Interfacial Passivation Engineering for Highly Efficient Quantum Dot Light-Emitting Diodes via Aromatic Amine-Functionalized Dipole Molecules.

Blue quantum dot (QD) light-emitting diodes (QLEDs) exhibit unsatisfactory operational stability and electroluminescence (EL) properties due to severe nonradiative recombination induced by large numbers of dangling bond defects and charge imbalance in QD. Herein, dipolar aromatic amine-functionalized molecules with different molecular polarities are employed to regulate charge transport and passivate interfacial defects between QD and the electron transfer layer (ETL). The results show that the stronger the molecular polarity, especially with the -CF3 groups possessing a strong electron-withdrawing capacity, the more effective the defect passivation of S and Zn dangling bonds at the QD surface. Moreover, the dipole interlayer can effectively reduce electron injection into QD at high current density, enhancing charge balance and mitigating Joule heat. Finally, blue QLEDs exhibit a peak external quantum efficiency (EQE) of 21.02% with an operational lifetime (T50 at 100 cd m-2) exceeding 4000 h.

Low-Temperature Cross-Linked Hole Transport Layer for High-Performance Blue Quantum-Dot Light-Emitting Diodes.

Quantum-dot light-emitting diodes (QLEDs), a kind of promising optoelectronic device, demonstrate potential superiority in next-generation display technology. Thermal cross-linked hole transport materials (HTMs) have been employed in solution-processed QLEDs due to their excellent thermal stability and solvent resistance, whereas the unbalanced charge injection and high cross-linking temperature of cross-linked HTMs can inhibit the efficiency of QLEDs and limit their application. Herein, a low-temperature cross-linked HTM of 4,4'-bis(3-(((4-vinylbenzyl)oxy)methyl)-9H-carbazol-9-yl)-1,1'-biphenyl (DV-CBP) with a flexible styrene side chain is introduced, which reduces the cross-linking temperature to 150 °C and enhances the hole mobility up to 1.01 × 10-3 cm2 V-1 s-1. More importantly, the maximum external quantum efficiency of 21.35% is successfully obtained on the basis of the DV-CBP as a cross-linked hole transport layer (HTL) for blue QLEDs. The low-temperature cross-linked high-mobility HTL using flexible side chains could be an excellent alternative for future HTL development.

Unified Crystal Phase Control with MACl for Inducing Single-Crystal-Like Perovskite Thin Films in High-Pressure Fusion Toward High Efficiency Perovskite Solar Cell Modules.

Perovskite solar cells, recognized for their high photovoltaic conversion efficiency (PCE), cost-effectiveness, and simple fabrication, face challenges in PCE improvement due to structural defects in polycrystalline films. This study introduces a novel fabrication method for perovskite films using methylammonium chloride (MACl) to align grain orientation uniformly, followed by a high-pressure process to merge these grains into a texture resembling single-crystal perovskite. Employing advanced visual fluorescence microscopy, charge dynamics in these films are analyzed, uncovering the significant impact of grain boundaries on photo-generated charge transport within perovskite crystals. A key discovery is that optimal charge transport efficiency and speed occur in grain centers when the grain size exceeds 10 µm, challenging the traditional view that efficiency peaks when grain size surpasses film thickness to form a monolayer. Additionally, the presence of large-sized grains enhances ion activation energy, reducing ion migration under light and improving resistance to photo-induced degradation. In application, a perovskite solar cell module with large grains achieve a PCE of 22.45%, maintaining performance with no significant degradation under continuous white LED light at 100 mA cm-2 for over 1000 h. This study offers a new approach to perovskite film fabrication and insights into optimizing perovskite solar cell modules.

Synergetic Electrostatic and Steric Effects in α-FAPbI3 Single Crystals For X-Ray Detection and Imaging.

