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Quantifying photoinduced polaronic distortions in inorganic lead halide perovskites nanocrystals

Oliviero Cannelli1, Nicola Colonna2,3*, Michele Puppin1, Thomas Rossi1, Dominik Kinschel1, Ludmila Leroy1,4, Janina Löffler1, Anne Marie March5, Gilles Doumy5, Andre Al Haddad5, Ming-Feng Tu5, Yoshiaki Kumagai5, Donald Walko6, Grigory Smolentsev7, Franziska Krieg8,9, Simon C. Boehme8,9, Maksym V. Kovalenko8,9, Majed Chergui1, Giulia F. Mancini1,10

1 École Polytechnique Fédérale de Lausanne, Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), CH-1015 Lausanne, Switzerland.

2 Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institute, CH-5232 Villigen-PSI, Switzerland.

3 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

4 LabCri, Universidade Federal de Minas Gerais, Belo Horizonte, Brazil.

5 Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, IL 60439, USA

6 Advanced Photon Source, Argonne National Laboratory, 9700 S. Cass Ave, Lemont, IL, 60439, USA.

7 Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland.

8 Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland.

9 Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland

10 Department of Physics, University of Pavia, I-27100 Pavia, Italy

* Corresponding authors emails: nicola.colonna@psi.ch
DOI10.24435/materialscloud:2p-e8 [version v1]

Publication date: Oct 25, 2021

How to cite this record

Oliviero Cannelli, Nicola Colonna, Michele Puppin, Thomas Rossi, Dominik Kinschel, Ludmila Leroy, Janina Löffler, Anne Marie March, Gilles Doumy, Andre Al Haddad, Ming-Feng Tu, Yoshiaki Kumagai, Donald Walko, Grigory Smolentsev, Franziska Krieg, Simon C. Boehme, Maksym V. Kovalenko, Majed Chergui, Giulia F. Mancini, Quantifying photoinduced polaronic distortions in inorganic lead halide perovskites nanocrystals, Materials Cloud Archive 2021.167 (2021), doi: 10.24435/materialscloud:2p-e8.


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.

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Time-dependent X-Ray absorption Halide Perovskites Fröhilch polarons Electron-phonon coupling MARVEL SNSF H2020

Version history:

2021.167 (version v1) [This version] Oct 25, 2021 DOI10.24435/materialscloud:2p-e8