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Scintillator-based X-ray imaging technology is widely applied in medical diagnostics and nondestructive detection. Low-dimensional metal halide perovskites (MHPs) offer great potential in scintillation applications due to their flexible crystal structures. However, achieving strongly localized excitonic emission in low-dimensional MHPs remains challenging to further improve the photoemission performance. Herein, we report an entropy-engineering strategy to construct four-element Cs2MCl6(M = Te4+, Sn4+, Zr4+, and Hf4+) vacancy-ordered double-perovskite scintillators for enhanced X-ray detection, demonstrating an 8-fold enhancement in photoluminescence quantum yield, a 17-fold enhancement in photoluminescence intensity, and a low detection limit of 50.3 nGy s–1. Structural characterizations combined with theoretical calculations reveal that increased configurational entropy induces intense lattice distortion in [MCl6]2–octahedral clusters, increasing exciton transport barriers. Femtosecond transient absorption and temperature-dependent spectroscopic analyses indicate that this four-element Cs2MCl6shows strong electron–phonon and energy interactions between confined exciton states in isolated [MCl6]2–octahedral structures, thus promoting photoluminescence emission. A flexible scintillation screen containing high-entropy Cs2MCl6achieves a high resolution of over 20 lp mm–1for X-ray imaging. This work presents enhanced emission of MHPs by entropy engineering, providing potential implications for radiation detection and other optoelectronic applications. © 2025 American Chemical Society
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ACS Nano
ISSN: 1936-0851
Year: 2025
Issue: 33
Volume: 19
Page: 30396-30406
1 5 . 8 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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