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Enhancing Reverse Intersystem Crossing via Secondary Acceptors: towards Sky-Blue Fluorescent Diodes with Tenfold-Improved Exter-nal Quantum Efficiency
摘要: How to simply but effectively facilitate reverse intersystem crossing (RISC) transition is always the key issue for developing high-performance thermally activated delayed fluorescence (TADF) dyes. In this work, as a proof of concept, a feasible strategy named 'acceptor enhancement' is demonstrated with a series of ternary blue emitters (xCzmPOnTPTZ) using diphenylphosphine oxide (PO) as secondary acceptors. Compared with its PO-free binary analogue, such simple introduction of PO groups in pCzPO2TPTZ dramatically enhances its RISC rate constant (kRISC) by 10 times to the level of ~105 s-1, accompanied by RISC efficiency (ηRISC) of 92%, which further improves the triplet-to-singlet upconversion for effective triplet harvesting in its devices. As the result, on the basis of a trilayer device structure, pCzPO2TPTZ realized a state-of-the-art external quantum efficiency (EQE) beyond 20% with tenfold improvement.
关键词: Organic Light-Emitting Diode,Thermally Activated Delayed Fluorescence,Excited State Transition,Blue Emission,Reverse Intersystem Crossing,Phosphine Oxide Acceptor
更新于2025-09-23 15:23:52
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Efficient and Stable Deep-Blue Fluorescent Organic Light-Emitting Diodes Employing a Sensitizer with Fast Triplet Upconversion
摘要: Multiple donor–acceptor-type carbazole–benzonitrile derivatives that exhibit thermally activated delayed fluorescence (TADF) are the state of the art in efficiency and stability in sky-blue organic light-emitting diodes. However, such a motif still suffers from low reverse intersystem crossing rates (kRISC) with emission peaks <470 nm. Here, a weak acceptor of cyanophenyl is adopted to replace the stronger cyano one to construct blue emitters with multiple donors and acceptors. Both linear donor–π–donor and acceptor–π–acceptor structures are observed to facilitate delocalized excited states for enhanced mixing between charge-transfer and locally excited states. Consequently, a high kRISC of 2.36 × 106 s?1 with an emission peak of 456 nm and a maximum external quantum efficiency of 22.8% is achieved. When utilizing this material to sensitize a blue multiple-resonance TADF emitter, the corresponding device simultaneously realizes a maximum external quantum efficiency of 32.5%, CIEy ≈ 0.12, a full width at half maximum of 29 nm, and a T80 (time to 80% of the initial luminance) of > 60 h at an initial luminance of 1000 cd m?2.
关键词: stable deep-blue devices,sensitized emission,high reverse intersystem crossing,thermally activated delayed fluorescence,multiple donors and acceptors
更新于2025-09-23 15:21:01
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Recent advances in thermally activated delayed fluorescence for white OLEDs applications
摘要: Thermally activated delayed fluorescence (TADF) materials, which can harvest all excitons without utilizing any noble metals to emit light, are becoming the key cornerstone for developing the next generation of organic light-emitting diode (OLED) devices. In recent years, TADF materials are attracting numerous attentions as a new surge of research focuses on both science and industry owing to their high efficiency, low power consumption, and low production cost attributes when applied to white OLEDs. The design and application of TADF in WOLED devices have also experienced the rapid development in fundamental science and industrial technology perspectives. In the present review, the specific reverse intersystem crossing mechanism and evolution of TADF is outlined firstly, and then the latest research progress of TADF-WOLEDs is summarized and discussed. TADF/conventional fluorescence, TADF/phosphorescence, all TADF and TADF exciplex-based WOLEDs are categorized and elaborated in terms of the device structure, working mechanism, efficiency, color-rendering index, etc. Finally, we conclude with the future challenges and opportunities in high-quality TADF devices and application area.
关键词: Thermally activated delayed fluorescence,exciplex,OLED,TADF,RISC,white OLEDs,organic light-emitting diode,reverse intersystem crossing
更新于2025-09-19 17:13:59
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Aggregation-Induced Delayed Fluorescence Luminogens with Accelerated Reverse Intersystem Crossing for High-Performance OLEDs
摘要: A fast reverse intersystem crossing (RISC) is of high importance for delayed fluorescence emitters in terms of increasing exciton utilization and suppressing efficiency roll-off. Herein, new robust luminogens comprised of carbonyl, phenoxazine and chlorine-substituted carbazole derivatives are synthesized and characterized. They own distinct aggregation-induced delayed fluorescence (AIDF) feature, and exhibit high photoluminescence efficiencies and short delayed fluorescence lifetimes in neat films. The RISC is conspicuously accelerated owing to their tiny singlet-triplet energy splitting and greatly enhanced spin-orbit coupling by heavy atom effect in neat films. They can function efficiently as light-emitting layers in nondoped OLEDs, providing excellent maximum electroluminescence (EL) efficiencies of 20.4–21.7%, and can also perform outstandingly in doped OLEDs in a wide doping concentration range (5–90 wt%), affording impressive EL efficiencies of up to 100.1 cd A–1, 104.8 lm W–1 and 29.1%, with small efficiency roll-off. These findings demonstrate the AIDF luminogens with fast RISC are promising candidates to fulfill various demands of production and application of OLEDs.
