Organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) materials are promising for the realization of highly efficient light emitters. However, such devices ...have so far suffered from efficiency roll-off at high luminance. Here, we report the design and synthesis of two diboron-based molecules, CzDBA and tBuCzDBA, which show excellent TADF properties and yield efficient OLEDs with very low efficiency roll-off. These donor–acceptor–donor (D–A–D) type and rod-like compounds concurrently generate TADF with a photoluminescence quantum yield of ~100% and an 84% horizontal dipole ratio in the thin film. A green OLED based on CzDBA exhibits a high external quantum efficiency of 37.8 ± 0.6%, a current efficiency of 139.6 ± 2.8 cd A−1 and a power efficiency of 121.6 ± 3.1 lm W−1 with an efficiency roll-off of only 0.3% at 1,000 cd m−2. The device has a peak emission wavelength of 528 nm and colour coordinates of the Commission International de l´Eclairage (CIE) of (0.31, 0.61), making it attractive for colour-display applications.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, SBMB, UL, UM, UPUK
Highly efficient thermally activated delayed fluorescence (TADF) molecules are in urgent demand for solid‐state lighting and full‐color displays. Here, the design and synthesis of three ...triarylamine‐pyridine‐carbonitrile‐based TADF compounds, TPAPPC, TPAmPPC, and tTPAmPPC, are shown. They exhibit excellent photoluminescence quantum yields of 79−100% with small ΔEST values, fast reverse intersystem crossing (RISC), and high horizontal dipole ratios (Θ// = 86−88%) in the thin films leading to the enhancement of device light outcoupling. Consequently, a green organic light‐emitting diode (OLED) based on TPAmPPC shows a high average external quantum efficiency of 38.8 ± 0.6%, a current efficiency of 130.1 ± 2.1 cd A–1, and a power efficiency of 136.3 ± 2.2 lm W–1. The highest device efficiency of 39.8% appears to be record‐breaking among TADF‐based OLEDs to date. In addition, the TPAmPPC‐based device shows superior operation lifetime and high‐temperature resistance. It is worth noting that the TPA‐PPC‐based materials have excellent optical properties and the potential for making them strong candidates for TADF practical application.
Three 2,6‐diphenylpyridine‐3,5‐dicarbonitrile‐based compounds with excellent photoluminescent quantum yields (79–100%) and high horizontal dipole ratios (86−88%) in the thin films are demonstrated. With two methyl groups on the triarylamines, the spin−orbit coupling is enhanced due to the elevated locally excited triplet states (3LE), leading to a fast reverse intersystem crossing. Green thermally activated delayed fluorescence (TADF) organic light‐emitting diodes based on them exhibit a record‐high external quantum efficiency of 39.8% without any optical extraction technique.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
This work reports an efficient synthesis of novel benzo7,8indolizino2,3,4,5-
ija
quinazoline derivatives between 2-(2-ethynylaryl)acetonitriles 1 and anthranils 2. The synthetic approach involves the ...initial formation of 7-formylindole intermediates that can be implemented by DBU to activate a novel indole-nitrile-aldehyde cyclization.
This work reports novel gold catalysis and DBU-promoted cyclizations between 2-(2-ethynylaryl)acetonitriles and anthranils to construct benzo7,8indolizino2,3,4,5-
ija
quinazoline frameworks.
Ongoing brain activity can be recorded as electroen-cephalograph (EEG) to discover the links between emotional states and brain activity. This study applied machine-learning algorithms to categorize ...EEG dynamics according to subject self-reported emotional states during music listening. A framework was proposed to optimize EEG-based emotion recognition by systematically 1) seeking emotion-specific EEG features and 2) exploring the efficacy of the classifiers. Support vector machine was employed to classify four emotional states (joy, anger, sadness, and pleasure) and obtained an averaged classification accuracy of 82.29% ± 3.06% across 26 subjects. Further, this study identified 30 subject-independent features that were most relevant to emotional processing across subjects and explored the feasibility of using fewer electrodes to characterize the EEG dynamics during music listening. The identified features were primarily derived from electrodes placed near the frontal and the parietal lobes, consistent with many of the findings in the literature. This study might lead to a practical system for noninvasive assessment of the emotional states in practical or clinical applications.