It is still challenging to stabilize α-FAPbI3 perovskite for high performance optoelectrical devices. Herein, a novel strategy is proposed utilizing the synergetic electrostatic and steric effect to stabilize the α-FAPbI3 phase and suppress the ion migration. Dimethylamine (DMA+) cations are chosen as the dopant to fabricate FA0.96DMA0.04PbI3 single crystals (SCs). DFT calculations reveal that DMA+ cations can improve the stability of α-FAPbI3 phase in both thermodynamics (lower Gibbs free energy) and kinetics (higher defect formation and migration energy). The resulting SCs exhibit an environmental stability over 100 days and an extraordinary low dark current drift of 3.7 × 10-7 nA cm-1 s-1 V-1, comparable to 2D perovskite SCs. The X-ray detectors have also achieved the-state-of-the-art performance in X-ray detection and imaging. This work demonstrates the significance of electrostatic and steric effects in improving the phase and operational stability of perovskites.

Pattern-Matched Polymer Ligands Toward Near-Perfect Synergistic Passivation for High-Performance and Stable Br/Cl Mixed Perovskite Light-Emitting Diodes.

Mixed Br/Cl perovskite nanocrystals (PeNCs) exhibit bright pure-blue emission benefiting for fulfilling the Rec. 2100 standard. However, phase segregation remains a significant challenge that severely affects the stability and emission spectrum of perovskite light-emitting diodes (PeLEDs). Here, we demonstrate the optimization of the spacing between polydentate functional groups of polymer ligands to match the surface pattern of CsPbBr1.8Cl1.2 PeNCs, resulting in effective synergistic passivation effect and significant improvements in PeLED performances. The block and alternating copolymers with different inter-functional group spacing are facilely synthesized as ligands for PeNCs. Surprisingly, block copolymers with a higher functional group density do not match PeNCs, while alternating copolymers enable efficient PeNCs with the high photoluminescence intensity, low non-radiative recombination rate and high exciton binding energy. Density functional theory calculations clearly confirm the almost perfect match between alternating copolymers and PeNCs. Finally, pure-blue PeLEDs are achieved with the emission at 467 nm and Commission Internationale de l'Eclairage (CIE) coordinates of (0.131, 0.071), high external quantum efficiency (9.1 %) and record spectral and operational stabilities (~80 mins) in mixed-halide PeLEDs. Overall, this study contributes to designing the polymer ligands and promoting the development of high-performance and stable pure-color PeLEDs towards display applications.

Bias-Switchable Dual-Mode Organic Photodetector with High Operational Stability Using Self-Trapped Cs3Cu2I5 Interfacial Layer.

Conventional photovoltaic (PV)-photodetectors are hard to detect fainted signals, while photomultiplication (PM)-capable devices indispensable for detecting weak light and are prone to degrade under strong light illumination and large bias, and it is urgent to realize highly efficient integrated detecting system with both PM and PV operation modes. In this work, one lead-free Cs3Cu2I5 nanocrystals with self-trapping exciton nature was introduced as interfacial layer adjacent to bulk and layer-by-layer heterojunction structure, and corresponding organic photodetectors with bias-switchable dual modes are demonstrated. The fabricated device exhibits low operating bias (0 V for PV mode and 0.8 V for PM mode), high specific detectivity (~1013 Jones), fast response speed as low as 1.59 µs, large bandwidth over 0.2 MHz and long-term operational stability last for 4 months in ambient condition. This synergy strategy also validated in different materials and device architectures, providing a convenient and scalable production process to develop highly efficient bias-switchable multi-functional organic optoelectrical applications.

Ultra-Stable and Highly Efficient White Light Emitting Diodes through CsPbBr3 Perovskite Nanocrystals-Silica Composite Phosphor Functionalized with Surface Phenyl Molecules.

