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Molecular emitters that combined thermally activated delayed and circularly polarized fluorescence (CP‐TADF) is of paramount importance for the next generation of displays. While most efforts have thus far focused on covalent donor and acceptor CP‐TADF emitters, a novel strategy based on chiral exciplexes has recently emerged. In this context, we present the synthesis and chiroptical properties of four new CP‐TADF exciplexes, involving two distinct C2‐symmetric bicarbazole systems and two terpyridine‐based derivatives, which serve as the chiral donor and achiral acceptor units, respectively. These exciplexes exhibit CP‐luminescence, with intensity dependent on both the chiral donor and achiral constituents, resulting in emission dissymmetry factors reaching up to 10⁻2 in the thin‐film solid state. Additionally, small singlet‐triplet gaps (∆EST ≤ 0.1 eV) have been measured, leading to TADF characteristics with a photoluminescence quantum yield of 20% for the most efficient emitter, which is also successfully used in non‐optimized organic lightemitting diodes (OLEDs). Interestingly, these chiral exciplexes allow us to explore the impact of the locally‐excited (LE) state of the chiral donor on overall exciplex emission, particularly in relation to the intensity of polarized emission—potentially highlighting a key factor in the design of this type of bimolecular CP‐TADF emitter. [ABSTRACT FROM AUTHOR]

Exciplex emitters have been extensively studied owing to their natural thermally activated delayed fluorescence characteristic, and many efforts have been made to improve their performance in organic light emitting diodes (OLEDs). In this work, the authors propose a novel strategy by introducing intermolecular hydrogen bond (HB) between electron‐donating and electron‐accepting constituting molecules (D and A) to suppress non‐radiative transition of exciplex emitters and thus improve their efficiencies and stabilities in the OLEDs. Accordingly, three exciplex emitters are constructed by using 1,3‐di(10H‐phenoxazin‐10‐yl)benzene (13PXZB) as donor and 4,6‐bis(3,5‐di(pyridin‐4‐yl)phenyl)‐2‐methylpyrimidine (B4PyMPM), 4,6‐bis(3,5‐di(pyridin‐3‐yl)phenyl)‐2‐methylpyrimidine (B3PyMPM), and 4,6‐bis(3,5‐di(pyridin‐2‐yl)phenyl)‐2‐methylpyrimidine (B2PyMPM) as acceptors. With the most intermolecular HBs, 13PXZB:B4PyMPM shows the highest photoluminescence quantum yield (69.6%) and the lowest rate constant of non‐radiative process of triplet excitons (3.4 × 105 S−1). And the OLED using 13PXZB:B4PyMPM as the emitter successfully exhibits a much higher external quantum efficiency of 14.6% than other contrastive devices. Moreover, the half lifetime of 13PXZB:B4PyMPM is 4.8 and 8.2 times higher than those of 13PXZB:B3PyMPM and 13PXZB:B2PyMPM in the devices. This work not only demonstrates that intermolecular HBs between D and A molecules can improve the performance of exciplex emitters, but also paves a new route to develop efficient and stable exciplex emitters. [ABSTRACT FROM AUTHOR]

Organic light emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) utilize molecular systems with a small energy splitting between singlet and triplet states. This can either be realized in intramolecular charge transfer states of molecules with near‐orthogonal donor and acceptor moieties or in intermolecular exciplex states formed between a suitable combination of individual donor and acceptor materials. Here, 4,4′‐(9H,9′H‐[3,3′‐bicarbazole]‐9,9′‐diyl)bis(3‐(trifluoromethyl) benzonitrile) (pCNBCzoCF3) is investigated, which shows intramolecular TADF but can also form exciplex states in combination with 4,4′,4′′‐tris[phenyl(m‐tolyl)amino]triphenylamine (m‐MTDATA). Orange emitting exciplex‐based OLEDs additionally generate a sky‐blue emission from the intramolecular emitter with an intensity that can be voltage‐controlled. Electroluminescence detected magnetic resonance (ELDMR) is applied to study the thermally activated spin‐dependent triplet to singlet up‐conversion in operating devices. Thereby, intermediate excited states involved in OLED operation can be investigated and the corresponding activation energy for both, intra‐ and intermolecular based TADF can be derived. Furthermore, a lower estimate is given for the extent of the triplet wavefunction to be ≥ 1.2 nm. Photoluminescence detected magnetic resonance (PLDMR) reveals the population of molecular triplets in optically excited thin films. Overall, the findings allow to draw a comprehensive picture of the spin‐dependent emission from intra‐ and intermolecular TADF OLEDs. [ABSTRACT FROM AUTHOR]

