Zinc-Halide-Integrated Thermally Reprocessable Molecular-Emitter Supramolecular Glass Scintillators for...

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 ZnX₂ (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-ZnI₂ 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.