Abstract
Through-space charge transfer (TSCT) thermally activated delayed fluorescence (TADF) materials have recently shown great potential for applications in X-ray detection and imaging due to their efficient triplet exciton utilization. By rational tuning of molecular/electronic structures of D and A moieties and precise regulation of TSCT interactions, tunable emission and TSCT-based TADF can be achieved. However, the TSCT interactions in organic D-A systems are somewhat difficult to design and control precisely resulting from relatively weak D-A supramolecular interactions. Herein, we propose a concept of TADF host-guest MOF scintillators with modulational TSCT interactions by confining D molecules as guests in the pore spaces of host MOFs composed of A ligands. Based on the synergy of the coordination and D-A interactions, various D molecules can be introduced into MOFs and manipulation of TSCT interactions can be achieved. As a result, tunable emission wavelengths spanning from 532 nm to 738 nm and successful construction of TADF host-guest MOF materials for X-ray scintillators can be achieved. Thanks to stable and enhanced triplet exciton utilization efficiency induced by TADF, the scintillator performance of compound 1 obviously surpassed that of separate D and A components as well as that of traditional organic commercial scintillator anthracene. The potential application of this scintillator in X-ray imaging was also demonstrated. This work provides a novel strategy for developing host-guest MOF scintillators.