Quantifying photoinduced polaronic distortions in inorganic lead halide perovskites nanocrystals
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{
"revision": 9,
"id": "785",
"created": "2021-03-21T13:31:16.343284+00:00",
"metadata": {
"doi": "10.24435/materialscloud:2p-e8",
"status": "published",
"title": "Quantifying photoinduced polaronic distortions in inorganic lead halide perovskites nanocrystals",
"mcid": "2021.167",
"license_addendum": null,
"_files": [
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"_oai": {
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"keywords": [
"Time-dependent X-Ray absorption",
"Halide Perovskites",
"Fr\u00f6hilch polarons",
"Electron-phonon coupling",
"MARVEL",
"SNSF",
"H2020"
],
"conceptrecid": "784",
"is_last": true,
"references": [
{
"type": "Preprint",
"url": "https://arxiv.org/abs/2103.02575",
"citation": "O. Cannelli et. al, arXiv:2103.02575 (2021)"
},
{
"type": "Journal reference",
"doi": "10.1021/jacs.1c02403",
"url": "https://doi.org/10.1021/jacs.1c02403",
"comment": "Paper in which the data and results are desribed",
"citation": "O. Cannelli, et al., Journal of the American Chemical Society, 143, 9048\u22129059 (2021)"
}
],
"publication_date": "Oct 25, 2021, 14:37:31",
"license": "Creative Commons Attribution 4.0 International",
"id": "785",
"description": "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.",
"version": 1,
"contributors": [
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "Cannelli",
"givennames": "Oliviero"
},
{
"email": "nicola.colonna@psi.ch",
"affiliations": [
"Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institute, CH-5232 Villigen-PSI, Switzerland.",
"National Centre for Computational Design and Discovery of Novel Materials (MARVEL), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, CH-1015 Lausanne, Switzerland"
],
"familyname": "Colonna",
"givennames": "Nicola"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "Puppin",
"givennames": "Michele"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "Rossi",
"givennames": "Thomas"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "Kinschel",
"givennames": "Dominik"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland.",
"LabCri, Universidade Federal de Minas Gerais, Belo Horizonte, Brazil."
],
"familyname": "Leroy",
"givennames": "Ludmila"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "L\u00f6ffler",
"givennames": "Janina"
},
{
"affiliations": [
"Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA"
],
"familyname": "March",
"givennames": "Anne Marie"
},
{
"affiliations": [
"Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA"
],
"familyname": "Doumy",
"givennames": "Gilles"
},
{
"affiliations": [
"Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA"
],
"familyname": "Haddad",
"givennames": "Andre Al"
},
{
"affiliations": [
"Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA"
],
"familyname": "Tu",
"givennames": "Ming-Feng"
},
{
"affiliations": [
"Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA"
],
"familyname": "Kumagai",
"givennames": "Yoshiaki"
},
{
"affiliations": [
"Advanced Photon Source, Argonne National Laboratory, 9700 S. Cass Ave, Lemont, IL, 60439, USA."
],
"familyname": "Walko",
"givennames": "Donald"
},
{
"affiliations": [
"Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland."
],
"familyname": "Smolentsev",
"givennames": "Grigory"
},
{
"affiliations": [
"Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Z\u00fcrich, Vladimir Prelog Weg 1, CH-8093 Z\u00fcrich, Switzerland.",
"Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, CH-8600 D\u00fcbendorf, Switzerland"
],
"familyname": "Krieg",
"givennames": "Franziska"
},
{
"affiliations": [
"Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Z\u00fcrich, Vladimir Prelog Weg 1, CH-8093 Z\u00fcrich, Switzerland.",
"Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, CH-8600 D\u00fcbendorf, Switzerland"
],
"familyname": "Boehme",
"givennames": "Simon C."
},
{
"affiliations": [
"Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Z\u00fcrich, Vladimir Prelog Weg 1, CH-8093 Z\u00fcrich, Switzerland.",
"Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, CH-8600 D\u00fcbendorf, Switzerland"
],
"familyname": "Kovalenko",
"givennames": "Maksym V."
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland."
],
"familyname": "Chergui",
"givennames": "Majed"
},
{
"affiliations": [
"\u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland.",
"Department of Physics, University of Pavia, I-27100 Pavia, Italy"
],
"familyname": "Mancini",
"givennames": "Giulia F."
}
],
"edited_by": 100
},
"updated": "2021-10-25T12:37:31.870276+00:00"
}