Supramolecular Method Enabling Effective Through-Space Charge Transfer in Thermally Activated Delayed Fluorescence Materials with Pure Orange Emission

Abstract

Achieving efficient charge transfer remains a significant challenge for thermally activated delayed fluorescence (TADF) materials that rely on through-space charge transfer (TSCT). In this study, we successfully applied a novel donor-acceptor pair characterized by non-exclusive charge transfer to TSCT-based TADF polymers. We propose a supramolecular strategy to optimize charge transfer by regulating the spatial arrangement of the donor-acceptor pairs. As the order of these pairs increases, localized emission from monomers is gradually quenched, ultimately resulting in pure orange emission. Photophysical studies reveal that improved spatial order accelerates the reverse intersystem crossing process, thereby enhancing the radiative transition rate of TADF emission and enabling efficient TSCT. This research offers a feasible method for designing TSCT-TADF materials. The resulting supramolecular systems with ordered configurations exhibit excellent energy and charge transfer performance, indicating their potential applications in optoelectronic devices, bioimaging, photodynamic therapy, and other fields.