Red Quantum Dot Light-emitting Diodes Research Articles

Inverted Red Quantum Dot Light-Emitting Diodes with ZnO Nanoparticles Synthesized Using Zinc Acetate Dihydrate and Potassium Hydroxide in Open and Closed Systems

We developed inverted red quantum dot light-emitting diodes (QLEDs) with ZnO nanoparticles synthesized in open and closed systems. Wurtzite-structured ZnO nanoparticles were synthesized using potassium hydroxide and zinc acetate dihydrate at various temperatures in the open and closed systems. The particle size increases with increasing synthesis temperature. The ZnO nanoparticles synthesized at 50, 60, and 70 °C in the closed system have an average particle size of 3.2, 4.0, and 5.4 nm, respectively. The particle size is larger in the open system compared to the closed system as the methanol solvent evaporates during the synthesis process. The surface defect-induced emission in ZnO nanoparticles shifts to a longer wavelength and the emission intensity decreases as the synthesis temperature increases. The inverted red QLEDs were fabricated with a synthesized ZnO nanoparticle electron transport layer. The driving voltage of the inverted QLEDs decreases as the synthesis temperature increases. The current efficiency is higher in the inverted red QLEDs with the ZnO nanoparticles synthesized in the closed system compared to the devices with the nanoparticles synthesized in the open system. The device with the ZnO nanoparticles synthesized at 60 °C in the closed system exhibits the maximum current efficiency of 5.8 cd/A.

High Efficiency Ultra-Narrow Emission Quantum Dot Light-Emitting Diodes Enabled by Microcavity.

A wide-color-gamut display enableby a narrow emission linewidth facilitates a visually immersive experience akin to the real world. Quantum dot light-emitting diodes (QLEDs) with excellent color purity and high efficiency hold great promise as future candidates for high-definition displays. However, most devices typically exhibit emission linewidths exceeding 20nm, and lack a universal strategy for further enhancing the color purity. In this study, a planar microcavity structure for realizing ultra-narrow emissions is developed by incorporating a distributed Bragg reflector into normal electroluminescent devices. By leveraging the strong optical resonance effect derived from this microcavity structure, red QLEDs are successfully fabricated with an extraordinary full width at half maximum of 11nm in the normal direction, beyond the BT.2020 color coordinates. The fabricated red-microcavity QLEDs exhibit a considerable enhancement in the external quantum efficiency, which increases from 28.2% to 35.6%, together with an extended operating lifetime. The strategy adopted herein will serve as an effective reference for achieving ultra-narrow emission and high-efficiency QLEDs.

One-Pot Synthesis of Color-Tunable Narrow-Bandwidth Ag-In-Ga-Zn-S Semiconductor Nanocrystals for Quantum-Dot Light-Emitting Diodes.

I-III-VI type semiconductor nanocrystals (NCs) have attracted considerable attention due to their environmental friendly nature and large-scale tunable emission. Herein, we report the successful synthesis of full-spectrum (470 to 614 nm) Ag-In-Ga-Zn-S (AIGZS) NCs by precisely regulating the In/Ga ratios using a facile one-pot method. Intriguingly, the photoluminescence (PL) peak width exhibits a continuous narrowing trend with extended reaction time, ultimately reaching a full width at half-maximum (fwhm) of 34 nm for green AIGZS NCs. Furthermore, the exciton relaxation dynamics of AIGZS NCs were systematically investigated using time-resolved photoluminescence and femtosecond transient absorption spectroscopy. Remarkably, we successfully fabricated blue, green, and red quantum-dot light-emitting diodes (QLEDs), forecasting the potential of AIGZS NCs with high color purity for applications in full-spectrum QLEDs.

Flexible Substrate-Compatible and Efficiency-Improved Quantum-Dot Light-Emitting Diodes with Reduced Annealing Temperature of NiOx Hole-Injecting Layer

