Ambipolar Self-Host Functionalization Accelerates Blue Multi-Resonance Thermally Activated Delayed Fluorescence with Internal Quantum Efficiency of 100

Adv Mater. 2022 Apr;34(17):e2110547. doi: 10.1002/adma.202110547. Epub 2022 Mar 27.

Abstract

Emerging multi-resonance (MR) thermally activated delayed fluorescence (TADF) emitters can combine 100% exciton harvesting and high color purity for their organic light-emitting diodes (OLED). However, the highly planar configurations of MR molecules lead to intermolecular-interaction-induced quenching. A feasible way is integrating host segments into MR molecules, namely a "self-host" strategy, but without involving additional charge transfer and/or vibrational components to excited states. Herein, an ambipolar self-host featured MR emitter, tCBNDADPO, is demonstrated, whose ambipolar host segment (DADPO) significantly and comprehensively improves the TADF properties, especially greatly accelerated singlet radiative rate constant of 2.11 × 108 s-1 and exponentially reduced nonradiative rate constants. Consequently, at the same time as preserving narrowband blue emission with an FWHM of ≈28 nm at a high doping concentration of 30%, tCBNDADPO reveals state-of-the-art photoluminescence and electroluminescence quantum efficiencies of 99% and 30%, respectively. The corresponding 100% internal quantum efficiency of tCBNDADPO supported by an ultrasimple trilayer and heavily doped device demonstrates the feasibility of the ambipolar self-host strategy for constructing practically applicable MR materials.

Keywords: blue emission; hosts; multiple resonance; organic light-emitting diodes; thermally activated delayed fluorescence.