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  4. Quantifying Photoinduced Polaronic Distortions in Inorganic Lead Halide Perovskite Nanocrystals
 
research article

Quantifying Photoinduced Polaronic Distortions in Inorganic Lead Halide Perovskite Nanocrystals

Cannelli, Oliviero  
•
Colonna, Nicola  
•
Puppin, Michele  
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June 23, 2021
Journal Of The American Chemical Society

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 timeresolved and temperature-dependent studies at Br K and Pb L-3 X-ray absorption edges 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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Type
research article
DOI
10.1021/jacs.1c02403
Web of Science ID

WOS:000667994700014

Author(s)
Cannelli, Oliviero  
Colonna, Nicola  
Puppin, Michele  
Rossi, Thomas C.  
Kinschel, Dominik  
Leroy, Ludmila M. D.  
Loeffler, Janina
Budarz, James M.  
March, Anne Marie
Doumy, Gilles
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Date Issued

2021-06-23

Published in
Journal Of The American Chemical Society
Volume

143

Issue

24

Start page

9048

End page

9059

Subjects

Chemistry, Multidisciplinary

•

Chemistry

•

phase-transitions

•

electron

•

crystal

•

cspbbr3

•

transport

•

dynamics

•

lengths

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

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LUMES  
Available on Infoscience
July 31, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/180381
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