Devices utilizing sterically shielded blue thermally activated delayed fluorescence emitters achieve high efficiencies and long lifetimes simultaneously.

Aromatic-imide-based thermally activated delayed fluorescent (TADF) enantiomers, (+)-(S,S)-CAI-Cz and (-)-(R,R)-CAI-Cz, were efficiently synthesized by introducing a chiral 1,2-diaminocyclohexane to the achiral TADF unit. The TADF enantiomers exhibited high PLQYs of up to 98 %, small ΔE values of 0.06 eV, as well as obvious temperature-dependent transient PL spectra, thus demonstrating their excellent TADF properties. Moreover, the TADF enantiomers showed mirror-image CD and CPL activities. Notably, the CP-OLEDs with CPEL properties based on the TADF enantiomers not only achieved high EQE values of up to 19.7 and 19.8 %, but also displayed opposite CPEL signals with g values of -1.7×10 and 2.3×10 , which represents the first CP-OLEDs, based on the enantiomerically pure TADF materials, having both high efficiencies and intense CPEL.

Multiple donor–acceptor‐type carbazole–benzonitrile derivatives that exhibit thermally activated delayed fluorescence (TADF) are the state of the art in efficiency and stability in sky‐blue organic light‐emitting diodes. However, such a motif still suffers from low reverse intersystem crossing rates (kRISC) with emission peaks <470 nm. Here, a weak acceptor of cyanophenyl is adopted to replace the stronger cyano one to construct blue emitters with multiple donors and acceptors. Both linear donor–π–donor and acceptor–π–acceptor structures are observed to facilitate delocalized excited states for enhanced mixing between charge‐transfer and locally excited states. Consequently, a high kRISC of 2.36 × 106 s−1 with an emission peak of 456 nm and a maximum external quantum efficiency of 22.8% is achieved. When utilizing this material to sensitize a blue multiple‐resonance TADF emitter, the corresponding device simultaneously realizes a maximum external quantum efficiency of 32.5%, CIEy ≈ 0.12, a full width at half maximum of 29 nm, and a T80 (time to 80% of the initial luminance) of > 60 h at an initial luminance of 1000 cd m−2.

Organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence-sensitized fluorescence (TSF) offer the possibility of attaining an ultimate high efficiency with low roll-off utilizing noble-metal free, easy-to-synthesize, pure organic fluorescent emitters. However, the performances of TSF-OLEDs are still unsatisfactory. Here, TSF-OLEDs with breakthrough efficiencies even at high brightnesses by suppressing the competitive deactivation processes, including direct charge recombination on conventional fluorescent dopants (CFDs) and Dexter energy transfer from the host to the CFDs, are demonstrated. On the one hand, electronically inert terminal-substituents are introduced to protect the electronically active core of the CFDs; on the other hand, delicate device structures are designed to provide multiple energy-funneling paths. As a result, unprecedentedly high maximum external quantum efficiency/power efficiency of 24%/71.4 lm W in a green TSF-OLED are demonstrated, which remain at 22.6%/52.3 lm W even at a high luminance of 5000 cd m . The work unlocks the potential of TSF-OLEDs, paving the way toward practical applications.

Maintaining high efficiency at high brightness levels is an exigent challenge for real-world applications of thermally activated delayed fluorescent organic light-emitting diodes (TADF-OLEDs). Here, versatile indolocarbazole-isomer derivatives are developed as highly emissive emitters and ideal hosts for TADF-OLEDs to alleviate efficiency roll-off. It is observed that photophysical and electronic properties of these compounds can be well modulated by varying the indolocarbazole isomers. A photoluminescence quantum yield (η ) approaching unity and a maximum external quantum efficiency (EQE ) of 25.1% are obtained for the emitter with indolo[3,2-a]carbazolyl subunit. Remarkably, record-high EQE/power efficiency of 26.2%/69.7 lm W at the brightness level of 5000 cd m with a voltage of only 3.74 V are also obtained using the same isomer as the host in a green TADF-OLED. It is evident that TADF hosts with high η values, fast reverse intersystem crossing processes, and balanced charge transport properties may open the path toward roll-off-free TADF-OLEDs.