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Electronic States Modulation by Coherent Optical Phonons in 2D Halide Perovskites

Fu, Jianhui ; Li, Mingjie ; Solanki, Ankur ; Xu, Qiang ; Lekina, Yulia ; Ramesh, Sankaran LU orcid ; Shen, Ze Xiang and Sum, Tze Chien (2021) In Advanced Materials 33(11).
Abstract

Excitonic effects underpin the fascinating optoelectronic properties of 2D perovskites that are highly favorable for photovoltaics and light-emitting devices. Analogous to switching in transistors, manipulating these excitonic properties in 2D perovskites using coherent phonons could unlock new applications. Presently, a detailed understanding of this underlying mechanism remains modest. Herein, the origins of the carrier-phonon coupling in 2D perovskites using transient absorption (TA) spectroscopy are explicated. The exciton fine structure is modulated by coherent optical phonons dominated by the vibrational motion of the PbI6 octahedra via deformation potential. Originating from impulsive stimulated Raman scattering, these... (More)

Excitonic effects underpin the fascinating optoelectronic properties of 2D perovskites that are highly favorable for photovoltaics and light-emitting devices. Analogous to switching in transistors, manipulating these excitonic properties in 2D perovskites using coherent phonons could unlock new applications. Presently, a detailed understanding of this underlying mechanism remains modest. Herein, the origins of the carrier-phonon coupling in 2D perovskites using transient absorption (TA) spectroscopy are explicated. The exciton fine structure is modulated by coherent optical phonons dominated by the vibrational motion of the PbI6 octahedra via deformation potential. Originating from impulsive stimulated Raman scattering, these coherent vibrations manifest as oscillations in the TA spectrum comprising of the generation and detection processes of coherent phonons. This two-step process leads to a unique pump- and probe-energy dependence of the phonon modulation determined by the imaginary part of the refractive index and its derivative, respectively. The phonon frequency and lattice displacement of the inorganic octahedra are highly dependent on the organic cation. This study injects fresh insights into the exciton–phonon coupling of 2D perovskites relevant for emergent optoelectronics development.

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author
; ; ; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
subject
keywords
coherent optical phonons, deformation potential, exciton–phonon coupling, impulsive stimulated Raman scattering
in
Advanced Materials
volume
33
issue
11
article number
2006233
publisher
John Wiley & Sons Inc.
external identifiers
  • pmid:33576093
  • scopus:85101036891
ISSN
0935-9648
DOI
10.1002/adma.202006233
language
English
LU publication?
no
additional info
Publisher Copyright: © 2021 Wiley-VCH GmbH
id
28352f16-2b8e-4302-a451-659a2df49b37
date added to LUP
2023-02-15 22:06:07
date last changed
2024-06-15 02:50:25
@article{28352f16-2b8e-4302-a451-659a2df49b37,
  abstract     = {{<p>Excitonic effects underpin the fascinating optoelectronic properties of 2D perovskites that are highly favorable for photovoltaics and light-emitting devices. Analogous to switching in transistors, manipulating these excitonic properties in 2D perovskites using coherent phonons could unlock new applications. Presently, a detailed understanding of this underlying mechanism remains modest. Herein, the origins of the carrier-phonon coupling in 2D perovskites using transient absorption (TA) spectroscopy are explicated. The exciton fine structure is modulated by coherent optical phonons dominated by the vibrational motion of the PbI<sub>6</sub> octahedra via deformation potential. Originating from impulsive stimulated Raman scattering, these coherent vibrations manifest as oscillations in the TA spectrum comprising of the generation and detection processes of coherent phonons. This two-step process leads to a unique pump- and probe-energy dependence of the phonon modulation determined by the imaginary part of the refractive index and its derivative, respectively. The phonon frequency and lattice displacement of the inorganic octahedra are highly dependent on the organic cation. This study injects fresh insights into the exciton–phonon coupling of 2D perovskites relevant for emergent optoelectronics development.</p>}},
  author       = {{Fu, Jianhui and Li, Mingjie and Solanki, Ankur and Xu, Qiang and Lekina, Yulia and Ramesh, Sankaran and Shen, Ze Xiang and Sum, Tze Chien}},
  issn         = {{0935-9648}},
  keywords     = {{coherent optical phonons; deformation potential; exciton–phonon coupling; impulsive stimulated Raman scattering}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{11}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Materials}},
  title        = {{Electronic States Modulation by Coherent Optical Phonons in 2D Halide Perovskites}},
  url          = {{http://dx.doi.org/10.1002/adma.202006233}},
  doi          = {{10.1002/adma.202006233}},
  volume       = {{33}},
  year         = {{2021}},
}