2026-06-03T14:54:06Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:785 2021-10-25T14:37:31Z openaire_data community-mcarchive

Colonna, Nicola Cannelli, Oliviero Colonna, Nicola Puppin, Michele Rossi, Thomas Kinschel, Dominik Leroy, Ludmila Löffler, Janina March, Anne Marie Doumy, Gilles Haddad, Andre Al Tu, Ming-Feng Kumagai, Yoshiaki Walko, Donald Smolentsev, Grigory Krieg, Franziska Boehme, Simon C. Kovalenko, Maksym V. Chergui, Majed Mancini, Giulia F. 2021-10-25 The development of next generation perovskite-based optoelectronic devices relies critically on the understanding of the interaction between charge carriers and the polar lattice in out-of-equilibrium conditions. While it has become increasingly evident for CsPbBr3 perovskites that the Pb-Br framework flexibility plays a key role in their light-activated functionality, the corresponding local structural rearrangement has not yet been unambiguously identified. In this work, we demonstrate that the photoinduced lattice changes in the system are due to a specific polaronic distortion, associated with the activation of a longitudinal optical phonon mode at 18 meV by electron-phonon coupling, and we quantify the associated structural changes with atomic-level precision. Key to this achievement is the combination of time-resolved and temperature-dependent studies at Br K-edge and Pb L3-edge X-ray absorption with refined ab-initio simulations, which fully account for the screened core-hole final state effects on the X-ray absorption spectra. From the temporal kinetics, we show that carrier recombination reversibly unlocks the structural deformation at both Br and Pb sites. The comparison with the temperature-dependent XAS results rules out thermal effects as the primary source of distortion of the Pb-Br bonding motif during photoexcitation. Our work provides a comprehensive description of the CsPbBr3 perovskites photophysics, offering novel insights on the light-induced response of the system and its exceptional optoelectronic properties. application/gzip text/markdown text/plain https://doi.org/10.24435/materialscloud:2p-e8 oai:materialscloud.org:785 mcid:2021.167 eng Materials Cloud https://arxiv.org/abs/2103.02575 https://doi.org/10.1021/jacs.1c02403 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:ch-j7 info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Time-dependent X-Ray absorption Halide Perovskites Fröhilch polarons Electron-phonon coupling MARVEL SNSF H2020 Quantifying photoinduced polaronic distortions in inorganic lead halide perovskites nanocrystals info:eu-repo/semantics/other