With the inherent organic–metal system property, phosphorescent organic light‐emitting diodes (PhOLEDs) are capable of exhibiting high performance. However, the existence of unintended triplet–triplet annihilation (TTA), which is mainly originated from high triplet exciton density leading to inferior device performance, is a current predicament. For mitigating the TTA in devices, reported herein is an effective host system with the role of precisely controlling the triplet excitons via the multichannel processes, in which a bipolar host material, a hole‐transporting material, and an electron‐transporting material are mixed to manage the triplet exciton transfer. The mixed‐host with so‐called "triplet excitons harvesting" strategy exhibits two concomitant reverse intersystem crossing (RISC) processes that simultaneously occur in the bipolar host material:electron‐transporting material and the host‐transporting material:electron‐transporting material exciplexes, respectively. Highly efficient green and red PhOLEDs are demonstrated by these multichannel processes, in which phosphorescent emitters bis(2‐phenylpyridine) (acetylacetonate) iridium(III) (Ir(ppy)2(acac)) and bis(2‐methyldibenzo[f,h]‐quinoxaline) (acetylacetonate) iridium(III) (Ir(MDQ)2(acac)) are doped into the mixed‐host, respectively. The green and red PhOLEDs realize nearly 30% of maximum external quantum efficiencies of 29.4% and 29.2%, respectively, and also maintain 29.1% and 28.3% at 1000 cd m−2. These excellent efficiencies and low roll‐offs confirm that the concomitant RISC processes effectively manage and utilize triplet excitons. [ABSTRACT FROM AUTHOR]

Near‐infrared exciplex can weaken molecular design difficulties, and has the advantage of easy bathochromic‐shift spectra via selecting the suitable electron donors and acceptors. In this contribution, exciplex is applied to fabricate near‐infrared (NIR) organic light‐emitting diodes (OLEDs) incorporating a synthesized fluorescent material 3‐([1,1″:3′,1″‐terphenyl]‐5′‐yl)acenaphtho[1,2‐b]pyrazine‐8,9‐dicarbonitrile (APDC‐tPh) and a commercially available material 4,4′,4″‐tris(carbazol‐9‐yl)triphenylamine (TCTA). The device having a mixed TCTA:APDC‐tPh as an emitting layer shows a 730 nm NIR emission with a maximum external quantum efficiency (EQE) of about 0.1%, while the device having 2‐[4‐(diphenylamino)phenyl]‐10,10‐dioxide‐9H‐thioxanthen‐9‐one (TXO‐TPA):APDC‐tPh as the emitting layer exhibits an emission peak of 704 nm with a maximum EQE of 1.27%. These results prove the feasibility of fabricating the efficient exciplex‐based NIR OLEDs. [ABSTRACT FROM AUTHOR]

The thermally-activated-delayed-fluorescence (TADF) characteristics makes exciplexes being the hot subject in the organic light-emitting diode (OLED) research field. The theoretical limit for the efficiency of the conventional fluorescent OLEDs have been leaped by exploiting the triplet harvesting ability of exciplexes. Exciplexes are easily formed by blending electron donor molecules and electron acceptor molecules, which are generally hole transporting materials and electron transporting materials, respectively, resulting in easy access for employing exciplexes to OLEDs. We introduce the photo-physical characteristics of exciplexes derived from the charge-transfer characteristics and their application to OLEDs as emitters. Single exciplex-emitting OLEDs as well as exciplex emission-based white OLEDs are covered in this review. [ABSTRACT FROM AUTHOR]

Deep‐red to near‐infrared (NIR) OLEDs, which yield emission peak wavelengths beyond λ=660 nm, are applicable as unique light sources in plant growth or health monitoring systems. Compared with other visible‐spectrum OLEDs, however, research in the field of deep‐red OLEDs is not as advanced. In this work, three new types of dibenzofuran‐based host materials are developed as n‐type exciplex host partners. Combining these with the deep‐red iridium complex bis(2,3‐diphenylquinoxaline)iridium(dipivaloylmethane) ([(DPQ)2Ir(dpm)]) and N,N′‐di(naphalene‐1‐yl)‐N,N′‐diphenylbenzidine (α‐NPD) as a p‐type exciplex host partner, a highly efficient deep‐red OLED can be realized with a maximum external quantum efficiency (ηext,max) of over 16 % with Comission Internationale de l′Éclairge (CIE) coordinates of (0.71, 0.28). In addition, the effect of the doping concentration and the p/n ratio of the exciplex host on the efficiency and the lifetime of the OLEDs are investigated. Consequently, the optimized device exhibits a ηext,max of over 15 % and a six‐time longer lifetime operating at high brightness of 100 cd m−2 compared with other state‐of‐the‐art deep‐red OLEDs. [ABSTRACT FROM AUTHOR]

