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Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals : the effect of surface layer

Lin, Weihua LU ; Liang, Mingli LU ; Niu, Yuran LU ; Chen, Zhesheng ; Cherasse, Marie ; Meng, Jie LU ; Zou, Xianshao LU ; Zhao, Qian ; Geng, Huifang LU and Papalazarou, Evangelos , et al. (2022) In Journal of Materials Chemistry C 10(44). p.16751-16760
Abstract

We investigate hot carrier (HC) cooling in two-dimensional (2D) perovskite single crystals by applying two complementary ultrafast spectroscopy techniques - transient absorption (TA) and time-resolved two-photon photoemission (TR-2PPE) spectroscopies. TR-2PPE directly maps the hot electron distribution and its dynamics in the conduction band to the detected photoelectron distribution. While TR-2PPE selectively probes the upper layer of the material, TA provides information on the whole bulk. Two cooling regimes are resolved in both techniques. The fast timescale of 100-200 fs is related to the electron scattering by longitudinal optical (LO) phonons and the slow timescale of 3-4 ps corresponds to the LO phonon relaxation. The HC cooling... (More)

We investigate hot carrier (HC) cooling in two-dimensional (2D) perovskite single crystals by applying two complementary ultrafast spectroscopy techniques - transient absorption (TA) and time-resolved two-photon photoemission (TR-2PPE) spectroscopies. TR-2PPE directly maps the hot electron distribution and its dynamics in the conduction band to the detected photoelectron distribution. While TR-2PPE selectively probes the upper layer of the material, TA provides information on the whole bulk. Two cooling regimes are resolved in both techniques. The fast timescale of 100-200 fs is related to the electron scattering by longitudinal optical (LO) phonons and the slow timescale of 3-4 ps corresponds to the LO phonon relaxation. The HC cooling dynamic of TA measurement has faster initial stage and higher starting temperature for the slower stage than in TR-2PPE measurements. Conclusions about spatial sensitivity of the cooling dynamics across the 2D perovskite single crystals constitute valuable information that can guide the future development of HC solar cells and thermoelectric applications based on 2D perovskites.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Materials Chemistry C
volume
10
issue
44
pages
16751 - 16760
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85141857462
ISSN
2050-7526
DOI
10.1039/d2tc03111f
language
English
LU publication?
yes
id
72221f3c-000e-4c34-963f-652e94376a74
date added to LUP
2023-01-13 14:18:46
date last changed
2023-11-21 15:38:48
@article{72221f3c-000e-4c34-963f-652e94376a74,
  abstract     = {{<p>We investigate hot carrier (HC) cooling in two-dimensional (2D) perovskite single crystals by applying two complementary ultrafast spectroscopy techniques - transient absorption (TA) and time-resolved two-photon photoemission (TR-2PPE) spectroscopies. TR-2PPE directly maps the hot electron distribution and its dynamics in the conduction band to the detected photoelectron distribution. While TR-2PPE selectively probes the upper layer of the material, TA provides information on the whole bulk. Two cooling regimes are resolved in both techniques. The fast timescale of 100-200 fs is related to the electron scattering by longitudinal optical (LO) phonons and the slow timescale of 3-4 ps corresponds to the LO phonon relaxation. The HC cooling dynamic of TA measurement has faster initial stage and higher starting temperature for the slower stage than in TR-2PPE measurements. Conclusions about spatial sensitivity of the cooling dynamics across the 2D perovskite single crystals constitute valuable information that can guide the future development of HC solar cells and thermoelectric applications based on 2D perovskites.</p>}},
  author       = {{Lin, Weihua and Liang, Mingli and Niu, Yuran and Chen, Zhesheng and Cherasse, Marie and Meng, Jie and Zou, Xianshao and Zhao, Qian and Geng, Huifang and Papalazarou, Evangelos and Marsi, Marino and Perfetti, Luca and Canton, Sophie E. and Zheng, Kaibo and Pullerits, Tönu}},
  issn         = {{2050-7526}},
  language     = {{eng}},
  month        = {{10}},
  number       = {{44}},
  pages        = {{16751--16760}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Journal of Materials Chemistry C}},
  title        = {{Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals : the effect of surface layer}},
  url          = {{http://dx.doi.org/10.1039/d2tc03111f}},
  doi          = {{10.1039/d2tc03111f}},
  volume       = {{10}},
  year         = {{2022}},
}