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Rationally tuning the emission position and narrowing the full width at half‐maximum (FWHM) of an emitter is of great importance for many applications. By synergistically improving rigidity, strengthening the resonant strength, inhibiting molecular bending and rocking, and destabilizing the HOMO energy level, a deep‐blue emitter (CZ2CO) with a peak wavelength of 440 nm and an ultranarrow spectral FWHM of 16 nm (0.10 eV) was developed via intramolecular cyclization in a carbonyl/N resonant core (QAO). The dominant υ0‐0 transition character of CZ2CO gives a Commission Internationale de I'Éclairage coordinates (CIE) of (0.144, 0.042), nicely complying with the BT.2020 standard. Moreover, a hyper‐fluorescent device based on CZ2CO shows a high maximum external quantum efficiency (EQEmax) of 25.6 % and maintains an EQE of 22.4 % at a practical brightness of 1000 cd m−2. [ABSTRACT FROM AUTHOR]

High‐performance nondoped organic light‐emitting diodes (OLEDs) are promising technologies for future commercial applications. Herein, we synthesized two new thermally activated delayed fluorescence (TADF) emitters that enable us, for the first time, to combine three effective approaches for enhancing the efficiency of nondoped OLEDs. First, the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching. On the other hand, each of the two emitters has two stable conformations in solid films. In their neat films, molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation. One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of "self‐doped" neat films. Furthermore, both emitters have relatively high aspect ratios in terms of their molecular shapes. This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical out‐coupling. With these three factors, OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100% exciton utilization and deliver over 30% external quantum efficiencies and ultralow efficiency roll‐off at high brightness, which have not been observed in reported nondoped OLEDs. [ABSTRACT FROM AUTHOR]

Multiple resonance (MR) type thermally activated delayed fluorescence (TADF) material is currently a research hotspot in organic light‐emitting diodes (OLEDs) due to their high color purity and high exciton utilization. However, there are only a handful of MR‐TADF emitters with emissions beyond the blue‐to‐green region. The very limited emission colors for MR‐TADF emitters are mainly caused by the fact that so far molecular modifications of MR‐TADF do not offer much change in the emission colors. Here, we report a new approach to modifying a prototypical MR core of DABNA by fusing carbazoles to the MR framework. The carbazole‐fused molecule (TCZ‐F‐DABNA) basically maintains the MR‐dominated features of DABNA while red‐shifting the emission. Its OLED achieves an external quantum efficiency of 39.2 % with a peak at 588 nm, which is a record‐high efficiency for OLEDs with peaks beyond 560 nm. This work provides a new approach for significantly tunning emission colors of MR‐TADF emitters. [ABSTRACT FROM AUTHOR]

Non‐doped organic light‐emitting diodes (OLEDs) are particularly appealing due to the merit of the extremely simple device structure. However, the performance of non‐doped OLEDs is usually far inferior than that of doped devices, mainly due to the lack of desirable emitters. An ideal emitter for non‐doped OLEDs should not merely be highly emissive in the host matrix but also be capable of delivering excellent properties in its condensed state. Herein, through molecular engineering, an "axial and equatorial carbazolyl extension" approach to manipulate the molecular packing behavior is developed, and thus, the emitter is awarded with superior properties in its neat film. Based on this approach, through simply modifying the conventional acridine donor in a thermally activated delayed fluorescence (TADF) emitter with carbazole moieties in the way of hyper‐conjugation, two new TADF emitters with the molecular skeleton being extended both horizontally and vertically by carbazole moieties are constructed. The resulted TADF emitters reveal superb properties with simultaneous excellent thermal and morphological stabilities, photophysical behaviors, and charge transporting ability in their neat film. Owing to the merits of these synergistic superior properties, highly efficient non‐doped green emissive OLED with the state‐of‐the‐art external quantum efficiency of nearly 30% is realized. [ABSTRACT FROM AUTHOR]

Upon fusing the pyrazinyl pyrazole entity in giving pyrazolo[3,4‐f]quinoxaline chelate, the corresponding Os(II) based NIR emitter exhibited "invisible" and efficient electroluminescence with a peak maximum at 811 nm. A maximum external quantum efficiency of 0.97 % and a suppressed efficiency roll‐off till a current density of 300 mA cm−2 was also exhibited. [ABSTRACT FROM AUTHOR]

