The family of two-dimensional (2D) layered materials with strong excitonic effect offers fascinating opportunities for studying excited state exciton behavior at 2D limit. While exciton dynamics in conventional 2D semiconductors (e.g. transition metal dichalcogenides) has been extensively studied, little is known about exciton properties and dynamics in 2D layered semiconductors with strong electron/exciton-phonon coupling. Here, by combining experimental and theoretical approaches, we reveal the intrinsic highly localized exciton (i.e. self-trapped exciton) in 2D layered As2S3, driven by strong exciton-phonon interaction. It is shown that photoexcited electron/hole charges in As2S3 localize spontaneously in ~110 fs, giving rise to large stokes-shifted and broad photoluminescence. An interlayer partial bond is formed between chalcogen atoms, triggering lattice distortion and carrier localization. Together with Urbach-Martienssen analysis, this study provides a comprehensive physical picture to understand the complex interplay between exciton and lattice dynamics in 2D semiconductors, which has strong implications to their optoelectronic properties and applications.
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Ultrafast intrinsic excited state localization m 2D layered As2S3 by interlayer bond formation†
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December 2023
Research Article|
December 01 2023
Ultrafast intrinsic excited state localization m 2D layered As2S3 by interlayer bond formation†
Special Collection:
Virtual Issue on Ultrafast Spectroscopy (2023)
Xufeng Li;
Xufeng Li
‡
a
Department of Chemistry, Zhejiang University
, Hangzhou 310027, China
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Li Yao;
Li Yao
‡
b
Department of Physics, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and ICQD /Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
, Hefei 230026, China
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Weijian Tao;
Weijian Tao
a
Department of Chemistry, Zhejiang University
, Hangzhou 310027, China
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Jin Zhao;
Jin Zhao
*
b
Department of Physics, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and ICQD /Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
, Hefei 230026, China
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Haiming Zhu
Haiming Zhu
*
a
Department of Chemistry, Zhejiang University
, Hangzhou 310027, China
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Chin. J. Chem. Phys. 36, 646–654 (2023)
Article history
Received:
November 10 2023
Accepted:
November 28 2023
Citation
Xufeng Li, Li Yao, Weijian Tao, Jin Zhao, Haiming Zhu; Ultrafast intrinsic excited state localization m 2D layered As2S3 by interlayer bond formation. Chin. J. Chem. Phys. 1 December 2023; 36 (6): 646–654. https://doi.org/10.1063/1674-0068/cjcp2311112
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