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"Hot exciton" molecules that allow the transition of excitons from a high‐lying triplet state (Tn, n≥ 2) to singlet states (Sm, m≥1) by a reverse intersystem crossing (hRISC) process have become an effective strategy to achieve high efficiency fluorescence organic light emitting diodes (OLEDs). However, the understanding of the dynamic behavior of the "hot exciton" process is still very lacking. Herein, the exciton dynamics of an aggregation‐induced emission (AIE) molecule TPA‐An‐mPhCz with the "hot exciton" property are deeply investigated, and the proportion between hRISC and internal inversion (IC) of excitons on Tn is successfully quantified by in situ transient electroluminescent measurements and theoretical calculation. It is found that the IC process increases severe energy loss of Tn excitons. By introducing a triplet–triplet annihilation up‐conversion layer in the emissive layer to efficiently recapture the IC excitons and further doping a blue fluorescent emitter in the TPA‐An‐mPhCz layer to achieve high photoluminescence quantum yield (PLQY), the resulting OLED achieves a maximum external quantum efficiency of 12.5% with negligible efficiency roll‐off. More impressively, the operational lifetime LT75 (lifetime to 75% of the initial luminance) of the device with efficient triplets utilization performs a remarkable 116 h under 1000 cd m−2. This work provides the fundamentals for the design of hot exciton materials with efficient exciton utilization to develop efficient blue fluorescence OLEDs. [ABSTRACT FROM AUTHOR]

Aggregation‐induced emission (AIE) materials are attractive for the fabrication of high‐efficiency organic light‐emitting diodes (OLEDs) owing to the "hot exciton" process by reverse intersystem crossing (hRISC) and high photoluminescence quantum yields (PLQY). However, the internal conversion (IC) from the high‐lying triplet excitation states (Tn, n≥2) to the lower excited triplet state (Tn‐1) is inevitable, resulting in severe exciton losses. Herein, an effective device structure is designed that reuses the lost triplet excitons caused by IC and realizes the breakthrough in the efficiency of blue fluorescence OLEDs based on AIE molecule as an emitter. The maximum external quantum efficiency reached as high as 14.8% and is kept at 14.4% at the luminance of 1000 cd m−2. In the designed device, a triplet–triplet annihilation (TTA) up‐conversion material 1‐[2,5‐dimethyl‐4‐(1‐pyrenyl)phenyl]pyrene (DMPPP) is introduced into the AIE emitter as a triplet sensitizer to receive the lost triplet excitons, and a thin TTA up‐conversion layer 9‐[4‐(10‐phenyl‐9‐anthryl)phenyl]‐9H‐carbazole (CzPA) is introduced in the middle of the doped layer to form the emissive layer (EML). It is found that the hRISC process of iTPB‐2AC greatly enhances the utilization efficiency of TTA intermediate state ([TT]*) excitons on CzPA to iTPB‐2AC so that the utilization of the lost excitons is maximized. This work establishes physical insights into the AIE emission materials and device fabrication of high‐efficiency blue fluorescence OLEDs. [ABSTRACT FROM AUTHOR]

The operational lifetime of blue organic light‐emitting diodes (OLEDs) is still insufficient for practical applications in lighting and display. One type of blue organic emitting materials with hybridized local and charge‐transfer (HLCT) process are beneficial in achieving high‐efficiency OLEDs through "hot exciton" channel by harnessing high‐lying triplet (Tn) excitons. However, the operational lifetime of the resulting blue OLEDs is rarely studied and understood. In this article, the aging properties of blue fluorescent OLEDs based on an HLCT material (2‐(4‐(10‐(3‐(9H‐carbazol‐9‐yl)phenyl)anthracen‐9‐yl)phenyl)‐1‐phenyl‐1H‐phenanthro[9,10‐d]imidazole) (PAC) are systematically investigated by exciton dynamics calculation and transient EL experiments. It is experimentally and theoretically revealed that whether the reverse intersystem crossing (hRISC) process from high‐lying excited triplet to singlet in HLCT materials is completely effective determines the device degradation. A fluorescent emitter is doped into PAC host to accelerate the hRISC process, thus enhancing device operational lifetime to reach T75 = 110 ± 2 h (time to 75% of initial luminance) under 1000 cd m−2. This work provides inspirations to investigate the stability of blue fluorescent OLEDs based on HCLT materials and further enhance the operational lifetime. [ABSTRACT FROM AUTHOR]