Poor stability of CsPbBr3 perovskite nanocrystals (NCs) to moisture/heat/light has significantly limited their application as a green phosphor, despite their outstanding luminescent properties. Here, a remarkably stable CsPbBr3 NCs-silica composite phosphor functionalized with surface phenyl molecules (CsPbBr3 -SiO2 Ph ) is synthesized by controlling low-temperature hydrolysis and condensation reaction of perhydropolysilazane in the presence of CsPbBr3 NCs followed by phenyl-functionalization. Through the process, CsPbBr3 NCs are confined in a compact silica matrix, which is impermeable to H2 O. The synthesis strategy is extended to a classical red quantum dot, CdZnSeS@ZnS NCs, to fabricate a white light emitting diode (WLED) consisting of CsPbBr3 -SiO2 Ph and CdZnSeS@ZnS-SiO2 Ph phosphor and silicone resin packaged on a commercial blue InGaN chip with luminous efficacy (LE) of 9.36 lm W-1 . The WLED undergoes enhancements in both green and red photoluminescence over time to achieve a highly efficient performance of 38.80 lm W-1 . More importantly, the WLED exhibits unprecedented operational stability of LE/LE0  = 94% after 101 h-operation at 20 mA (2.56 V). The ultra-high operational stability and efficient performance are mainly attributed to thermal curing and aging through which grain growth occurs as well as deactivation of defect states by permeated atmospheric O2 .

Thermal Management Enables Stable Perovskite Nanocrystal Light-Emitting Diodes with Novel Hole Transport Material.

The severely insufficient operational lifetime of perovskite light-emitting diodes (LEDs) is incompatible with the rapidly increasing external quantum efficiency, even as it approaches the theoretical limit, thereby significantly impeding the commercialization of perovskite LEDs. In addition, Joule heating induces ion migration and surface defects, degrades the photoluminescence quantum yield and other optoelectronic properties of perovskite films, and induces the crystallization of charge transport layers with low glass transition temperatures, resulting in LED degradation under continuous operation. Here, a novel thermally crosslinked hole transport material, poly(FCA60 -co-BFCA20 -co-VFCA20 ) (poly-FBV), with temperature-dependent hole mobility is designed, which is advantageous for balancing the charge injection of the LEDs and limiting the generation of Joule heating. The optimised CsPbI3 perovskite nanocrystal LEDs with poly-FBV realise approximately a 2-fold external quantum efficiency increase over the LED with commercial hole transport layer poly(4-butyl-phenyl-diphenyl-amine) (poly-TPD), owing to the balanced carrier injection and suppressed exciton quenching. Moreover, because of the Joule heating control provided by the novel crosslinked hole transport material, the LED utilising crosslinked poly-FBV has a 150-fold longer operating lifetime (490 min) than that utilizing poly-TPD (3.3 min). The study opens a new avenue for the use of PNC LEDs in commercial semiconductor optoelectronic devices.

Demonstration of a 263-GHz Traveling Wave Tube for Electron Paramagnetic Resonance Spectroscopy.

In this letter, a 263 GHz traveling wave tube for electron paramagnetic resonance spectroscopy is designed, fabricated and tested. A periodic permanent magnet focused pencil beam electron optical system is adopted. A folded waveguide slow-wave structure with modified serpentine bends is optimized to provide high-power wideband performance and stable operation. An experiment has been performed to verify the analysis results and confirm the amplifier stability. The device provides a maximum 11.9 W saturation output power and 25.5 dB saturation gain. Although the available solid-state signal source is unable to drive the amplifier to saturation beyond 260 - 264 GHz, 10 W output power over 5.6 GHz bandwidth has been measured.

Highly efficient isolation and purification of high-purity tea saponins from industrial camellia oil production by porous polymeric adsorbents.