In this study, a novel perovskite quantum dot (QD) spray‐synthesis method is developed by combining traditional perovskite QD synthesis with the technique of spray pyrolysis. By utilizing this new ...technique, the synthesis of cubic‐shaped perovskite QDs with a homogeneous size of 14 nm is demonstrated, which shows an unprecedented stable absolute photoluminescence quantum yield ≈100% in the solution and even in the solid‐state neat film. The highly emissive thin films are integrated with light emission devices (LEDs) and organic light emission displays (OLEDs). The color conversion type QD‐LED (ccQD‐LED) hybrid devices exhibit an extremely saturated green emission, excellent external quantum efficiency of 28.1%, power efficiency of 121 lm W−1, and extraordinary forward‐direction luminescence of 8 500 000 cd m−2. The conceptual ccQD‐OLED hybrid display also successfully demonstrates high‐definition still images and moving pictures with a 119% National Television System Committee 1931 color gamut and 123% Digital Cinema Initiatives‐P3 color gamut. These very‐stable, ultra‐bright perovskite QDs have the properties necessary for a variety of useful applications in optoelectronics.
Spray‐synthesized perovskite quantum dots (QDs) show an unprecedented cubic shape, and a stable photoluminescence quantum yield of ≈100% in both solution and the solid‐state neat film. QD‐LED (light emission device) and QD‐OLED (organic light emission display) hybrid devices exhibit an excellent external quantum efficiency of 28.1%, a power efficiency of 121 lm W−1, and successfully demonstrate high‐definition motion pictures.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Five emitters CzAZB, tBuCzAZB, tmCzAZB, dmAcAZB, and PxzAZB based on dibenzo-1,4-azaborine as the electron acceptors and two identical amine groups as the donors were designed and synthesized. The ...dihedral angles between the planes of dibenzo-1,4-azaborine acceptors and amine-based donors greatly affect the thermally activated delayed fluorescence (TADF) property of these materials. A simple concept “steric switching” is introduced to predict whether the emitter possesses TADF property. CzAZB and tBuCzAZB, with very high photoluminescence quantum yields (PLQYs) but small dihedral angles, do not show TADF. In contrast, tmCzAZB reveals a PLQY of only 56% but with a large dihedral angle due to the presence of two methyl groups at C1 and C8 of the carbazole groups, the steric switching operates, and the compound shows TADF property with a deep-blue color having CIE coordinates of (0.14, 0.15). In a similar manner, in dmAcAZB and PxzAZB with high PLQYs and large dihedral angles between the donor and acceptor planes, the “TADF steric switch” readily operates to achieve device external quantum efficiencies as high as 20.8 ± 1.2 and 27.5 ± 1.9% with blue and green emissions, respectively.
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IJS, KILJ, NUK, PNG, UL, UM
Ten ionic manganese(II) complexes of EMIm2MnX2Y2 (EMIm=1‐ethyl‐3‐methylimidazolium ion; X, Y=Cl, Br or I) and BnMIm2MnX2Y2 (BnMIm=1‐benzyl‐3‐methylimidazolium ion; X, Y=Cl, Br or I) types were ...synthesized and studied in terms of their thermal and photophysical properties. Complexes with BnMIm+ cation were found to exhibit higher crystallinity, owing to the aromatic π‐stacking, and superior photoluminescent quantum yields, promoted by the increased Mn⋅⋅⋅Mn distance. For complexes with chlorine and bromine ligands efficient tunability of photophysical parameters was demonstrated. Out of all complexes, BnMIm2MnBr4 was found to have the highest photoluminescence quantum yield at room temperature (Φ=0.59). To highlight the importance of a large Mn⋅⋅⋅Mn distance for achieving high Φ values, a mixed‐anion analog of complex BnMIm2MnBr4 was prepared, with the suggested formula of BnMIm4MnBr4Br2. The latter have shown a significant improvement in d–d absorption efficiency and a reduction in nonradiative deactivation, which led to an outstanding Φ value of 0.97. Finally, the optical band gap of BnMIm4MnBr4Br2 was estimated to describe its applicability as light‐emitting material.
A family of luminescent tetrahalidomanganate(II) complexes with imidazolium‐based cations were synthesized and characterized in detail. Their good thermal stability and photophysical tunability were demonstrated. In particular, BnMIm4MnBr4Br2, the complex with a novel mixed‐anion structure, showed exceptionally high photoluminescence quantum yield at room temperature, which suggests its future application as light‐emitting material in optoelectronic devices.
