Thermally Activated Delayed Fluorescence (TADF)-active Coinage-metal Sulfide Clusters for High-resolution X-ray Imaging

Angew Chem Int Ed Engl. 2024 Feb 12;63(7):e202318026. doi: 10.1002/anie.202318026. Epub 2024 Jan 15.

Abstract

The study of facile-synthesis and low-cost X-ray scintillators with high light yield, low detection limit and high X-ray imaging resolution plays a vital role in medical and industrial imaging fields. However, the optimal balance between X-ray absorption, decay lifetime and excitonic utilization efficiency of scintillators to achieve high-resolution imaging is extremely difficult due to the inherent contradiction. Here two thermally activated delayed fluorescence (TADF)-actived coinage-metal clusters M6 S6 L6 (M=Ag or Cu) were synthesized by simple solvothermal reaction, where the cooperation of heavy atom-rich character and TADF mechanism supports strong X-ray absorption and rapid luminescent collection of excitons. Excitingly, Ag6 S6 L6 (SC-Ag) displays a high photoluminescence quantum yield of 91.6 % and scintillating light yield of 17420 photons MeV-1 , as well as a low detection limit of 208.65 nGy s-1 that is 26 times lower than the medical standard (5.5 μGy s-1 ). More importantly, a high X-ray imaging resolution of 16 lp/mm based on SC-Ag screen is demonstrated. Besides, rigid core skeleton reinforced by metallophilicity endows clusters M6 S6 L6 strong resistance to humidity and radiation. This work provides a new view for the design of efficient scintillators and opens the research door for silver clusters in scintillation application.

Keywords: Coinage-Metal Clusters; Thermally Activated Delayed Fluorescence; X-Ray Imaging; X-Ray Scintillators.