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Efficient ultraviolet (UV) electroluminescent materials remain a great challenge, since short peak wavelength <400 nm and narrow full width at half maximum (FWHM) <50 nm are simultaneously required. In this sense, multi‐resonance (MR) thermally activated delayed fluorescence (TADF) emitters featuring narrow‐band emissions hold the promise for UV applications. Herein, a novel MR‐TADF skeleton featuring carbazole‐phosphine oxide (P=O) fused aromatics is developed to construct the first two UV MR emitters named CzP2PO and tBCzP2PO. In addition to synergistic resonance effects of P=O and N atom, sp3‐hybrid P atom renders the curved polycyclic planes of CzP2PO and tBCzP2PO, giving rise to their narrowband UV emissions with peak wavelengths <390 nm and FWHM<35 nm. Besides configuration quasi‐planarization for radiation enhancement and quenching suppression, P=O moiety further enhances singlet‐triplet coupling to facilitate reverse intersystem crossing, resulting in the state‐of‐the‐art photoluminescence quantum yield of 62 % in tBCzP2PO doped films. As consequence, tBCzP2PO endowed its UV organic light‐emitting diodes with the peak at 382 nm and FWHM of 32 nm, and especially the record‐high external quantum efficiency (EQE) of 15.1 % among all kinds of UV devices. Our results demonstrate great potential of P=O based MR emitters in practical applications including optoelectronics, biology and medicine science. [ABSTRACT FROM AUTHOR]

Herein, we report a deep‐red TADF emitter pCNQ–TPA, composed of quinoxaline‐5,8‐dicarbonitrile (pCNQ) acceptor and triphenylamine (TPA) donor. pCNQ–TPA supported its OLED with desired CIE coordinates of (0.69, 0.31) and the record maximum external quantum efficiency of 30.3 %, which is the best red TADF diode with Rec.2020 gamut for UHDTV. It is showed that through tuning pCNQ–TPA doping concentration, intra‐ and inter‐molecular charge transfer are balanced to synchronously improve emission color saturation and TADF radiation, and remedy aggregation‐induced quenching, rendering photoluminescence quantum yield (PLQY) reaching 90 % for deep‐red emission peaked at ≈690 nm. Quasi‐planar structure further endows pCNQ–TPA with an improved horizontal ratio of emitting dipole orientation, which increases light out‐coupling ratio to 0.34 for achieving the state‐of‐the‐art device efficiencies. [ABSTRACT FROM AUTHOR]