BACKGROUND: Recovery of high-purity tea saponin (TS), a promising non-ionic surfactant with well-documented properties, is one of the major challenges to broadening its industrial applications. In this study, an innovative and sustainable strategy for the highly-efficient purification of TS was developed by using well-designed highly-porous polymeric adsorbents. RESULTS: The prepared Pp-A with controllable macropores (~96 nm) and appropriate surface hydrophobic properties was found more favorable for achieving high adsorption efficiency towards TS/TS-micelles. Kinetic results showed the adsorption follows the pseudo-second-order model (R2 = 0.9800), and the Langmuir model is more qualified to explicate the adsorption isotherms with Qe-TS ~ 675 mg g-1 . Thermodynamic studies revealed the monolayer adsorption of TS was an endothermic process that was conducted spontaneously. Interestingly, ethanol-driven desorption (90% v/v ethanol) of TS was rapidly (< 30 min) complete due to the possible ethanol-mediated disassembling of TS-micelles. A possible mechanism that involves the interactions between the adsorbents and TS/TS-micelles, the formation and disassembling of TS-micelles was proposed to account for the highly efficient purification of TS. Afterwards, Pp-A-based adsorption method was developed to purify TS directly from industrial camellia oil production. Through selective adsorption, pre-washing, and ethanol-driven desorption, the applied Pp-A enabled the direct isolation of high-purity TS (~96%) with a recovery ratio > 90%. Notably, Pp-A exhibited excellent operational stability and is of high potential for long-term industrial application. CONCLUSION: Results ensured the practical feasibility of the prepared porous adsorbents in purifying TS, and the proposed methodology is a promising industrial-scale purification strategy. © 2023 Society of Chemical Industry.

Managing Excess Lead Iodide with Functionalized Oxo-Graphene Nanosheets for Stable Perovskite Solar Cells.

Stability issues could prevent lead halide perovskite solar cells (PSCs) from commercialization despite it having a comparable power conversion efficiency (PCE) to silicon solar cells. Overcoming drawbacks affecting their long-term stability is gaining incremental importance. Excess lead iodide (PbI2 ) causes perovskite degradation, although it aids in crystal growth and defect passivation. Herein, we synthesized functionalized oxo-graphene nanosheets (Dec-oxoG NSs) to effectively manage the excess PbI2 . Dec-oxoG NSs provide anchoring sites to bind the excess PbI2 and passivate perovskite grain boundaries, thereby reducing charge recombination loss and significantly boosting the extraction of free electrons. The inclusion of Dec-oxoG NSs leads to a PCE of 23.7 % in inverted (p-i-n) PSCs. The devices retain 93.8 % of their initial efficiency after 1,000 hours of tracking at maximum power points under continuous one-sun illumination and exhibit high stability under thermal and ambient conditions.

A Sub-20 nm Organic/Inorganic Hybrid Dielectric for Ultralow-Power Organic Thin-Film Transistor (OTFT) With Enhanced Operational Stability.

Organic/inorganic hybrid materials are utilized extensively as gate dielectric layers in organic thin-film transistors (OTFTs). However, inherently low dielectric constant of organic materials and lack of a reliable deposition process for organic layers hamper the broad application of hybrid dielectric materials. Here, a universal strategy to synthesize high-k hybrid dielectric materials by incorporating a high-k polymer layer on top of various inorganic layers generated by different fabrication methods, including AlOx and HfOx , is presented. Those hybrid dielectrics commonly exhibit high capacitance (>300 nF·cm-2 ) as well as excellent insulating properties. A vapor-phase deposition method is employed for precise control of the polymer film thickness. The ultralow-voltage (<3 V) OTFTs are demonstrated based on the hybrid dielectric layer with 100% yield and uniform electrical characteristics. Moreover, the exceptionally high stability of OTFTs for long-term operation (current change less than 5% even under 30 h of voltage stress at 2.0 MV·cm-1 ) is achieved. The hybrid dielectric is fully compatible with various substrates, which allows for the demonstration of intrinsically flexible OTFTs on the plastic substrate. It is believed that this approach for fabricating hybrid dielectrics by introducing the high-k organic material can be a promising strategy for future low-power, flexible electronics.

Mechanically and Ultraviolet Light Stable Ultrathin Organic Solar Cell via Semi-Embedding Silver Nanowires in a Hydrogen Bonds-Based Polyimide.

