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  4. Disentangling Thermal from Electronic Contributions in the Spectral Response of Photoexcited Perovskite Materials
 
research article

Disentangling Thermal from Electronic Contributions in the Spectral Response of Photoexcited Perovskite Materials

Wang, Lijie  
•
Nughays, Razan
•
Rossi, Thomas Charles Henry  
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February 15, 2024
Journal Of The American Chemical Society

Disentangling electronic and thermal effects in photoexcited perovskite materials is crucial for photovoltaic and optoelectronic applications but remains a challenge due to their intertwined nature in both the time and energy domains. In this study, we employed temperature-dependent variable-angle spectroscopic ellipsometry, density functional theory calculations, and broadband transient absorption spectroscopy spanning the visible to mid-to-deep-ultraviolet (UV) ranges on MAPbBr(3) thin films. The use of deep-UV detection opens a new spectral window that enables the exploration of high-energy excitations at various symmetry points within the Brillouin zone, facilitating an understanding of the ultrafast responses of the UV bands and the underlying mechanisms governing them. Our investigation reveals that the photoinduced spectral features remarkably resemble those generated by pure lattice heating, and we disentangle the relative thermal and electronic contributions and their evolutions at different delay times using combinations of decay-associated spectra and temperature-induced differential absorption. The results demonstrate that the photoinduced transients possess a significant thermal origin and cannot be attributed solely to electronic effects. Following photoexcitation, as carriers (electrons and holes) transfer their energy to the lattice, the thermal contribution increases from similar to 15% at 1 ps to similar to 55% at 500 ps and subsequently decreases to similar to 35-50% at 1 ns. These findings elucidate the intricate energy exchange between charge carriers and the lattice in photoexcited perovskite materials and provide insights into the limited utilization efficiency of photogenerated charge carriers.

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Type
research article
DOI
10.1021/jacs.3c12832
Web of Science ID

WOS:001166556600001

Author(s)
Wang, Lijie  
•
Nughays, Razan
•
Rossi, Thomas Charles Henry  
•
Oppermann, Malte  
•
Ogieglo, Wojciech
•
Bian, Tieyuan
•
Shih, Chun-Hua
•
Guo, Tzung-Fang
•
Pinnau, Ingo
•
Yin, Jun
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Date Issued

2024-02-15

Publisher

Amer Chemical Soc

Published in
Journal Of The American Chemical Society
Volume

146

Issue

8

Start page

5393

End page

5401

Subjects

Physical Sciences

•

Halide Perovskite

•

Phonon Bottleneck

•

Dynamics

•

Films

•

Spectroscopy

•

Transition

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSU  
FunderGrant Number

European Research Council

695197

European Research Council

Swiss NSF via the NCCR: MUST

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Available on Infoscience
April 3, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/206806
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