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The operational stability of the blue quantum dot light-emitting diode (QLED) has been one of the most important obstacles to initialize its industrialization. In this work, we demonstrate a machine learning assisted methodology to illustrate the operational stability of blue QLEDs by analyzing the measurements of over 200 samples (824 QLED devices) including current density-voltage-luminance (J-V-L), impedance spectra (IS), and operational lifetime (T95@1000 cd/m2). The methodology is able to predict the operational lifetime of the QLED with a Pearson correlation coefficient of 0.70 with a convolutional neural network (CNN) model. By applying a classification decision tree analysis of 26 extracted features of J-V-L and IS curves, we illustrate the key features in determining the operational stability. Furthermore, we simulated the device operation using an equivalent circuit model to discuss the device degradation related operational mechanisms.
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Quantum dots possess exceptional optoelectronic properties, such as narrow bandwidth, controllable wavelength, and compatibility with solution-based processing. However, for efficient and stable operation in electroluminescence mode, several issues require resolution. Particularly, as device dimensions decrease, a higher electric field may be applied through next-generation quantum dot light-emitting diode (QLED) devices, which could further degrade the device. In this study, we conduct a systematic analysis of the degradation phenomena of a QLED device induced by a high electric field, using scanning probe microscopy (SPM) and transmission electron microscopy (TEM). We apply a local high electric field to the surface of a QLED device using an atomic force microscopy (AFM) tip, and we investigate changes in morphology and work function in the Kelvin probe force microscopy mode. After the SPM experiments, we perform TEM measurements on the same degraded sample area affected by the electric field of the AFM tip. The results indicate that a QLED device could be mechanically degraded by a high electric field, and work function changes significantly in degraded areas. In addition, the TEM measurements reveal that In ions migrate from the indium tin oxide (ITO) bottom electrode to the top of the QLED device. The ITO bottom electrode also deforms significantly, which could induce work function variation. The systematic approach adopted in this study can provide a suitable methodology for investigating the degradation phenomena of various optoelectronic devices.
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Solution processes have promising advantages of low manufacturing cost and large-scale production, potentially applied for the fabrication of organic and quantum dot light-emitting diodes (OLEDs and QLEDs). To meet the expected lifespan of OLEDs/QLEDs in practical display and lighting applications, tandem architecture by connecting multiple light-emitting units (LEUs) through a feasible intermediate connection layer (ICL) is preferred. However, the combination of tandem architecture with solution processes is still limited by the choices of obtainable ICLs due to the unsettled challenges, such as orthogonal solubility, surface wettability, interfacial corrosion, and charge injection. This review focuses on the recent progresses of solution-processed tandem OLEDs and tandem QLEDs, covers the design and fabrication of various ICLs by solution process, and provides suggestions on the future challenges of corresponding materials and devices, which are anticipated to stimulate the exploitation of the emerging light technologies.
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This work reports the design, manufacturing and numerical simulation approach of a 6-pixel (4.5mm2/pixel) electroluminescent quantum dot light emitting device (QLED) based on CuInS2/ZnS quantum dots as an active layer. Following a conventional thin-film deposition multilayer approach, the QLED device was fabricated. In addition, the electrical I-V curve was measured for each pixel independently, observing how the fabrication process and layer thickness have an influence in the shape of the plot. This experimental device fabricated, enabled us to create a computational model for the QLED based on the Transfer Hamiltonian approach to calculate the current density J(mA/cm2), the band diagram of the system, and the accumulated charge distribution. Besides, it is worth highlighting that the simulator allows the possibility to study the influence of different parameters of the QLED structure like the junction capacitance between the distinct multilayer set. Specifically, we found that Anode-HIL interface capacitance has a greater influence in the I-V plot shape. That junction capacitance plays an important role in the current increase and the QLED turn-on value when a forward voltage is applied to the device. Thanks to the simulator, that influence could be put under control by the selection of the optimal thickness and transport layers during the experimental fabrication process. This work is remarkable since it achieves to fit simulation and experiment results in an accurate way for electroluminescent QLED devices; particularly the simulation of the device current, which is critical when designing the automotive electronics to control these new nanotechnology lighting devices in the future.
