Intramolecular charge transfer enables highly-efficient X-ray luminescence in cluster scintillators

Nan Zhang, Lei Qu, Shuheng Dai, Guohua Xie, Chunmiao Han, Jing Zhang, Ran Huo, Huan Hu, Qiushui Chen (), Wei Huang and Hui Xu ()
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Nan Zhang: Heilongjiang University
Lei Qu: Heilongjiang University
Shuheng Dai: Fuzhou University
Guohua Xie: Wuhan University
Chunmiao Han: Heilongjiang University
Jing Zhang: Heilongjiang University
Ran Huo: Heilongjiang University
Huan Hu: Heilongjiang University
Qiushui Chen: Fuzhou University
Wei Huang: Northwestern Polytechnical University (NPU)
Hui Xu: Heilongjiang University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract 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.

Date: 2023
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DOI: 10.1038/s41467-023-38546-x

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