In this paper, multiple-exciplexed white organic light-emitting diodes (WOLEDs) with blue and yellow - green emitting layers (EMLs) to improve charge balance and efficiency roll-off through exciton confinement are investigated. Several types of WOLEDs are fabricated a number of including exciplex generated by only host materials without fluorescent or phosphorescent dopant. Moreover, various multiple exciplex can control electrical behavior of holes and electrons in whole EML. The performance improvement by the insertion of multi-EMLs is realized throughout enhancement of exciton confinement and the reduced exciton quenching in EML. Efficiency roll-off was 40% improved comparing to WOLED without multi-EMLs and also color rendering index was achieved higher than 70 at 1000 cd m-2 in WOLED with multi-EMLs. [ABSTRACT FROM AUTHOR]

Aromatic difluoroboronated β-diketone ( BF2DK) derivatives are a widely known class of luminescent organic materials that exhibit high photoluminescent quantum efficiency and unique aggregation-dependent fluorescence behavior. However, there have been only a few reports on their use in solid-state electronic devices, such as organic light-emitting devices (OLEDs). Herein, we investigated the solid-state properties and OLED performance of a series of π-extended BF2DK derivatives that have previously been shown to exhibit intense fluorescence in the solution state. The BF2DK derivatives formed exciplexes with a carbazole derivative and exhibited thermally activated delayed fluorescence (TADF) behavior to give orange electroluminescence with a peak external quantum efficiency of 10 % that apparently exceeds the theoretical efficiency limit of conventional fluorescent OLEDs (7.5 %), assuming a light out-coupling factor of 30 %. [ABSTRACT FROM AUTHOR]

Phosphorescent organic light-emitting diodes (OLEDs) with ultimate efficiency in terms of the external quantum efficiency (EQE), driving voltage, and efficiency roll-off are reported, making use of an exciplex-forming co-host. This exciplex-forming co-host system enables efficient singlet and triplet energy transfers from the host exciplex to the phosphorescent dopant because the singlet and triplet energies of the exciplex are almost identical. In addition, the system has low probability of direct trapping of charges at the dopant molecules and no charge-injection barrier from the charge-transport layers to the emitting layer. By combining all these factors, the OLEDs achieve a low turn-on voltage of 2.4 V, a very high EQE of 29.1% and a very high power efficiency of 124 lm W−1. In addition, the OLEDs achieve an extremely low efficiency roll-off. The EQE of the optimized OLED is maintained at more than 27.8%, up to 10 000 cd m−2. [ABSTRACT FROM AUTHOR]

[Display omitted] • Four bipolar molecules were designed and synthesized for accessing exciplex and electroplex host systems. • Highly efficient green PhOLED with EQE max of 29.9% was achieved. • Extremely small efficiency roll-offs (1.3% at 1,000 cd m−2; 5.4% at 5,000 cd m−2) were obtained. Host materials are of great significance to achieve high-performance host–guest organic light-emitting diodes (OLEDs) through restraining the exciton annihilation in the emissive layer. Herein, four bipolar molecules bearing benzothienocarbazole (BTCz)/benzothienocarboline (BTCb) and benzimidazole (Bi) moieties were designed and synthesized. Using them as hosts, green phosphorescent OLEDs (PhOLEDs) with maximum current efficiency (CE max) of 90.8 cd A−1, power efficiency (PE max) of 76.5 lm W−1, and external quantum efficiency (EQE max) of 27.9% were obtained. More importantly, it was found that these four molecules could be used as electron-donating materials to interact with electron-accepting triazine derivatives to form electroplexes. Employing these electroplexes as hosts, highly efficient green PhOLEDs with CE max of 104.4 cd A−1, PE max of 85.1 lm W−1, EQE max of 29.9%, and extremely small efficiency roll-offs (EQE = 29.5%, 1.3% roll-off at 1,000 cd m−2; EQE = 28.3%, 5.4% roll-off at 5,000 cd m−2) were achieved. The excellent device performances fully exhibit the promising potential of electroplexes as hosts for high-performing OLEDs. [ABSTRACT FROM AUTHOR]

On page 4914, J.‐J. Kim and co‐workers use an exciplex‐forming co‐host to create phosphorescent organic light‐emitting diodes with ultimate efficiencies reported in terms of the external quantum efficiency (EQE), driving voltage, and efficiency rolloff. The image expresses the formation of an exciplex by the recombination of an electron and a hole, followed by energy transfer from the exciplex‐forming co‐host to the dopant, and the luminescence of the green light from the dopant. [ABSTRACT FROM AUTHOR]