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This article offers a materials-chemistry perspective for colloidal quantum dots (QDs) in the field of display, including QD-enhanced liquid-crystal-display (QD-LCD) and QD-based light-emitting-diodes (QLEDs) display. The rapid successes of QDs for display in the past five years are not accidental but have a deep root in both maturity of their synthetic chemistry and their unique chemical, optical, and optoelectronic properties. This article intends to discuss the natural match of QD emitters for display and chemical means to eventually bring about their full potential.
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Colloidal quantum dots (QDs), as a class of 0D semiconductor materials, have generated widespread interest due to their adjustable band gap, exceptional color purity, near-unity quantum yield, and solution-processability. With decades of dedicated research, the potential applications of quantum dots have garnered significant recognition in both the academic and industrial communities. Furthermore, the related quantum dot light-emitting diodes (QLEDs) stand out as one of the most promising contenders for the next-generation display technologies. Although QD-based color conversion films are applied to improve the color gamut of existing display technologies, the broader application of QLED devices remains in its nascent stages, facing many challenges on the path to commercialization. This review encapsulates the historical discovery and subsequent research advancements in QD materials and their synthesis methods. Additionally, the working mechanisms and architectural design of QLED prototype devices are discussed. Furthermore, the review surveys the latest advancements of QLED devices within the display industry. The narrative concludes with an examination of the challenges and perspectives of QLED technology in the foreseeable future.
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The presence of the acidic and weak ionic conductor polystyrenesulfonate (PSS) in poly(3,4-ethylenedioxythiophene:PSS (PEDOT:PSS) leads to degradation and limits the charge transfer within quantum dot light-emitting diodes (QLEDs). Two-step solvent treatment resulted in a 40% reduction of PSS, which could be attributed to ethylene glycol (EG) attenuating the ionic interactions between PSS and PEDOT via interacting with PSS through hydrogen bonding. Methanol dissolved the predominant PSS and EG from the surface. The redshift of the peak representing the symmetrical vibration of CαâCß in the Raman spectrum confirmed the conformation of benzoid structure to quinoid structure after the surface treatment. This conformation was attributed to the extension of the conjugation length and the reduction of the energy barrier within the PEDOT chain. This resulted in the improved conductivity and charge hopping of the PEDOT:PSS, which was also proven using density functional theory (DFT) calculations. Reducing the insulating and acidic PSS improved the electroluminescence performance and extended the operational lifetime of the QLEDs. The tris(dimethylamino)phosphine-based InP QLEDs exhibited an external quantum efficiency (EQE) of 6.4%, that value is comparable to those of tris(trimethylsilyl)phosphine-based QLEDs, and operational lifetime (T50) of 125.6 h.
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Positive aging has been reported to be effective for enhancing electroluminescence characteristics of quantum dot (QD) based optoelectrical devices. This study investigated the intricate mechanisms underlying the positive aging effect in quantum-dot light-emitting diodes (QLEDs) influenced by encapsulation with ultraviolet-curable resin. A 120-h analysis assessed the impact of the resin on the electron transport layer and emission layer, utilizing a strategically positioned perfluorinated ionomer (PFI) interlayer. The PFI layer effectively delayed the Al2O3 formation at the zinc magnesium oxide (ZMO)/Al interface and further reduced the interactions within the QD/ZMO interface, thereby curtailing exciton quenching at the interfaces. The time-sequential effect of positive aging demonstrated that resin encapsulation effectively passivates the ZMO surfaces after 12 h. The positive aging facilitated the reaction between aluminum and oxygen from ZMO, contributing to Al2O3 formation within 48 h of aging. Furthermore, positive aging passivated the defect states of the QD surface and the QD/ZMO interface, reducing exciton quenching at the QD or QD/ZMO interface. The enhanced electron injection and reduced exciton quenching resulted in aged InP QLEDs, exhibiting an external quantum efficiency of 12.04%. This is a significant increase from the 3.16% observed in the control device. Finally, a sequential mechanism of positive aging in InP QLEDs was devised, providing new insights into the time-related operation of aging agents. This study elucidates an advanced time-resolved mechanism of positive aging, thereby offering valuable insights into the intricate dynamics of excitons within the domain of QLED physics.
