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Copper halides, a new class of attractive and potential scintillators, have attracted tremendous attention in X‐ray imaging. However, the ambiguity surrounding their exciton properties and the unclear effect of crystal structure on their photophysical performance hinder an in‐depth understanding of their luminescence mechanism and their further application in the X‐ray imaging field. Herein, copper halide scintillators Cs3Cu2X5 (X = I, Br, and Cl) with a 0D crystal structure is prepared, and their photophysical properties and luminescence mechanism are revealed using both theoretical calculation and experimental verification. The small exciton Bohr diameter together with the high exciton binding energy can cause Cs3Cu2X5 to hold strongly confined excitons and lack quantum‐size effects. The 0D Cs3Cu2X5 materials exhibit a structural framework with a soft crystal lattice and Frenkel excitons with strong confinement effects, further resulting in a luminescence mechanism with self‐trapped excitons. In particular, Cs3Cu2I5 is demonstrated as an efficient scintillator with high radioluminescence efficiency and high spatial resolution of ≈106 µm in radiography, which is primarily attributed to strongly confined excitons to improve the radiative recombination probability of electron‐hole pairs. Overall, this work provides a pathway for developing 0D scintillators with strongly confined excitons to improve X‐ray imaging performance. [ABSTRACT FROM AUTHOR]

Scintillators for radiation detection are of great significance in medical imaging, security, and nondestructive inspection. The current challenge for scintillators is to simultaneously achieve high scintillation light yield, fast radioluminescence, simple film fabrication, large X‐ray attenuation efficiency as well as stable and nontoxic compositions; no previous scintillators fulfill all the above requirements. Here, metal halide Rb2AgBr3, possessing defect‐bound excitonic radioluminescence, is shown as efficient and fast scintillators. This nontoxic and stable scintillator emits from excitons bound to neutral bromine vacancies, enjoying an efficient and spin‐allowed fast emission with minimized self‐absorption. Rb2AgBr3 thus has a high light yield (25 600 photons MeV−1), fast scintillation decay time (5.31 ns), and a record value of light yield versus decay time (4821 photons MeV−1 ns−1). The close‐space sublimation method is developed for fast and scalable fabrication of oriented Rb2AgBr3 films. The scintillator film is further integrated with commercial flat‐panel imagers, and the spatial resolution reaches 10.2 line pairs per millimeter at the modulation transfer function of 0.2, doubling the resolution of conventional CsI:Tl flat‐panel detectors. The dynamic X‐ray imaging and its use to real‐time monitoring of bone movement without ghosting effect is also demonstrated. [ABSTRACT FROM AUTHOR]