Antenna-based optimization of triplet radioluminescence of Tb-organic complex scintillator for efficient X-ray...

Triplet exciton is both a luminescence quenching factor and an important luminescence sensitization technology solution, which is widely concerned in the field of optoelectronic materials. Since X-ray excited triplet excitons are dissipated through various pathways, there are still huge difficulties in achieving efficient triplet sensitized emission. Here, the antenna ligand is regulated through the carboxyl group, increasing the steric hindrance between the conjugated groups and improving triplet-enhanced radioluminescence (RL) efficiencies of Tb³⁺. The lanthanide metal-organic frameworks (Ln-MOFs) formed by the coordination of Tb³⁺ with mellitic acid (MA), pyromellitic acid (PMA) and trimesic acid (TMA) under low temperature preparation conditions. Among them, MA-Tb has a longer spacing between conjugated groups than PMA-Tb and TMA-Tb, and its triplet RL is relatively strongest, with a light yield of 28,000 photons MeV^-1. Mechanistic studies revealed that the RL efficiency of Ln-MOFs is related to the π-π stacking effect in the benzene ring. In addition, the application of MA-Tb in the field of X-ray detection was demonstrated. The RL intensity of MA-Tb has a good linear relationship with the X-ray dose rate, and the detection limit for X-ray reaches 82 nGy/s, which is 66 times lower than the typical medical imaging dose. These results will provide a universal strategy for the design of Ln-MOFs scintillator.