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In this work, an efficient and robust hole transport layer (HTL) based on blended poly((9,9-dioctylfluorenyl-2,7-diyl)-alt-(9-(2-ethylhexyl)-carbazole-3,6-diyl)) (PF8Cz) and crosslinkable 3,3'-(9,9-dimethyl-9H-fluorene-2,7-diyl)bis(9-(4-vinylphenyl)-9H-carbazole) (FLCZ-V) is introduced for high-performance and stable blue quantum dot-based light-emitting diodes (QLEDs), wherein FLCZ-V can in situ-crosslink to a continuous network polymer after thermal treatment and the linear polymer PF8CZ becomes intertwined and imprisoned. As a result, the blended HTL shows a high hole mobility (1.27 × 10-4 cm2 V-1 s-1) and gradient HOMO levels (-5.4 eV of PF8CZ and -5.7 eV of FLCZ-V) that can facilitate hole injecting so as to ameliorate the charge balance and, at the same time, achieve better electron-blocking capability that can effectively attenuate HTL decomposition. Meanwhile, the crosslinked blended HTL showed excellent solvent resistance and a high surface energy of 40.34 mN/m, which is favorable to enhance wettability for the deposition of a follow-up layer and attain better interfacial contact. Based on the blended HTL, blue QLEDs were fabricated by both spin-coating and inkjet printing. For the spin-coated blue QLED, a remarkable enhancement of external quantum efficiency (EQE) of 15.5% was achieved. Also, the EQE of the inkjet-printed blue QLED reached 9.2%, which is thus far the best result for the inkjet-printed blue QLED.
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Metal halide perovskite nanocrystals (PeNCs) have outstanding luminescent properties that are suitable for displays that have high color purity and high absorption coefficient; so they are evaluated for application as light emitters for organic light-emitting diodes, light-converters for downconversion displays, and future near-eye augmented reality/virtual reality displays. However, PeNCs are chemically vulnerable to heat, light, and moisture, and these weaknesses must be overcome before devices that use PeNCs can be commercialized. This review examines strategies to overcome the low stability of PeNCs and thereby permit the fabrication of stable downconversion films, and summarizes downconversion-type display applications and future prospects. First, methods to increase the chemical stability of PeNCs are examined. Second, methods to encapsulate PeNC downconversion films to increase their lifetime are reviewed. Third, methods to increase the long-term compatibility of resin with PeNCs, and finally, how to secure stability using fillers added to the resin are summarized. Fourth, the method to manufacture downconversion films and the procedure to evaluate their reliability for commercialization is then described. Finally, the prospects of a downconversion system that exploits the properties of PeNCs and can be employed to fabricate fine pixels for high-resolution displays and for near-eye augmented reality/virtual reality devices are explored.
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Quantum dot light-emitting diodes (QLEDs) have been identified as a next-generation display technology owing to their low-cost manufacturing, wide color gamut, and electrically driven self-emission properties. However, the efficiency and stability of blue QLEDs still pose a significant challenge, limiting their production and potential application. This review aims to analyse the factors leading to the failure of blue QLEDs and presents a roadmap to accelerate their development based on the progress made in the synthesis of II-VI (CdSe, ZnSe) quantum dots (QDs), III-V (InP) QDs, carbon dots, and perovskite QDs. The proposed analysis will include discussions on material synthesis, core-shell structures, ligand interactions, and device fabrication, providing a comprehensive overview of these materials and their development.
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Polymeric hole-transport materials (HTMs) have been widely used in quantum-dot light-emitting diodes (QLEDs). However, their solution processability normally causes interlayer erosion and unstable film state, leading to undesired device performance. Besides, the imbalance of hole and electron transport in QLEDs also damages the device interfaces. In this study, we designed a bis-diazo compound, X1, as carbene cross-linker for polymeric HTM. Irradiated by ultraviolet and heating, a poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt(4,4'-(N-(4-butylphenyl))] (TFB)/X1 blend can achieve fast "electronically clean" cross-linking with â¼100% solvent resistance. The cross-linking reduced the stacking behaviors of TFB and thus led to a lower hole-transport mobility, whereas it was a good match of electron mobility. The carbene-mediated TFB cross-linking also downshifted the HOMO level from -5.3 to -5.5 eV, delivering a smaller hole-transport energy barrier. Benefiting from these, the cross-linked QLED showed enhanced device performances over the pristine device, with EQE, power efficiency, and current efficiency being elevated by nearly 20, 15, and 83%, respectively. To the best of our knowledge, this is the first report about a bis-diazo compound based carbene cross-linker built into a polymeric HTM for a QLED with enhanced device performance.
