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1.
Angew Chem Int Ed Engl ; 63(27): e202318782, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38354089

RESUMEN

High performance solution-processable deep-blue emitters with a Commission International de l'Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh-definition display. Although, deep-blue materials with hybridized local and charge-transfer (HLCT) excited-state feature are promising candidates, their rigidity and planar molecular structures limit their application in solution-processing technique. Herein, four novel deep-blue solution-processable HLCT emitters were first proposed by attaching rigid imide aliphatic rings as functional units onto the HLCT emitting core. The functional units not only improve solubility, enhance thermal properties and morphological stability of the emitting core, but also promote photoluminescence efficiency, balance charge carrier transport, and inhibit aggregation-caused quenching effect due to the weak electron-withdrawing property as well as steric hindrance. The corresponding solution-processable organic light-emitting diodes (OLEDs) substantiate an unprecedented maximum external quantum efficiency (EQEmax) of 11.5 % with an emission peak at 456 nm and excellent colour purity (full width at half maximum=56 nm and CIEy=0.09). These efficiencies represent the state-of-the-art device performance among the solution-processable blue OLEDs based on the "hot exciton" mechanism. This simple strategy opens up a new avenue for designing highly efficient solution-processable deep-blue organic luminescent materials.

2.
Research (Wash D C) ; 2022: 9838120, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-35935131

RESUMEN

Multiresonance (MR) emitters featuring narrowband emissions and theoretically 100% exciton harvesting are great potential for organic light-emitting diode (OLED) applications. However, how to functionalize MR molecules without scarifying emission color purity is still a key challenge. Herein, we report a feasible strategy for selective optimization of MR molecules, which is demonstrated by a blue MR emitter tCBNDASPO substituted with a diphenylphosphine oxide (DPPO) group. Compared to its DPPO-free parent molecule, tCBNDASPO preserves narrowband feature with full widths at half maximum (FWHM) values of 28 nm in film and 32 nm in OLEDs and achieves 40% increased photoluminescence (92%) and electroluminescence quantum efficiencies (28%). It is showed that insulation effect of P=O effectively confines the singlet excited state on MR core to keep emission color purity, and its induction effect enhances singlet radiation and triplet-to-singlet conversion. This synergism for selective optimization is based on rational linkage between MR core and functional groups.

3.
Adv Mater ; 34(17): e2110547, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35233858

RESUMEN

Emerging multi-resonance (MR) thermally activated delayed fluorescence (TADF) emitters can combine 100% exciton harvesting and high color purity for their organic light-emitting diodes (OLED). However, the highly planar configurations of MR molecules lead to intermolecular-interaction-induced quenching. A feasible way is integrating host segments into MR molecules, namely a "self-host" strategy, but without involving additional charge transfer and/or vibrational components to excited states. Herein, an ambipolar self-host featured MR emitter, tCBNDADPO, is demonstrated, whose ambipolar host segment (DADPO) significantly and comprehensively improves the TADF properties, especially greatly accelerated singlet radiative rate constant of 2.11 × 108 s-1 and exponentially reduced nonradiative rate constants. Consequently, at the same time as preserving narrowband blue emission with an FWHM of ≈28 nm at a high doping concentration of 30%, tCBNDADPO reveals state-of-the-art photoluminescence and electroluminescence quantum efficiencies of 99% and 30%, respectively. The corresponding 100% internal quantum efficiency of tCBNDADPO supported by an ultrasimple trilayer and heavily doped device demonstrates the feasibility of the ambipolar self-host strategy for constructing practically applicable MR materials.

4.
Nat Commun ; 12(1): 3640, 2021 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-34131127

RESUMEN

Development of white organic light-emitting diodes based on purely thermally activated delayed fluorescence with a single-emissive-layer configuration has been a formidable challenge. Here, we report the rational design of a donor-acceptor energy-relaying exciplex and its utility in fabricating single-emissive-layer, thermally activated delayed fluorescence-based white organic light-emitting diodes that exhibit 100% internal quantum efficiency, 108.2 lm W-1 power efficiency, and 32.7% external quantum efficiency. This strategy enables thin-film fabrication of an 8 cm × 8 cm thermally activated delayed fluorescence white organic light-emitting diodes (10 inch2) prototype with 82.7 lm W-1 power efficiency and 25.0% external quantum efficiency. Introduction of a phosphine oxide-based acceptor with a steric group to the exciplex limits donor-acceptor triplet coupling, providing dual levels of high-lying and low-lying triplet energy. Transient spectroscopic characterizations confirm that a ladder-like energy relaying occurs from the high-lying triplet level of the exciplex to a blue emitter, then to the low-lying triplet level of the phosphine oxide acceptor, and ultimately to the yellow emitter. Our results demonstrate the broad applicability of energy relaying in multicomponent systems for exciton harvesting, providing opportunities for the development of third-generation white organic light-emitting diode light sources.

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