Highly efficient organic light-emitting diodes and light-emitting electrochemical cells employing multi-resonant thermally activated delayed fluorescent emitters with bulky donor or acceptor peripheral groups

Multi-resonant thermally activated delayed fluorescence (MR-TADF) emitters have been the focus of extensive design efforts as they are recognized to show bright, narrowband emission, which makes them very appealing for display applications. However, the planar geometry and relatively large singlet-triplet energy gap lead to, respectively, severe aggregation-caused quenching (ACQ) and slow reverse intersystem crossing (RISC). Here, a design strategy is proposed to address both issues. Two MR-TADF emitters TPPO-tBu-DiKTa and TPA-tBu-DiKTa have been synthesized. Twisted ortho-substituted groups help increase the intermolecular distance and largely suppress the ACQ. In addition, the contributions from intermolecular charge transfer states in the case of TPA-tBu-DiKTa help to accelerate RISC. The OLEDs with TPPO-tBu-DiKTa and TPA-tBu-DiKTa exhibit high maximum external quantum efficiencies (EQEmax) of 24.4 and 31.0%, respectively. Notably, the device with 25 wt% TPA-tBu-DiKTa showed both high EQEmax of 28.0% and reduced efficiency roll-off (19.9% EQE at 1000 cd m-2) compared to the device with 2 wt% emitter (31.0% EQEmax and 11.0% EQE at 1000 cd m-2). The new emitters were also introduced into single-layer LECs, equipped with air-stable electrodes. The LEC containing TPA-tBu-DiKTa dispersed at 0.5 wt% in a matrix comprising a mobility-balanced blend-host and an ionic-liquid electrolyte delivered blue luminance with an EQEmax of 2.6% at 425 cd m-2. The high efficiencies of the OLEDs and LECs with TPA-tBu-DiKTa illustrate the potential for improving device performance when the DiKTa core is decorated with twisted bulky donors.