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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]

Device simplification is of practical significance for organic light emitting diodes (OLEDs), and remains the great challenge for deep‐red emitters. Herein, a deep‐red thermally activated delayed fluorescence molecule (pTPA‐DPPZ) is reported which features a T shaped structure containing two triphenylamine (TPA) donors, one either side of a planar dipyridophenazine (DPPZ) acceptor. The rational spatial arrangement of the functional groups leads to limited but sufficient molecular packing for effective carrier transport. The neat pTPA‐DPPZ film achieves an around 90‐fold improved radiation rate constant of 107 s−1 and the nearly unitary reverse intersystem crossing (RISC) efficiency, as well as accelerated emission decays for quenching suppression. The high radiation and RISC result in a photoluminescence quantum yield of 87 %. The bilayer OLED based on the pTPA‐DPPZ emissive layer achieved the record external quantum efficiencies of 12.3 % for maximum and 10.4 % at 1000 nits, accompanied by the deep‐red electroluminescence with the excellent color purity. [ABSTRACT FROM AUTHOR]