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This report outlines a proposed method of packaging wide-angle (WA) mini-light-emitting diode (mini-LED) devices without optical lenses to create a highly efficient, ultrathin, flexible planar backlight for portable quantum dot light-emitting diode (QLED) displays. Since the luminous intensity curve for mini-LEDs generally recommends a beam angle of 120°, numerous LEDs are necessary to achieve a uniform surface light source for a QLED backlight. The light-guide layer and diffusion layer were packaged together on a chip surface to create WA mini-LEDs with a viewing angle of 180°. These chips were then combined with a quantum dot (QD) film and an optical film to create a high-efficiency, ultrathin, flexible planar light source with excellent color purity that can be used as a QLED display backlight. A 6 in (14.4 cm) light source was used as an experimental sample. When 1.44 W was supplied to the sample, the 3200-piece WA mini-LED with a flexible planar QLED display had a beam angle of 180° on the luminous intensity curve, a planar backlight thickness of 0.98 mm, a luminance of 10,322 nits, and a luminance uniformity of 92%.
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Light-emitting diodes based on colloidal quantum dots (QLEDs) show a good prospect in commercial application due to their narrow spectral linewidths, wide color range, excellent luminance efficiency, and long operating lifetime. However, the toxicity of heavy-metal elements, such as Cd-based QLEDs or Pb-based perovskite QLEDs, with excellent performance, will inevitably pose a serious threat to people's health and the environment. Among heavy-metal-free materials, InP quantum dots (QDs) have been paid special attention, because of their wide emission, which can, in principle, be tuned throughout the whole visible and near-infrared range by changing their size, and InP QDs are generally regarded as one of the most promising materials for heavy-metal-free QLEDs for the next generation displays and solid-state lighting. In this review, the great progress of QLEDs, based on the fundamental structure and photophysical properties of InP QDs, is illustrated systematically. In addition, the remarkable achievements of QLEDs, based on their modification of materials, such as ligands exchange of InP QDs, and the optimization of the charge transport layer, are summarized. Finally, an outlook is shown about the challenge faced by QLED, as well as possible pathway to enhancing the device performance. This review provides an overview of the recent developments of InP QLED applications and outlines the challenges for achieving the high-performance devices.
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Fabrication of high-performance, flexible quantum-dot light-emitting diodes (QLEDs) requires the reliable manufacture of a flexible transparent electrode to replace the conventional brittle indium tin oxide (ITO) transparent electrode, along with flexible substrate planarization. We deposited a transparent oxide/metal/oxide (OMO) electrode on a polymer planarization layer and co-optimized both layers. The visible transmittance of the OMO electrode on a polyethylene terephthalate substrate increased markedly. Good electron supply and injection into an electron-transporting layer were achieved using WOX/Ag/ WOX and MoOx/Ag/MoOX OMO electrodes. High-performance flexible QLEDs were fabricated from these electrodes; a QLED with a MoOX/Ag/ MoOX cathode and an SU-8 planarization layer had a current efficiency of 30.3 cd/A and luminance more than 7 × 104 cd/m2. The current efficiency was significantly higher than that of a rigid QLED with an ITO cathode and was higher than current efficiency values obtained from previously reported QLEDs that utilized the same quantum-dot and electron-transporting layer materials as our study.
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With many advantages including superior color saturation and efficiency, quantum dot light-emitting diodes (QLEDs) are considered a promising candidate for the next-generation displays. Emission uniformity over the entire device area is a critical factor to the overall performance and reliability of QLEDs. In this work, we performed a thorough study on the origin of dark spots commonly observed in operating QLEDs and developed a strategy to eliminate these defects. Using advanced cross section fabrication and imaging techniques, we discovered the occurrence of voids in the organic hole transport layer and directly correlated them to the observed emission nonuniformity. Further investigations revealed that these voids are thermal damages induced during the subsequent thermal deposition of other functional layers and can act as leakage paths in the device. By inserting a thermo-tolerant 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HATCN) interlayer with an optimized thickness, the thermally induced dark spots can be completely suppressed, leading to a current efficiency increase by 18%. We further demonstrated that such a thermal passivation strategy can work universally for various types of organic layers with low thermal stability. Our findings here provide important guidance in enhancing the performances and reliability of QLEDs and also other sandwich-structured devices via the passivation of heat-sensitive layers.
