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Multi‐resonance thermally activated delayed fluorescence (MR‐TADF) emitters offer natural advantages for creating power‐efficient, wide‐color‐gamut OLEDs. However, current green MR‐TADF emitters face challenges in simultaneously achieving high color purity and efficient reverse inter‐system crossing (RISC), leading to suboptimal device performance. In this study, we propose a synergistic molecular design approach that combines π‐extension and peripheral locking to address these challenges. This approach allows for the construction of quadruple borylated MR‐TADF emitters that not only deliver precisely tuned pure‐green emission with a narrow full width at half maximum (FWHM) of 15 nm, but also exhibit close‐to‐unity quantum yield, rapid RISC, and optimal horizontal dipole orientation. The resulting sensitizer‐free OLED approaches the BT.2020 standard with CIE coordinates of (0.18, 0.74) and demonstrates impressive external quantum efficiency (EQE) of 36.6 % at maximum and 31.8 % at 1000 cd m−2. Additionally, the device shows good operational stability, with a lifetime (LT80) of 485 hours at an initial luminance of 1000 cd m−2. This study hence offers a promising molecular design strategy that effectively enhances the comprehensive OLED performance. [ABSTRACT FROM AUTHOR]

Multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters offer natural advantages for creating power-efficient, wide-color-gamut OLEDs. However, current green MR-TADF emitters face challenges in simultaneously achieving high color purity and efficient reverse inter-system crossing (RISC), leading to suboptimal device performance. In this study, we propose a synergistic molecular design approach that combines π-extension and peripheral locking to address these challenges. This approach allows for the construction of quadruple borylated MR-TADF emitters that not only deliver precisely tuned pure-green emission with a narrow full width at half maximum (FWHM) of 15 nm, but also exhibit close-to-unity quantum yield, rapid RISC, and optimal horizontal dipole orientation. The resulting sensitizer-free OLED approaches the BT.2020 standard with CIE coordinates of (0.18, 0.74) and demonstrates impressive external quantum efficiency (EQE) of 36.6 % at maximum and 31.8 % at 1000 cd m -2 . Additionally, the device shows good operational stability, with a lifetime (LT 80 ) of 485 hours at an initial luminance of 1000 cd m -2 . This study hence offers a promising molecular design strategy that effectively enhances the comprehensive OLED performance., (© 2024 Wiley-VCH GmbH.)

The development of pure-green organic emitters with ideal emission peaks and ultra-narrow full-widths at half-maximum (FWHMs) remains a formidable challenge. Herein, we report two new green emitters, CNBN and MCNBN, which achieve extremely narrow FWHMs by synergistic rigid π-extension and cyano-substitution of a sky-blue multi-resonance thermally activated delayed fluorescence (MR-TADF) core. The introduction of cyano groups induces red-shifts in the emission to the green region and dramatically minimizes the FWHMs. In toluene solution, CNBN and MCNBN exhibit narrowband emission with a maximum at 501 nm and 510 nm with ultra-narrow FWHMs of 14 nm/0.066 eV and 15 nm/0.071 eV, respectively. Given the near-unity photoluminescence quantum yields and almost 100 % horizontal dipole orientation, the electroluminescent (EL) devices based on CNBN and MCNBN deliver external quantum efficiencies (EQEs) exceeding 30 % with FWHMs of 16 nm/0.072 eV and 17 nm/0.080 eV, respectively. Notably, the MCNBN-based device achieves pure-green emission with a maximum at 517 nm with Commission Internationale de l'Éclairage coordinates of (0.17, 0.74), closely aligning with the BT.2020 green standard., (© 2025 Wiley-VCH GmbH.)