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BFBNIB, FZAB, GIS, IJS, KILJ, OILJ, SBCE, SBMB, UPUK
Owing to the high technology maturity of thermally activated delayed fluorescence (TADF) emitter design with a specific molecular shape, extremely high-performance organic light-emitting diodes ...(OLEDs) have recently been achieved
via
various doping techniques. Recently, undoped OLEDs have drawn immense attention because of their manufacturing cost reduction and procedure simplification. However, capable materials as host emitters are rare and precious because general fluorophores in high-concentration states suffer from serious aggregation-caused quenching (ACQ) and undergo exciton quenching. In this work, a series of diboron materials, CzDBA, iCzDBA, and
t
BuCzDBA, is introduced to realize the effect of steric hindrance and the molecular aspect ratio
via
experimental and theoretical studies. We computed transition electric dipole moment (TEDM) and molecular dynamics (MD) simulations as a proof-of-concept model to investigate the molecular stacking in neat films. It is worth noting that the pure
t
BuCzDBA film with a high horizontal ratio of 92% is employed to achieve a nondoped OLED with an excellent external quantum efficiency of 26.9%. In addition, we demonstrated the first ultrathin emitting layer (1 nm) TADF device, which exhibited outstanding power efficiency. This molecular design and high-performance devices show the potential of power-saving and economical fabrication for advanced OLEDs.
A strategy of substituent engineering of DBA-based molecules is investigated
via
experimental and theoretical methods. A 1 nm-thick emitting layer OLED has been developed.
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IJS, KILJ, NUK, UL, UM, UPUK
Converting solar energy into hydrogen energy using conjugated polymers (CP) is a promising solution to the energy crisis. Improving water solubility plays one of the critical factors in enhancing the ...hydrogen evolution rate (HER) of CP photocatalysts. In this study, a novel concept of incorporating hydrophilic side chains to connect the backbones of CPs to improve their HER is proposed. This concept is realized through the polymerization of carbazole units bridged with octane, ethylene glycol, and penta‐(ethylene glycol) to form three new side‐chain‐braided (SCB) CPs: PCz2S‐OCt, PCz2S‐EG, and PCz2S‐PEG. Verified through transient absorption spectra, the enhanced capability of PCz2S‐PEG for ultrafast electron transfer and reduced recombination effects has been demonstrated. Small‐ and wide‐angle X‐ray scattering (SAXS/WAXS) analyses reveal that these three SCB‐CPs form cross‐linking networks with different mass fractal dimensions (f) in aqueous solution. With the lowest f value of 2.64 and improved water/polymer interfaces, PCz2S‐PEG demonstrates the best HER, reaching up to 126.9 µmol h−1 in pure water‐based photocatalytic solution. Moreover, PCz2S‐PEG exhibits comparable performance in seawater‐based photocatalytic solution under natural sunlight. In situ SAXS analysis further reveals nucleation‐dominated generation of hydrogen nanoclusters with a size of ≈1.5 nm in the HER of PCz2S‐PEG under light illumination.
Pioneer examples of side‐chain‐bridged polymer photocatalysts, of tunable hydrophilicity of the side chains are presented. These polymers are capable of generating hydrogen using natural sunlight in seawater‐based photocatalytic solution. The distinctive structural characteristics and impressive HER performance of the side‐chain‐bridged conjugated polymers suggest a potential avenue in the development of photocatalytic conjugated polymers.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Three pyridine-carbonitrile (PPC) fluorophores with amine-type donors, carbazole,
tert
-butylcarbazole, and spiroacridine have been designed and synthesized. These PPC-based emitters exhibit ...excellent photoluminescence quantum yields of 92-100%, thermally activated delayed fluorescence (TADF) and thermal stability. More importantly, with increasing molecular lengths
via
donor modification strategy, it fulfills the aim to rise the horizontal dipole orientation ratios from 76% to 83%. Remarkably, a high-performance green OLED based on spiroacidine-PPC dopant exhibited an external quantum efficiency of 37.2%, a current efficiency of 123.5 cd A
−1
and a power efficiency of 121.3 lm W
−1
with a relative low driving voltage, only 2.9 V.
Three pyridine-carbonitrile (PPC) fluorophores with amine-type donors, carbazole,
tert
-butylcarbazole, and spiroacridine have been designed and synthesized. A high-performance green OLED based on SAcmPPC dopant exhibited an external quantum efficiency of 37.2%.
