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1.
Adv Mater ; 34(33): e2202464, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35762112

RESUMEN

Achieving narrow-bandwidth emission and high external quantum efficiency (EQE) simultaneously is a challenge for next-generation blue-emitting organic light-emitting diodes (OLEDs). In this study, novel multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters are developed by fusing an indolocarbazole unit with two carbazole skeletons using para-oriented nitrogen atoms. The resulting rigid and planar π-system without electron-accepting atoms exhibits pure blue photoluminescence at 470 nm, reaching a 100% quantum yield with a full-width-at-half-maximum (FWHM) of 25 nm. Higher-level quantum chemistry calculations confirm an MR effect within the extended π-conjugation and an enhanced triplet-to-singlet crossover (104 s-1 ) through a reduced energy gap (ΔEST ) coupled with large spin-vibronic coupling mediated by low-lying triplet excited states. An OLED fabricated using the MR-TADF emitter with CIE color coordinates of (0.12, 0.16) exhibits a record high EQE of 30.9% and a small FWHM of 23 nm. With further optimization of the device structure, a high EQE of 33.8% is achieved without additional outcoupling enhancements owing to the near-perfect horizontal alignment of the emitting dipoles.

2.
Adv Sci (Weinh) ; 9(3): e2102141, 2022 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-34802190

RESUMEN

To utilize thermally activated delayed fluorescence (TADF) technology for future displays, it is necessary to develop host materials which harness the full potential of blue TADF emitters. However, no publication has reported such hosts yet. Although the most popular host for blue TADF, bis[2-(diphenylphosphino)phenyl]ether oxide (DPEPO) guarantees high-maximum external quantum efficiency (EQEmax ) TADF devices, they exhibit very short operational lifetimes. In contrast, long-lifespan blue TADF devices employing stable hosts such as 3',5-di(9H-carbazol-9-yl)-[1,1'-biphenyl]-3-carbonitrile (mCBP-CN) exhibit much lower EQEmax than the DPEPO-employed devices. Here, an elaborative approach for designing host molecules is suggested to achieve simultaneously stable and efficient blue TADF devices. The approach is based on engineering the molecular geometry, ground- and excited-state dipole moments of host molecules. The engineered hosts significantly enhance delayed fluorescence quantum yields of TADF emitters, as stabilizing the charge-transfer excited states of the TADF emitters and suppressing exciton quenching, and improve the charge balance. Moreover, they exhibit both photochemical and electrochemical stabilities. The best device employing one of the engineered hosts exhibits 79% increase in EQEmax compared to the mCBP-CN-employed device, together with 140% and 92-fold increases in operational lifetime compared to the respective mCBP-CN- and the DPEPO-based devices.

3.
J Phys Chem A ; 124(46): 9589-9596, 2020 Nov 19.
Artículo en Inglés | MEDLINE | ID: mdl-33170694

RESUMEN

The design of stable organic light-emitting diode materials is the key to long lifetime displays under various stressful conditions. Elucidating the degradation mechanism of the materials at the molecular level provides useful information for securing high stability. Previous works based on experiments or computations disclosed only a part of the whole degradation process. Here, we propose a holistic approach to the systematic analysis of the degradation mechanism by combining experimental mass analysis and computation in a semi-automated fashion. The mass analysis identifies molecular weights of feasible products from degradation reactions. Then, the computational analysis goes through initiation, propagation, and termination phases. The initiation phase determines radical fragments and reactive sites, triggering the propagation process. In the propagation phase, we subsequently perform intermediate sampling, reaction network construction, and kinetic analysis. As a proof of concept, this approach was applied to the thermal degradation problem during the sublimation purification process. Two major pathways were successfully elucidated with full atomistic details.

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