关键词: OLEDs,Reverse Intersystem Crossing,Luminogens,Aggregation-Induced Delayed Fluorescence,High-Performance
更新于2025-09-11 14:15:04
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Highly efficient thermally activated delayed fluorescence with slow reverse intersystem crossing
摘要: We report an efficient luminescent molecule exhibiting thermally activated delayed fluorescence with a long-delayed fluorescence lifetime of 0.8 ms. Although the reverse intersystem crossing rate constant is small at 2.1 × 103 s?1, the molecule shows a high photoluminescence quantum yield of 89±2%, indicating the suppression of nonradiative decay from the triplet state.
关键词: Long triplet lifetime,Thermally activated delayed fluorescence (TADF),Reverse intersystem crossing (RISC)
更新于2025-09-10 09:29:36
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Kinetic Modelling of Transient Photoluminescence from Thermally Activated Delayed Fluorescence
摘要: A simplified state model and associated rate equations are used to extract the reverse intersystem crossing and other key rate constants from transient photoluminescence measurements of two high performance thermally activated delayed fluorescence materials. The values of the reverse intersystem crossing rate constant are in close agreement with established methods, but do not require a priori assumption of exponential decay kinetics, nor any additional steady state measurements. The model is also applied to measurements at different temperatures and found to reproduce previously reported thermal activation energies for the thermally activated delayed fluorescence process. Transient absorption measurements provide independent confirmation that triplet decay channels (neglected here) have no adverse effect on the fitting.
关键词: Thermally Activated Delayed Fluorescence,Transient Photoluminescence,Reverse Intersystem Crossing,Kinetic Modelling
更新于2025-09-10 09:29:36
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Photo-Physical Properties of Thermally Activated Delayed Fluorescent Materials upon Distortion of Central Axis of Donor Moiety
摘要: In this study, we showed the distortion of central axis of donor moiety can switch critically the rate of reverse intersystem crossing (kRISC) process, which is the trigger point to modulate the lifetime of delayed fluorescence. To achieve kRISC what we desired (105 to 106 s-1) in a series of donor-acceptor-donor (D-A-D) type thermally activated delayed fluorescence (TADF) materials, the donor groups (phenoxazine and phenothiazine) was selectively introduced. Maintaining the near orthogonality between donor and acceptor (benzonitrile) moiety, the occurrence of the distortion of central axis of donor moiety could make the effect of locally excited triplet state (3LE). In other words, the interaction between 3LE and the charge transfer counterparts (i.e., 1CT and 3CT) contributes an opposite propensity of kRISC for each target TADF materials when those are dissolved in solution and condensed in solid-state. Herein, we have theoretically and experimentally shown the photo-physical behavior of common D-A-D type TADF upon the different system.
关键词: Reverse Intersystem Crossing,Thermally Activated Delayed Fluorescence,Benzonitrile,Phenoxazine,Donor-Acceptor-Donor,Phenothiazine
更新于2025-09-09 09:28:46
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Experimental Evidence for “Hot Exciton” Thermally Activated Delayed Fluorescence Emitters
摘要: Contradiction between no effective photophysical experiments and high device results causes the “hot exciton” thermally activated delayed fluorescence (TADF) mechanism to be still a controversial question. Here, the steady and transient photophysical characterization combined with theoretical calculation based on 4,7-bis(9,9-dimethyl-9H-fluoren-2-yl)-5,6-difluorobenzo[c][1,2,5]thiadiazole (2F-BTH-DMF), 4,7-bis(9,9-dimethyl-9H-fluoren-2-yl)benzo[c][1,2,5]thiadiazole (BTH-DMF), and 5,6-bis(9,9-dimethyl-9H-fluoren-2-yl)benzo[c][1,2,5] thiadiazole (o-BTH-DMF) demonstrate that all the emitters exhibit TADF via reverse intersystem crossing (RISC) from “hot exciton” triplet excited state. The fast RISC process “hot exciton” mechanism affords a very short delayed lifetime (1 μs). Organic light-emitting diodes (OLEDs) based on these emitters exhibit high exciton utilization over 25% and the best device shows a maximum current efficiency of 31.02 cd A?1, maximum power efficiency of 27.85 lm W?1, and external quantum efficiency of 9.13%, which are the highest performances for reported OLEDs with “hot exciton” mechanism. The experimental evidence for fast RISC process via “hot exciton” triplet state and short delayed lifetime highlights the TADF emitters with “hot exciton” mechanism for high-performance OLEDs with very low efficiency roll-off.
关键词: hot excitons,reverse intersystem crossing,thermally activated delayed fluorescence,organic light-emitting devices
更新于2025-09-04 15:30:14