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  4. A theoretical perspective of the ultrafast transient absorption dynamics of CsPbBr3
 
research article

A theoretical perspective of the ultrafast transient absorption dynamics of CsPbBr3

Boziki, Ariadni  
•
Baudin, Pablo  
•
Liberatore, Elisa  
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February 11, 2022
Journal Of Computational Chemistry

Transient absorption spectra (TAS) of lead halide perovskites can provide important insights into the nature of the photoexcited state dynamics of this prototypical class of materials. Here, we perform ground and excited state molecular dynamics (MD) simulations within a restricted open shell Kohn-Sham (ROKS) approach in order to interpret the characteristic features of the TAS of CsPbBr3. Our results reveal that properties such as the finite temperature band gap, the Stokes shift, and therefore, also the TAS are strongly size-dependent. Our TAS simulations show an early positive red-shifted feature on the fs scale that can be explained by geometric relaxation in the excited state. As excited-state processes can crucially affect the electronic properties of this class of photoactive materials, our observations are an important ingredient for further optimization of lead halide based optoelectronic devices.

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Type
research article
DOI
10.1002/jcc.26815
Web of Science ID

WOS:000753892500001

Author(s)
Boziki, Ariadni  
Baudin, Pablo  
Liberatore, Elisa  
Astani, Negar Ashari  
Rothlisberger, Ursula  
Date Issued

2022-02-11

Publisher

WILEY

Published in
Journal Of Computational Chemistry
Volume

43

Issue

8

Start page

577

End page

582

Subjects

Chemistry, Multidisciplinary

•

Chemistry

•

absorption spectra

•

cspbbr3

•

excited state dynamics

•

molecular dynamics

•

roks

•

stokes shifts

•

transient absorption spectra

•

dependent stokes shift

•

molecular-dynamics

•

halide perovskites

•

charge-carriers

•

solar-cell

•

electron

•

cesium

•

pseudopotentials

•

evolution

•

exchange

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCBC  
Available on Infoscience
February 28, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/185800
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