Ultrathin organic solar cells (OSCs) with both high power conversion efficiency (PCE) and operational stability are of great significance for the industrial applications but still challenging. Here, a polyimide (PI) substrate for high-performance and stable ultrathin OSCs, which is physically crosslinked via strong hydrogen bonds (denoted as HB-PI) to enhance the mechanical, thermal, solvent-resistant, and UV filtering properties (with a cut-off wavelength of 376 nm), is synthesized. An ultrathin flexible transparent composite electrode (FTCE, ≈7 µm) is fabricated via semi-embedding AgNWs in the HB-PI substrate. The FTCE possesses excellent optoelectronic property, smooth surface, and high mechanical stability simultaneously. Based on this FTCE, an ultrathin OSC is constructed with a PCE of 13.52% (average of 13.22%). Moreover, the ultrathin OSC shows outstanding mechanical stability (PCE decreased by less than 4% after 1000 bending cycles at a small bending radius of 0.5 mm) and superior UV light stability (no evident PCE degradation after irradiation under UV light for 10 h). This work will provide a new avenue for fabricating high-performance and stable ultrathin OSCs.

Characterization of proteins from the 3N5M family reveals an operationally stable amine transaminase.

Amine transaminases (ATA) convert ketones into optically active amines and are used to prepare active pharmaceutical ingredients and building blocks. Novel ATA can be identified in protein databases due to the extensive knowledge of sequence-function relationships. However, predicting thermo- and operational stability from the amino acid sequence is a persisting challenge and a vital step towards identifying efficient ATA biocatalysts for industrial applications. In this study, we performed a database mining and characterized selected putative enzymes of the ß-alanine:pyruvate transaminase cluster (3N5M) - a subfamily with so far only a few described members, whose tetrameric structure was suggested to positively affect operational stability. Four putative transaminases (TA-1: Bilophilia wadsworthia, TA-5: Halomonas elongata, TA-9: Burkholderia cepacia, and TA-10: Burkholderia multivorans) were obtained in a soluble form as tetramers in E. coli. During comparison of these tetrameric with known dimeric transaminases we found that indeed novel ATA with high operational stabilities can be identified in this protein subfamily, but we also found exceptions to the hypothesized correlation that a tetrameric assembly leads to increased stability. The discovered ATA from Burkholderia multivorans features a broad substrate specificity, including isopropylamine acceptance, is highly active (6 U/mg) in the conversion of 1-phenylethylamine with pyruvate and shows a thermostability of up to 70 °C under both, storage and operating conditions. In addition, 50% (v/v) of isopropanol or DMSO can be employed as co-solvents without a destabilizing effect on the enzyme during an incubation time of 16 h at 30 °C. KEY POINTS: • Database mining identified a thermostable amine transaminase in the ß-alanine:pyruvate transaminase subfamily. • The tetrameric transaminase tolerates 50% DMSO and isopropanol under operating conditions at 30 °C. • A tetrameric structure is not necessarily associated with a higher operational stability.

High-sodium maltobionate production by immobilized Zymomonas mobilis cells in polyurethane.

The purpose of this study was the production of maltobionic acid, in the form of sodium maltobionate, by Z. mobilis cells immobilized in polyurethane. The in situ immobilized system (0.125-0.35 mm) was composed of 7 g polyol, 3.5 g isocyanate, 0.02 g silicone, and 7 g Z. mobilis cell, at the concentration of 210 g/L. The bioconversion of maltose to sodium maltobionate was performed with different cell concentrations (7.0-9.0 gimobilized/Lreaction_medium), temperature (30.54-47.46 °C), pH (5.55-7.25), and substrate concentration (0.7-1.3 mol/L). The stability of the immobilized system was evaluated for 24 h bioconversion cycles and storage of 6 months. The maximum concentration of sodium maltobionate was 648.61 mmol/L in 34.34 h process (8.5 gdry_cell/Lreaction_medium) at 39 °C and pH 6.30. The immobilized system showed stability for 19 successive operational cycles of 24 h bioconversion and 6 months of storage, at 4 °C or 22 °C.

