Polymer Anchoring of Copper‐Iodide Clusters for Dual‐Modal Radiation Detection

ABSTRACT Transparent, uniformly luminescent scintillator films are urgently needed for next‐generation X‐ray imaging and radiation detection. Conventional single‐crystal scintillators exhibit high performance yet are intrinsically brittle and costly, while physical blending of metal halide clusters with polymers suffers from phase separation‐induced scattering losses. Herein, we report a facile in situ photopolymerization strategy for the successful preparation of highly transparent and uniformly luminescent copper(I) iodide cluster‐polymer composite scintillator films (Cu 4 I 4 ‐PUP). Triggered by ultraviolet light, the precursor solution can be rapidly cured within 50 s to form a homogeneous film with a polymer network structure featuring a “rigid inorganic core‐flexible organic shell”. The as‐obtained film exhibits excellent optical transmittance and intense yellowish‐green radioluminescence (RL) with a light yield of 33 091 ph MeV −1 , spatial resolution of 22.7 lp mm −1 , and detection limit of 240 nGy air s −1 . Furthermore, by virtue of pulse shape discrimination (PSD) technology, the film achieves pulse‐shape discrimination with a figure‐of‐merit (FoM) of 0.62 for efficient α/γ separation, demonstrating distinct and reliable PSD performance among copper‐halide scintillators. This work provides a scalable platform for high‐performance scintillators suitable for medical radiography, industrial inspection, and nuclear security applications.