The conformational distribution and mutual interconversion of thermally activated delayed fluorescence (TADF) emitters significantly affect the exciton utilization. However, their influence on the photophysics in amorphous film states is still not known due to the lack of a suitable quantitative analysis method. Herein, we used temperature‐dependent time‐resolved photoluminescence spectroscopy to quantitatively measure the relative populations of the conformations of a TADF emitter for the first time. We further propose a new concept of "self‐doping" for realizing high‐efficiency nondoped OLEDs. Interestingly, this "compositionally" pure film actually behaves as a film with a dopant (quasi‐equatorial form) in a matrix (quasi‐axial form). The concentration‐induced quenching that may occur at high concentrations is thus expected to be effectively relieved. The "self‐doping" OLED prepared with the newly developed TADF emitter TP2P‐PXZ as a neat emitting layer realizes a high maximum external quantum efficiency of 25.4 % and neglectable efficiency roll‐off. [ABSTRACT FROM AUTHOR]

Organic light‐emitting diodes (OLEDs) with simple nondoped device structure are extremely attractive for real applications since excitons can be utilized without considering the possible charge trapping and morphology issues in the host–dopant systems. Emitters with suppressed concentration annihilation capability are essential for nondoped devices. Herein, two thermally activated delayed fluorescence (TADF) emitters based on a novel 3D electron donor, namely, TDMAC, are constructed. The TDMAC donor consists of a conventional donor with fused triptycene scaffold. Benefitting from the unique rigid and bulky triptycene moiety, these TADF emitters exhibit excellent thermal, morphological, and photophysical properties. Consequently, highly efficient OLEDs with external quantum efficiencies up to 24.2% and 23% are realized for doped and nondoped devices, respectively. [ABSTRACT FROM AUTHOR]

Near‐infrared (NIR) organic‐light emitting devices (OLEDs) with high radiance are useful for applications including invisible marking, communication, and biomedical imaging. However, performances of NIR OLEDs are typically limited by their severe efficiency roll‐offs at high current density. Herein, three isoquinolinyl azolate based Os(II) complexes (Isq‐1–3) with short radiative decay lifetime (in hundreds of ns), and photoluminescence with peak wavelengths > 745 nm and quantum yield up to 48% as doped thin films, are reported. Upon concomitant employment of exciplex‐forming co‐host (tris(4‐carbazoyl‐9‐ylphenyl)amine and 2,4,6‐tris(biphenyl‐3‐yl)‐1,3,5‐triazine), efficiency roll‐off is greatly reduced, giving external quantum efficiency of 9.66% at a current density of 300 mA cm−2. A maximum radiance over 170 W sr−1 m−2 is also achieved in devices based on Isq‐2 and Isq‐3. [ABSTRACT FROM AUTHOR]

The design of square‐planar Pt(II) complexes with highly efficient solid‐state near infrared (NIR) luminescence for electroluminescence is attractive but challenging. This study presents the fine‐turning of excited‐state properties and application of a series of isoquinolinyl pyrazolate Pt(II) complexes that are modulated by steric demanding substituents. It reveals that the bulky substituents do not always disfavor metallophilic Pt···Pt interactions. Instead, π–π stacking among chelates, which are fine‐tuned by the associated substituents, also exerts strong influence to the metal‐metal‐to‐ligand charge transfer (MMLCT) transition character. Theoretical calculations indicate that Pt···Pt contacts become more relevant in the trimers rather than the dimers, especially in their T1 states, associated with a change from mixed 3LC/3MLCT transition in the monomer/dimer to mixed 3LC/3MMLCT transition character in the trimer. Electroluminescence devices affording intense deep‐red/NIR emission (near 670 nm) with unprecedentedly high external quantum efficiency over 30% are demonstrated. This work provides deep insights into formation MMLCT transition of square‐planar Pt(II) complexes and efficient molecular design for deep‐red/NIR electroluminescence. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) provides great potential for the realization of efficient and stable organic light‐emitting diodes (OLEDs). However, it is still challenging for blue TADF emitters to simultaneously achieve high efficiency, high brightness, and low Commission Internationale de l'Eclairage (CIE) y coordinate (CIEy) value. Here, the design and synthesis of two new benzonitrile‐based TADF emitters (namely 2,6‐di(9H‐carbazol‐9‐yl)‐3,5‐bis(3,6‐diphenyl‐9H‐carbazol‐9‐yl)benzonitrile (2PhCz2CzBn) and 2,6‐di(9H‐carbazol‐9‐yl)‐3,5‐bis(3,6‐di‐tert‐butyl‐9H‐carbazol‐9‐yl)benzonitrile (2tCz2CzBn)) with a symmetrical and rigid heterodonor configuration are reported. The TADF OLEDs doped with both the emitters can achieve a high external quantum efficiency (EQE) over 20% and narrowband blue emission of 464 nm with a CIEy < 0.2. Moreover, the incorporation of a terminal tert‐butyl group can weaken the intermolecular π–π stacking in the nondoped TADF emitter, and thus significantly suppress self‐aggregation‐caused emission quenching for enhanced delayed fluorescence. A peak EQE of 21.6% is realized in the 2tCz2CzBn‐based nondoped device with an extremely low turn‐on voltage of 2.7 V, high color stability, a high brightness over 20 000 cd m−2, a narrow full‐width at half‐maximum of 70 nm, and CIE color coordinates of (0.167, 0.248). [ABSTRACT FROM AUTHOR]

