Spectroscopy Facility (ETSF), Via Salaria Km 29.3, I-00016 Monterotondo Stazione, Italy.
authors: Andrea
authors: A
authors: Marini
authors: †Department of Chemical System Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.|‡CREST-JST, 7 Gobancho, Chiyoda-ku, Tokyo 102-0076, Japan.
authors: Koichi
authors: K
authors: Yamashita
keywords: Solar cells; carrier lifetime; density functional theory; many-body perturbation theory; mixed organic−inorganic halide perovskites