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Multiphoton excited singlet/triplet mixed self-trapped exciton emission.

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Zhou, Rui 
Sui, Laizhi 
Liu, Xinbao 
Guo, Dengyang 


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.


Acknowledgements: This work was supported by the National Natural Science Foundation of China (Grant Nos. 62075198, 11974317, 12274378), Outstanding Youth Foundation of Henan (Grant Nos. 222300420087).


Article, /639/624/399/354, /639/301/357/354, /123, /132, /128, article

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Nat Commun

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Springer Science and Business Media LLC