Zinc–Halide–Integrated Thermally Reprocessable Molecular–Emitter Supramolecular Glass Scintillators for High–Resolution X–Ray Imaging

ABSTRACT Transparent glass scintillators suppress grain−boundary scattering, but in many metal−halide glasses x−ray attenuation and terminal emission originate from the same local coordination unit, making their optimization mutually constraining. Here, we report molecular−emitter supramolecular glasses that functionally partition these roles between an organic phosphonium chromophore and a stoichiometrically incorporated zinc–halide environment. The phosphonium salt melt quenching methyl(4−(diphenylamino)phenyl)diphenylphosphonium iodide ( o ‐TNP) with ZnX 2 (X = Cl, Br, or I) and a trace amount of 4,4′−bipyridine (BP) produced transparent amorphous materials with glass−transition temperatures above 100°C. Across the halide series, the principal emission maximum remained within 493–500 nm, whereas the photoluminescence quantum yield increased from 3.53% to 10.01%, the average long−lived emission lifetime decreased from 9.7 to 4.4 µs, and the attenuation−corrected light yield rose from 14 909 to 22 954 photons MeV −1 . The optimized TNP−ZnI 2 screen achieved a system spatial resolution of 28.4 lp mm −1 at a thickness of 650 µm. After ten fragment−soften−recast cycles at 220°C, it retained 84% of its initial radioluminescence while preserving the emission maximum and spectral profile. This work provides a modular route for functional partitioning x−ray attenuation and long‐lived excited‐state dynamics with minimal perturbation of terminal emission energy.