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Luminescent metal halides doped with ns2-metal ions such as 6s2-metal Bi3+ have aroused reviving interest owing to their outstanding optical properties; however, the origin of the photoluminescence (PL) remains controversial and unclear. Herein, we report a strategy for the controlled synthesis of Bi3+-doped vacancy-ordered double perovskite Cs2SnCl6 nanocrystals (NCs) and unravel the triplet excited-state dynamics of Bi3+ through temperature-dependent PL and ultrafast femtosecond transient absorption spectroscopies. Owing to the aliovalent Bi3+ doping in the spatially confined zero-dimensional (0D) structure of Cs2SnCl6, Bi3+ ions experience an enhancive Jahn-Teller distortion in the excited state, which results in intense broadband blue PL originating from the inter-configurational 3P0,11S0 transitions of Bi3+ at 450 nm, with a large Stokes shift and a quantum yield of 35.2%. Specifically, an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K to μs at 300 K were observed, as solid evidence for the isolated Bi3+ emission. These findings clarify the controversy about the PL origin in ns2-metal ion-doped lead-free luminescent metal halides, thereby paving the way for exploring their optoelectronic applications.

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Publication history
Copyright
Acknowledgements

Publication history

Received: 25 January 2022
Revised: 27 February 2022
Accepted: 27 February 2022
Published: 25 April 2022
Issue date: July 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work is supported by the National Natural Science Foundation of China (NSFC, Nos. 12074379, U1805252, 21875250, 12074380, 11904365, and 12004384), and the Chinese Academy of Sciences/State Administration of Foreign Experts Affairs (CAS/SAFEA) International Partnership Program for Creative Research Teams.

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