Aromatic‐Imide‐Based Thermally Activated Delayed Fluorescence Materials for Highly Efficient Organic Light‐Emitting Diodes

Aromatic‐imide‐based thermally activated delayed fluorescence (TADF) materials with a twisted donor–acceptor–donor skeleton were efficiently synthesized and exhibited excellent thermal stability and high photoluminescence quantum yields. The small ΔE _ST value (<0.1 eV) along with the clear temperature‐dependent delayed component of their transient photoluminescence (PL) spectra demonstrated their excellent TADF properties. Moreover, the performance of organic light‐emitting diodes in which TADF materials AI‐Cz and AI‐TBCz were used as dopants were outstanding, with external quantum efficiencies up to 23.2 and 21.1 %, respectively.     

Four‐Coordinate Boron Emitters with Tridentate Chelating Ligand for Efficient and Stable Thermally Activated Delayed Fluorescence Organic Light‐Emitting Devices

A new class of four‐coordinate donor‐acceptor fluoroboron‐containing thermally activated delayed fluorescence (TADF) compounds bearing a tridentate 2,2′‐(pyridine‐2,6‐diyl)diphenolate (dppy) ligand has been successfully designed and synthesized. Upon varying the donor moieties from carbazole to 10H‐spiro[acridine‐9,9′‐fluorene] to 9,9‐dimethyl‐9,10‐dihydroacridine, these boron derivatives exhibit a wide range of emission colors spanning from blue to yellow with a large spectral shift of 2746 cm^?1, with high PLQYs of up to 96 % in the doped thin film. Notably, vacuum‐deposited organic light‐emitting devices (OLEDs) made with these boron compounds demonstrate high performances with the best current efficiencies of 55.7 cd A^?1, power efficiencies of 58.4 lm W^?1 and external quantum efficiencies of 18.0 %. More importantly, long operational stabilities of the green‐emitting OLEDs based on 2 with half‐lifetimes of up to 12 733 hours at an initial luminance of 100 cd m^?2 have been realized. This work represents for the first time the design and synthesis of tridentate dppy‐chelating four‐coordinate boron TADF compounds for long operational stabilities, suggesting great promises for the development of stable boron‐containing TADF emitters.     

Bipolar Host Materials for Organic Light‐Emitting Diodes

It is important to balance holes and electrons in the emitting layer of organic light‐emitting diodes to maximize recombination efficiency and the accompanying external quantum efficiency. Therefore, the host materials of the emitting layer should transport both holes and electrons for the charge balance. From this perspective, bipolar hosts have been popular as the host materials of thermally activated delayed fluorescent devices and phosphorescent organic light‐emitting diodes. In this review, we have summarized recent developments of bipolar hosts and suggested perspectives of host materials for organic light‐emitting diodes.     

Synthesis,Characterization, and Functionalization of 1‐Boraphenalenes

1‐Boraphenalenes have been synthesized by reaction of BBr₃ with 1‐(aryl‐ethynyl)naphthalenes, 1‐ethynylnaphthalene, and 1‐(pent‐1‐yn‐1‐yl)naphthalene and they can be selectively functionalized at boron or carbon to form bench‐stable products. All of these 1‐boraphenalenes have LUMOs localized on the planar C₁₂B core that are closely comparable in character to isoelectronic phenalenyl cations. In contrast to the comparable LUMOs, the aromatic stabilization of the C₅B ring in 1‐boraphenalenes is dramatically lower than the C₆ rings in phenalenyl cations. This is due to the occupied orbitals of π symmetry being less delocalised in the 1‐boraphenalenes.     

High‐Performance CsPb1−xSnxBr3 Perovskite Quantum Dots for Light‐Emitting Diodes

All inorganic CsPbBr₃ perovskite quantum dots (QDs) are potential emitters for electroluminescent displays. We have developed a facile hot‐injection method to partially replace the toxic Pb²⁺ with highly stable Sn⁴⁺. Meanwhile, the absolute photoluminescence quantum yield of CsPb_1−x Sn_x Br₃ increased from 45 % to 83 % with Sn^IV substitution. The transient absorption (TA) exciton dynamics in undoped CsPbBr₃ and CsPb_0.67Sn_0.33Br₃ QDs at various excitation fluences were determined by femtosecond transient absorption, time‐resolved photoluminescence, and single‐dot spectroscopy, providing clear evidence for the suppression of trion generation by Sn doping. These highly luminescent CsPb_0.67Sn_0.33Br₃ QDs emit at 517 nm. A device based on these QDs exhibited a luminance of 12 500 cd m⁻², a current efficiency of 11.63 cd A⁻¹, an external quantum efficiency of 4.13 %, a power efficiency of 6.76 lm w⁻¹, and a low turn‐on voltage of 3.6 V, which are the best values among reported tin‐based perovskite quantum‐dot LEDs.     

Photoprogrammable Organic Light‐Emitting Diodes

Enlightening the memory : The integration of a crosslinkable photochromic dithienylperfluorocyclopentene (DTE) into organic light‐emitting diodes (OLED) allows for the individualization of the emissive area of the OLED device, for example, for signage applications. The operation principle is based on switching the injection barrier for holes (positive charge carriers). Very large ON/OFF ratios of up to 3000 for current as well as electroluminescence have been achieved.

