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Luminescence clusters composed of organic ligands and metals have gained significant interests as scintillators owing to their great potential in high X-ray absorption, customizable radioluminescence, and solution processability at low temperatures. However, X-ray luminescence efficiency in clusters is primarily governed by the competition between radiative states from organic ligands and nonradiative cluster-centered charge transfer. Here we report that a class of Cu4I4 cubes exhibit highly emissive radioluminescence in response to X-ray irradiation through functionalizing biphosphine ligands with acridine. Mechanistic studies show that these clusters can efficiently absorb radiation ionization to generate electron-hole pairs and transfer them to ligands during thermalization for efficient radioluminescence through precise control over intramolecular charge transfer. Our experimental results indicate that copper/iodine-to-ligand and intraligand charge transfer states are predominant in radiative processes. We demonstrate that photoluminescence and electroluminescence quantum efficiencies of the clusters reach 95% and 25.6%, with the assistance of external triplet-to-singlet conversion by a thermally activated delayed fluorescence matrix. We further show the utility of the Cu4I4 scintillators in achieving a lowest X-ray detection limit of 77 nGy s(-1) and a high X-ray imaging resolution of 12 line pairs per millimeter. Our study offers insights into universal luminescent mechanism and ligand engineering of cluster scintillators. X-ray luminescence efficiency of copper halide clusters is limited by nonradiative charge transfer. Here, Zhang et al. report highly emissive radioluminescence of Cu4I4 cubes by functionalizing biphosphine ligands with acridine, unlocking the potential use as low-cost and eco-friendly scintillators.
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NATURE COMMUNICATIONS
ISSN: 2041-1723
Year: 2023
Issue: 1
Volume: 14
1 4 . 7
JCR@2023
1 4 . 7 0 0
JCR@2023
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 0
SCOPUS Cited Count: 7
ESI Highly Cited Papers on the List: 2 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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