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A blend of perovskite quantum dots (QDs) and a hole transport layer (HTL) is a feasible candidate to solve the long-standing issues in light-emitting diodes (LEDs) such as charge injection, energy state matching, and defect passivation. However, QD:HTL blend structures for QD-based LEDs suffer from fast charge and energy transfers due to an inhomogeneous distribution of QDs and the HTL matrix. Here we report new cross-linkable spacer ligands between QDs and TFB that result in a highly emissive QD:TFB-blended LED device. We synthesize three representative spacer ligands to control the charge and energy transfers between QDs and the HTL. The first spacer ligand is used for controlling the molecular distance between QDs and TFB, and the second spacer ligand is designed to investigate how molecular interaction between QDs and the spacer ligand affects the optical property of the QD:TFB blend. Subsequently, the best spacer ligand, a 10-((2-benzoylbenzoyl)oxy)decanoic acid, is designed to anchor TFB (via a benzophenone group) and simultaneously bond to QDs (with a carboxylic acid functional group). The carboxylic acid group strongly interacts with QDs, dramatically improving the cross-linking rate between QDs and TFB. Due to the direct interaction between QDs and TFB, hole carriers can be effectively injected to perovskite QDs through the conductive backbone of TFB, resulting in the highest luminance values of 10917 cd/m2 at 7.4 V due to carrier injection balance. This is at least 10 times better LED performance compared with a pristine QD device.
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An environment-friendly inverted indium phosphide red quantum dot light-emitting diode (InP QLED) was fabricated using Mg-doped zinc oxide (ZnMgO) as the electron transport layer (ETL). The effects of ZnMgO ETL on the performance of InP QLED were investigated. X-ray diffraction (XRD) analysis indicated that ZnMgO film has an amorphous structure, which is similar to zinc oxide (ZnO) film. Comparison of morphology between ZnO film and ZnMgO film demonstrated that Mg-doped ZnO film remains a high-quality surface (root mean square roughness: 0.86 nm) as smooth as ZnO film. The optical band gap and ultraviolet photoelectron spectroscopy (UPS) analysis revealed that the conduction band of ZnO shifts to a more matched position with InP quantum dot after Mg-doping, resulting in the decrease in turn-on voltage from 2.51 to 2.32 V. In addition, the ratio of irradiation recombination of QLED increases from 7% to 25% using ZnMgO ETL, which can be attributed to reduction in trap state by introducing Mg ions into ZnO lattices. As a result, ZnMgO is a promising material to enhance the performance of inverted InP QLED. This work suggests that ZnMgO has the potential to improve the performance of QLED, which consists of the ITO/ETL/InP QDs/TCTA/MoO3/Al, and Mg-doping strategy is an efficient route to directionally regulate ZnO conduction bands.
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In this report, blue fluorescent zinc selenide quantum dots (ZnSe QDs) were synthesized using 3-mercaptopropionic acid through a direct aqueous route at a lower temperature of 70 °C. The photoluminescence (PL) characteristics of ZnSe QDs have been employed to recognize nitroaromatic compounds, i.e., traces of 2,4,6-TNP (picric acid) in water. The sensing of nitroaromatic compounds was performed via fluorescence techniques. The PL band of ZnSe QDs observed at 490 nm is selectively quenched with an increasing concentration of picric acid in DI water and river water. For the proposed sensing probe, the Stern-Volmer (S-V) plot shows linearity over the range of 2.0 µM-0.25 mM with the detection limit of 12.4 × 10-6 M without any interference effect of other nitroaromatic compounds. The plausible mechanism of PL quenching is considered as the inner filter effect, based on absorption, PL and PL lifetimes.
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It was demonstrated through a comparison between the spin-coated and inkjet-printed quantum-dot light-emitting diodes' (QLED) performance analysis outcomes that the annealing temperature of a zinc oxide nanoparticle (ZnO NP) electron transport layer (ETL) optimized for intense pulsed light (IPL) via a post-treatment differs depending on the film-formation method used. For a naturally dried ZnO NP ETL formulated without annealing, different film morphologies were observed according to the film-formation method of spin coating and inkjet printing, and the surface-roughness root mean square (RMS) value was increased in an IPL post-treatment due to unevaporated residual solvent. Based on this phenomenon, we classified and analyzed different film profiles according to the deposition method, the presence or absence of annealing, and the annealing temperature.