     

Lewis Acid–Base Interaction‐Controlled ortho‐Selective C−H Borylation of Aryl Sulfides

An iridium/bipyridine‐catalyzed ortho ‐selective C−H borylation of aryl sulfides was developed. High ortho ‐selectivity was achieved by a Lewis acid–base interaction between a boryl group of the ligand and a sulfur atom of the substrate. This is the first example of a catalytic and regioselective C−H transformation controlled by a Lewis acid–base interaction between a ligand and a substrate. The C−H borylation reaction could be conducted on a gram scale, and with a bioactive molecule as a substrate, demonstrating its applicability to late‐stage regioselective C−H borylation. A bioactive molecule was synthesized from an ortho ‐borylated product by converting the boryl and methylthio groups of the product.     

Aggregation‐Induced Delayed Fluorescence Luminogens for Efficient Organic Light‐Emitting Diodes

Aggregation‐induced delayed fluorescence (AIDF) can be regarded as a special case of aggregation‐induced emission (AIE). Luminogens with AIDF can simultaneously emit strongly in solid state and fully utilize the singlet and triplet excitons in organic light‐emitting diodes (OLEDs). In this work, two new AIDF luminogens, DMF‐BP‐DMAC and DPF‐BP‐DMAC, with an asymmetric D–A–D′ structure, are designed and synthesized. The characteristics of both luminogens are systematically investigated, including single crystal structures, theoretical calculations, photophysical properties and thermal stabilities. Inspired by their AIDF nature, the green‐emission non‐doped OLEDs based on them are fabricated, which afford good electroluminescence performances, with low turn‐on voltages of 2.8 V, high luminance of 52560 cd m^?2, high efficiencies of up to 14.4 %, 42.3 cd A^?1 and 30.2 lm W^?1, and very small efficiency roll‐off. The results strongly indicate the bright future of non‐doped OLEDs on the basis of robust AIDF luminogens.     

Luminescent Tungsten(VI) Complexes: Photophysics and Applicability to Organic Light‐Emitting Diodes and Photocatalysis

The synthesis, excited‐state dynamics, and applications of two series of air‐stable luminescent tungsten(VI) complexes are described. These tungsten(VI) complexes show phosphorescence in the solid state and in solutions with emission quantum yields up to 22 % in thin film (5 % in mCP) at room temperature. Complex 2 c , containing a 5,7‐diphenyl‐8‐hydroxyquinolinate ligand, displays prompt fluorescence (blue–green) and phosphorescence (red) of comparable intensity, which could be used for ratiometric luminescent sensing. Solution‐processed organic light‐emitting diodes (OLEDs) based on 1 d showed a stable yellow emission with an external quantum efficiency (EQE) and luminance up to 4.79 % and 1400 cd m⁻² respectively. These tungsten(VI) complexes were also applied in light‐induced aerobic oxidation reactions.     

Broadband Cr3+, Sn4+‐Doped Oxide Nanophosphors for Infrared Mini Light‐Emitting Diodes

Light‐emitting diodes break barriers of size and performance for displays. With devices becoming smaller, the materials also need to get smaller. Chromium(III)‐doped oxide phosphors, which emit near‐infrared (NIR) light, have recently been used in small electronic devices. In this work, mesoporous silica nanoparticles were used as nanocarriers. The nanophosphor ZnGa₂O₄:Cr³⁺,Sn⁴⁺ formed in the mesopore after sintering. Good dispersity and morphology were performed with average diameters of 71±7 nm. It emitted light at 600–850 nm; the intensity was optimized by tuning the doping ratio of Cr³⁺ and Sn⁴⁺. Meanwhile, the light conversion efficiency increased from 7.8 % to 37 % and the molar concentration increased from 0.125 m to 0.5 m . The higher radiant flux of 3.3 mW was obtained by operating an input current of 45 mA. However, the NIR nanophosphor showed good performance on mini light‐emitting diode chips.     

Versatile Synthesis of Luminescent Tetradentate Cyclometalated Alkynylgold(III) Complexes and Their Application in Solution‐Processable Organic Light‐Emitting Devices

A new class of cyclometalated tetradentate alkynylgold(III) complexes has been successfully synthesized by post‐synthetic modification. Through the judicious design and choice of pincer ligands, post‐synthetic cyclization could be achieved to produce the robust and structurally rigid class of tetradentate gold(III) C^N^C^C complexes with high photoluminescence quantum yields of up to 0.49 in solution and 0.78 in doped thin films at room temperature, at least an order of magnitude higher than those of the structurally related uncyclized tridentate alkynylgold(III) analogues. High‐performance yellow to orange‐red emitting solution‐processable organic light‐emitting devices have also been achieved with external quantum efficiency of 11.1 %. This work describes for the first time of the use of post‐synthetic ligand modification approach to overcome the synthetic challenge for tetradentate alkynylgold(III) complexes.     

Doping‐Free White Organic Light‐Emitting Diodes

Doping‐free white organic light‐emitting diodes (WOLEDs) have great potential to the next‐generation solid‐state lighting and displays due to the excellent properties, such as high efficiency, bright luminance, low power consumption, simplified structure and low cost. In this account, our recent developments on doping‐free WOLEDs have been summarized. Firstly, fundamental concepts of doping‐free WOLEDs have been described. Then, the effective strategies to develop doping‐free WOLEDs have been presented. Particularly, the manipulation of charges and excitons distribution in different kinds of doping‐free WOLEDs have been highlighted, including doping‐free fluorescent/phosphorescent hybrid WOLEDs, doping‐free thermally activated delayed fluorescent WOLEDs and doping‐free phosphorescent WOLEDs. In the end, an outlook for the future development of doping‐free WOLEDs have been clarified.