Multiphoton excited singlet/triplet mixed self-trapped exciton emission

Rui Zhou, Laizhi Sui, Xinbao Liu, Kaikai Liu (), Dengyang Guo, Wenbo Zhao, Shiyu Song, Chaofan Lv, Shu Chen, Tianci Jiang, Zhe Cheng, Sheng Meng and Chongxin Shan ()
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Rui Zhou: Zhengzhou University
Laizhi Sui: Chinese Academy of Sciences
Xinbao Liu: Chinese Academy of Sciences
Kaikai Liu: Zhengzhou University
Dengyang Guo: Zhengzhou University
Wenbo Zhao: Zhengzhou University
Shiyu Song: Zhengzhou University
Chaofan Lv: Zhengzhou University
Shu Chen: Zhengzhou University
Tianci Jiang: The First Affiliated Hospital of Zhengzhou University
Zhe Cheng: The First Affiliated Hospital of Zhengzhou University
Sheng Meng: Chinese Academy of Sciences
Chongxin Shan: Zhengzhou University

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Multiphoton excited luminescence is of paramount importance in the field of optical detection and biological photonics. Self-trapped exciton (STE) emission with self-absorption-free advantages provide a choice for multiphoton excited luminescence. Herein, multiphoton excited singlet/triplet mixed STE emission with a large full width at half-maximum (617 meV) and Stokes shift (1.29 eV) has been demonstrated in single-crystalline ZnO nanocrystals. Temperature dependent steady state, transient state and time-resolved electron spin resonance spectra demonstrate a mixture of singlet (63%) and triplet (37%) mixed STE emission, which contributes to a high photoluminescence quantum yield (60.5%). First-principles calculations suggest 48.34 meV energy per exciton stored by phonons in the distorted lattice of excited states, and 58 meV singlet-triplet splitting energy for the nanocrystals being consistent with the experimental measurements. The model clarifies long and controversial debates on ZnO emission in visible region, and the multiphoton excited singlet/triplet mixed STE emission is also observed.

Date: 2023
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DOI: 10.1038/s41467-023-36958-3

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