A new ternary acceptor (A)–donor (D)–acceptor (A) asymmetrically twisted deep‐blue emitting molecule, PPI‐2BI, was synthesized by attaching two electrophilic benzimidazole (BI) units to the C2 and N1 positions of a phenanthroimidazole (PI) donor unit. Profiting from the enhanced D–A electronic coupling, the electron injecting and transporting abilities of the new triangle‐shaped A–D–A molecule are considerably improved and the molecule shows high photoluminescence (PL) and electroluminescence (EL) efficiencies. By using PPI‐2BI as a non‐doped emitting layer (EML), the resulting organic light‐emitting device exhibits emission with color coordinates of (0.158, 0.124) and a maximum external quantum efficiency (EQE), current efficiency (CE), and power efficiency (PE) of 4.63 %, 4.98 cd A−1, and 4.82 lm W−1, respectively. Additionally, a simple bilayer device using PPI‐2BI as both the EML and the electron‐transporting layer (ETL) also shows an EQE of 3.81 % with little changes to the color purity. Remarkably, a PPI‐2BI‐based doped device emits efficient near‐ultraviolet EL with color coordinates of (0.154, 0.047) and an EQE of 4.12 %, which is comparable to that of the best reported near‐UV emitting devices. Triangular A–D–A: A new ternary acceptor (A)–donor (D)–acceptor (A) asymmetrically twisted deep‐blue emitting molecule, PPI‐2BI, is synthesized by attaching two electrophilic benzimidazole (BI) units to the C2 and N1 positions of a phenanthroimidazole (PI) donor unit. Profiting from the enhanced D–A electronic coupling, the electron injecting and transporting abilities of the new triangle‐shaped A–D–A molecule are considerably improved and the molecule shows high photoluminescence and electroluminescence efficiencies. [ABSTRACT FROM AUTHOR]

Abstract: Organic light‐emitting diodes (OLEDs) are the most successful product of organic electronics in the market and continually receive attention from scientific and industrial communities. Imidazoles have been extensively investigated for OLED applications, and demonstrated their versatility in molecular design for different functions. This review presents a summary of recent studies on imidazole (including imidazole derived moieties) derivatives, with special focus on discussing various molecular design tactics, for applications as electron‐transporting materials, emitters, and host materials in OLEDs. At last, perspectives and challenges regarding to imidazole semiconductors for electroluminescence applications are also discussed. [ABSTRACT FROM AUTHOR]

A blue fluorescent compound, 9-[4-(4,6-diphenoxy-1,3,5-triazin-2-yl)phenyl]-9 H-carbazole (POTC), the triplet energy level of which reaches 2.76 eV, has been designed and synthesized. POTC is an excellent blue emitter as well as host for green and red phosphors, and therefore, matches the requirements of the host for single-emitting-layer fluorescence and phosphorescence hybrid white organic light-emitting diodes (OLEDs). The blue, green, red, and white devices based on POTC show maximum external quantum efficiencies (EQEs) of 2.4, 22.4, 13.0, and 8.1 %, respectively. Even at a high brightness of 1000 cd m−2, these values maintain EQEs of 2.3, 22.1, 11.1, and 7.0 %, respectively, indicating less than 15 % roll-offs from the maxima. [ABSTRACT FROM AUTHOR]