Aggregation‐induced emission (AIE) and hybridized local and charge‐transfer (HLCT) materials are two kinds of promising electroluminescence systems for the fabrication of high‐efficiency organic light‐emitting diodes (OLEDs) by harnessing "hot excitons" at the high‐lying triplet exciton states (Tn, n ≥ 2). Nonetheless, the efficiency of the resulting OLEDs did not meet expectations due to the possible loss of Tn→Tn−1. Herein, experimental results and theoretical calculations demonstrate the "hot exciton" process between the high‐lying triplet state T3 and the lowest excited singlet state S1 in an AIE material 4⁗‐(diphenylamino)‐2″,5″‐diphenyl‐[1,1″:4′,1″:4″,1′″:4′″,1⁗‐quinquephenyl]‐4‐carbonitrile (TPB‐PAPC) and it is found that the Förster resonance energy transfer (FRET) between two molecules can facilitate the "hot exciton" process and inhibit the T3→T2 loss by doping a blue fluorescent emitter in TPB‐PAPC. Finally, the doped TPB‐PAPC blue OLEDs achieve a maximum external quantum efficiency (EQEmax) of 9.0% with a small efficiency roll‐off. Furthermore, doping the blue fluorescent emitter in a HLCT material 2‐(4‐(10‐(3‐(9H‐carbazol‐9‐yl)phenyl)anthracen‐9‐yl)phenyl)‐1‐phenyl‐1H‐phenanthro[9,10‐d] imidazole (PAC) is used as the emission layer, and the resulting blue OLEDs exhibit an EQEmax of 17.4%, realizing the efficiency breakthrough of blue fluorescence OLEDs. This work establishes a physical insight in the design of high‐performance "hot exciton" molecules and the fabrication of high‐performance blue fluorescence OLEDs. [ABSTRACT FROM AUTHOR]

Abstract: The highly efficient charge generation and transport is realized by simply stacking several 1,4,5,8,9,11‐hexa‐azatriphenylene hexacarbonitrile (HAT‐CN)/4,4′,4″‐tris(N‐3‐methylphenyl‐N‐phenylamino) triph‐enylamine (m‐MTDATA) organic heterojunctions in series. Mechanism analysis confirms that the highly effective charge transport property benefits from the efficient charge generation and recombination processes at the HAT‐CN/m‐MTDATA interfaces. It is found that the efficient multialternating organic heterojunctions can be used not only as hole and electron transporters to supply large charge injection, but also as excellent charge generation layer (CGL) to fabricate high‐performance tandem organic light‐emitting diodes (OLEDs). The resulting red phosphorescent OLEDs by simultaneously using the multialternating organic heterojunctions as hole and electron transporters realize the power efficiency (PE) of 36.7 lm W−1, current efficiency (CE) of 28.0 cd A−1, and external quantum efficiency (EQE) of 15.4%, whereas the PE, CE, and EQE, respectively, reach 37.1 lm W−1, 56.0 cd A−1, and 31.8% when simultaneously using the multialternating organic heterojunctions as hole and electron transporters and CGL to fabricate tandem red phosphorescent OLEDs, indicating the validity of the multialternating organic heterojunctions as the charge generator and transporters. The results provide us a totally new way of fabricating high‐performance OLEDs. [ABSTRACT FROM AUTHOR]

Triplet‐triplet fusion (TTF) can effectively transfer triplet excitons to singlet energy level and exhibit good stability, making it widely used in blue fluorescence organic light emitting diodes (OLEDs) for practical application. However, the efficiency of the resulting blue fluorescence OLEDs is still fundamentally limited. Herein, this work introduces a hot exciton efficiency enhancement layer (EEL) between TTF emissive layer and electron‐transporting layer for the first time. It can be found that the triplet excitons are greatly utilized by the efficient hot exciton EEL. As a result, a high efficiency blue fluorescence OLED is successfully developed, exhibiting a maximum external quantum efficiency of 15.2% at the luminance of 4068.0 cd m−2, achieving a breakthrough in the efficiency of blue TTF‐OLEDs. Transient electroluminescence (TrEL) measurements and detailed theoretical calculations confirm the key role of the effective hot exciton process from the high‐lying triplet energy level (Tn, n ≥ 2) to S1 via a reverse intersystem crossing (hRISC). Furthermore, the device lifetime is also greatly improved owing to the fast and efficient hRISC in the introduced hot exciton EEL. This work has important guiding significance for constructing high efficiency blue fluorescence OLEDs by introducing hot exciton molecules. [ABSTRACT FROM AUTHOR]