Judicious Choice of N-Heterocycles for the Realization of Sky-Blue- to Green-Emitting Carbazolylgold(III) C

A new class of sky-blue- to green-emitting carbazolylgold(III) C^C^N complexes containing pyrazole or benzimidazole moieties has been successfully designed and synthesized. Through the judicious choice of the N-heterocycles in the cyclometalating ligand and the tailor-made carbazole moieties, maximum photoluminescence quantum yields of 0.52 and 0.39 have been realized in the green- and sky-blue-emitting complexes, respectively. Solution-processed and vacuum-deposited organic light-emitting devices (OLEDs) based on the benzimidazole-containing complexes have been prepared. The sky-blue-emitting device shows an emission peaking at 484 nm with a narrow full-width at half-maximum of 57 nm (2244 cm-1 ), demonstrating the potential of this class of complexes in the application of OLEDs with high color purity. In addition, high maximum external quantum efficiencies of 12.3 % and a long operational half-lifetime of over 5300 h at 100 cd m-2 have been achieved in the vacuum-deposited green-emitting devices.

Design Strategy Towards Horizontally Oriented Luminescent Tetradentate-Ligand-Containing Gold(III) Systems.

Phosphorescent dopants are promising candidates for organic light-emitting diodes (OLEDs). Although it has been established that the out-coupling efficiency and overall performances of vacuum-deposited OLEDs can be significantly improved by a horizontal orientation of the dopants, no horizontally oriented gold(III) complexes have been reported to date. Herein, a novel class of tetradentate C^C^N^N ligand-containing gold(III) complexes with a preferential horizontal orientation successfully generated through a one-pot reaction is reported. These complexes demonstrate high photoluminescence quantum yields of 70 % and a high horizontal dipole ratio of 0.87 in solid-state thin films. Green-emitting OLEDs based on these complexes operate with a maximum external quantum efficiency of 20.6 % with an estimated out-coupling efficiency of around 30 %. A promising device stability has been achieved in the vacuum-deposited OLEDs, with operational half-lifetimes of around 37 500 h at 100 cd m-2 .

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.

Three in One: Temperature, Solvent and Catalytic Stability by Engineering the Cofactor-Binding Element of Amine Transaminase.

Amine transaminase (ATA) catalyse enantioselectively the direct amination of ketones, but insufficient stability during catalysis limits their industrial applicability. Recently, we revealed that ATAs suffer from substrate-induced inactivation mechanism involving dissociation of the enzyme-cofactor intermediate. Here, we report on engineering the cofactor-ring-binding element, which also shapes the active-site entrance. Only two point mutations in this motif improved temperature and catalytic stability in both biphasic media and organic solvent. Thermodynamic analysis revealed a higher melting point for the enzyme-cofactor intermediate. The high cofactor affinity eliminates the need for pyridoxal 5'-phosphate supply, thus making large-scale reactions more cost effective. This is the first report on stabilising a tetrameric ATA by mutating a single structural element. As this structural "hotspot" is a common feature of other transaminases it could serve as a general engineering target.

Chitosan hydrogel microspheres: an effective covalent matrix for crosslinking of soluble dextranase to increase stability and recycling efficiency.

Dextranase is a unique biocatalyst that has high specificity and stereo-selectivity towards a complex biopolymer known as dextran. Dextranase has wide industrial application, but most of the time harsh environmental conditions adversely affect the functionality and stability of the enzyme. To overcome this issue, a covalent cross-linking immobilization method was adapted in the current study utilizing a nontoxic and biocompatible matrix known as chitosan. Chitosan hydrogel microspheres were synthesized using chitosan which exhibited noteworthy physical and mechanical strength. After treatment with glutaraldehyde, chitosan hydrogel microspheres were used for immobilization of dextranase. The kinetic characteristics of immobilized dextranase were compared with that of the soluble enzyme. A shift in optimum pH and temperature from 7.0 to 7.5 and 50 to 60 °C was observed after immobilization, respectively. Recycling efficiency, thermal stability, and activation energy distinctly improved after immobilization, whereas anchoring of substrate at the active site of the soluble dextranase exhibited an increase in K m with no change in V max after crosslinking. This technique involves the reduction in the size of carrier molecules (microspheres) that provide a larger surface area for improved immobilization efficiency. Therefore, it is concluded that increased stability and reusability of this immobilized biocatalyst makes it a promising aspirant for the utilization at commercial level.