A new triphenylamine-bridged fluoranthene derivative, 4-(7,10-diphenylfluoranthen-8-yl)- N-[4-(7,10-diphenylfluoranthen-8-yl)phenyl]- N-phenylaniline (BDPFPA), with a high glass transition temperature of 220 °C has been synthesized and characterized. BDPFPA is a highly fluorescent and versatile material that can be used as a nondoped green emitter and as a hole transporter. BDPFPA was used in a standard trilayer device as the emitting layer, which showed a low turn-on voltage (<3 V) and a high efficiency of 11.6 cd A−1. The device also shows little efficiency roll-off at high brightness. For example, the efficiency can still be maintained at 11.4 cd A−1 (5.4 lm W−1) at a brightness of 10 000 cd m−2. These results are among the best reported for nondoped fluorescent green organic light-emitting diodes. A simple bilayer device, in which BDPFPA serves as a hole-transporting layer, has a maximum power efficiency of 3.3 lm W−1 and the performance is nearly 40 % higher than that of an N, N′-bis(1-naphthyl)- N, N′- diphenyl-1,1′-biphenyl-4,4′-diamine (NPB)-based standard device. [ABSTRACT FROM AUTHOR]

Tremendous effort has been devoted to developing novel near‐infrared (NIR) emitters and to improving the performance of NIR organic light‐emitting diodes (OLEDs). Os(II) complexes are known to be an important class of NIR electroluminescent materials. However, the highest external quantum efficiency achieved so far for Os(II)‐based NIR OLEDs with an emission peak wavelength exceeding 700 nm is still lower than 3%. A new series of Os(II) complexes (1–4) based on functional pyrazinyl azolate chelates and dimethyl(phenyl)phosphane ancillaries is presented. The reduced metal‐to‐ligand charge transfer (MLCT) transition energy gap of pyrazinyl units in the excited states results in efficient NIR emission for this class of metal complexes. Consequently, NIR OLEDs based on 1–4 show excellent device performance, among which complex 4 with a triazolate fragment gives superior performance with maximum external quantum efficiency of 11.5% at peak wavelength of 710 nm, which represent the best Os(II)‐based NIR‐emitting OLEDs with peak maxima exceeding 700 nm. [ABSTRACT FROM AUTHOR]

Transparent flexible organic light‐emitting diodes (TF‐OLEDs) are emerging as a leading technique in bendable display and curved lighting applications due to their merits including superior mechanical flexibility, low power consumption, and broad color gamut. However, it is challenging to turn TF‐OLEDs into a power‐efficient large‐area light source. Here, an improved TF‐OLED structure on a plastic substrate that achieves a device transparency over 70% and extremely efficient warm‐white emission from both sides is reported. The key feature of this device structure is the combination of transparent metal–dielectric composite electrodes, which are patterned with moth‐eye nanostructures for broadband and angle‐independent light outcoupling. By collectively reducing ohmic losses and releasing the trapped photons, the TF‐OLEDs achieve a record external quantum efficiency of 72.4% and power efficiency of 168.5 lm W−1 with a color‐rendering index over 84. These results present the great potential of TF‐OLEDs for use in a wide variety of flexible applications. By taking a full advantage of the optical design, an extremely efficient transparent flexible organic light‐emitting diode achieves a record external quantum efficiency of 72.4% and power efficiency of 168.5 lm W−1 for white emission with a color‐rendering‐index of 84.5. The substantial increase in efficiency is due to the synergetic interplay of light outcoupling enhancement and minimized surface plasmon losses. [ABSTRACT FROM AUTHOR]

To increase the fluorescence quantum yield of hybrid local and charge-transfer (HLCT) material, we introduce a symmetric linear D- π -A- π -D structure into molecular design and synthesized a new blue emitter, 2,2'-(2′,3′,5′,6'-tetrafluoro-[1,1':4′,1″-terphenyl]-4,4″-diyl)bis(1-(4-( tert -butyl)phenyl)-1 H -phenanthro[9,10- d ]imidazole) ( 4FBTPI ). Organic light-emitting devices employing 4FBTPI as a dopant emitter show good performances, with CIE (Commission Internationale de l’Enclairage) coordinates of (0.15, 0.09), which is very close to NTSC blue light standard (0.14, 0.08), current efficiencies (CE) of 6.03 cd A −1 , external quantum efficiencies of 6.94%. This performance is comparable to those of recently reported state-of-the-art deep-blue materials with CIE y < 0.10. [ABSTRACT FROM AUTHOR]