Excited-State and Steric Hindrances Engineering Enable Fast Spin-Flip Narrowband Thermally Activated Delayed...

Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have great potential for applications in ultrahigh-definition (UHD) organic light-emitting diode (OLED) displays, that benefit from their narrowband emission characteristic. However, key challenges such as aggregation-caused quenching (ACQ) effect and slow triplet-to-singlet spin-flip process, especially for blue MR-TADF materials, continue to impede their development due to planar skeletons and relatively large ΔE_STs. Here, an effective strategy that incorporates multiple carbazole donors into the parent MR moieties is proposed, synergistically engineering their excited states and steric hindrances to enhance both the spin-flip process and quenching resistance. As expected, the designed materials namely 5Cz-BNO and 5Cz-BN exhibit bright blue and green emissions with narrow full-width at half-maximums (FWHMs) around 23 nm, together with significantly improved reverse intersystem crossing (RISC) rates. The OLEDs based on 5Cz-BNO and 5Cz-BN with doping concentrations from 5 to 20 wt % achieve high maximum external quantum efficiency (EQE_max) values exceeding 30 % with suppressed efficiency roll-offs and improved operational stability. This work offers an effective approach for designing doping-insensitive blue and green MR-TADF materials with fast spin-flip processes by integrating the engineering of excited states and steric hindrances.