The growing demand for wearable and attachable displays has sparked significant interest in flexible quantum-dot light-emitting diodes (QLEDs). However, the challenges of fabricating and operating QLEDs on flexible substrates persist due to the lack of stable and low-temperature processable charge-injection/-transporting layers with aligned energy levels. In this study, we utilized NiOx nanoparticles that are compatible with flexible substrates as a hole-injection layer (HIL). To enhance the work function of the NiOx HIL, we introduced a self-assembled dipole modifier called 4-(trifluoromethyl)benzoic acid (4–CF3–BA) onto the surface of the NiOx nanoparticles. The incorporation of the dipole molecules through adsorption treatment has significantly changed the wettability and electronic characteristics of NiOx nanoparticles, resulting in the formation of NiO(OH) at the interface and a shift in vacuum level. The alteration of surface electronic states of the NiOx nanoparticles not only improves the carrier balance by reducing the hole injection barrier but also prevents exciton quenching by passivating defects in the film. Consequently, the NiOx-based red QLEDs with interfacial modification demonstrate a maximum current efficiency of 16.1 cd/A and a peak external quantum efficiency of 10.3%. This represents a nearly twofold efficiency enhancement compared to control devices. The mild fabrication requirements and low annealing temperatures suggest potential applications of dipole molecule-modified NiOx nanoparticles in flexible optoelectronic devices.

Nondestructive Direct Patterning of Both Hole Transport and Emissive Layers for Pixelated Quantum-Dot Light-Emitting Diodes.

Considering the increasing demand for high-resolution light-emitting diodes (LEDs), it is important that direct fine patterning technologies for LEDs be developed, especially for quantum-dot LEDs (QLEDs). Traditionally, the patterning of QLEDs relies on resin-based photolithography techniques, requiring multiple steps and causing performance deterioration. Nondestructive direct patterning may provide an easy and stepwise method to achieve fine-pixelated units in QLEDs. In this study, two isomeric tridentate cross-linkers (X8/X9) are presented and can be blended into the hole transport layer (HTL) and the emissive layer (EML) of QLEDs. Because of their photosensitivity, the in situ cross-linking process can be efficiently triggered by ultraviolet irradiation, affording high solvent resistance and nondestructive direct patterning of the layers. Red QLEDs using the cross-linked HTL demonstrate an impressive external quantum efficiency of up to 22.45%. Through lithographic patterning enabled by X9, line patterns of HTL and EML films exhibit widths as narrow as 2 and 4 μm, respectively. Leveraging the patterned HTL and EML, we show the successful fabrication of pixelated QLED devices with an area size of 3 × 3 mm2, alongside the successful production of dual-color pixelated QLED devices. These findings showcase the promising potential of direct patterning facilitated by engineered cross-linkers for the cost-effective fabrication of pixelated QLED displays.

Improving the Stability of Ink-Jet Printed Red QLEDs By Optimizing The Device Fabrication Process

Improving the Stability of Ink-Jet Printed Red QLEDs By Optimizing The Device Fabrication Process

Solution‐Processed Tandem Quantum‐Dot Light‐Emitting Diodes with Dual Charge Generation Interfaces: Achieving Over Threefold Efficiency Enhancement

AbstractDespite the commercialization of thermally evaporated tandem organic light‐emitting diodes (OLEDs), challenges remain for solution‐processed tandem quantum‐dot light‐emitting diodes (QLEDs), including low efficiency and solvent‐induced damage to functional layers. Therefore, there is an urgent need for the optimization of the interconnecting layer (ICL) design in order to fabricate high‐performance solution‐processed tandem QLEDs. Here, by introducing a phosphomolybdic acid (PMA) layer between poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) and poly(9‐vinylcarbazole) (PVK), an novel ICL, PVK/PMA/PEDOT:PSS/ZnO is proposed, with dual charge generation interfaces (CGIs): PVK/PMA and PEDOT:PSS/ZnO. The PMA interlayer serves not only smoothing the morphology of PEDOT:PSS to improve charge transport, but also forming a PVK/PMA CGI to enhance charge generation. Based on the excellent electrical and optical properties of the dual‐CGI ICL, the solution‐processed inverted tandem red QLEDs achieve an increased external quantum efficiency (EQE) of over three times compared to single‐junction devices. This provides a novel approach for the high‐efficiency solution‐processed tandem QLEDs, paving the way for the practical application of QLEDs.

Record high external quantum efficiency of 20% achieved in fully solution-processed quantum dot light-emitting diodes based on hole-conductive metal oxides

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) has been widely used as a hole injection material in quantum dot (QD) light-emitting diodes (QLEDs). However, it degrades the organic materials and electrodes in QLEDs due to its strong hydroscopicity and acidity. Although hole-conductive metal oxides have a great potential to solve this disadvantage, it is still a challenge to achieve efficient and stable QLEDs by using these solution-processed metal oxides. Herein, the state-of-the-art QLEDs fabricated by using hole-conductive MoOx QDs are achieved. The α-phase MoOx QDs exhibit a monodispersed size distribution with clear and regular crystal lattices, corresponding to high-quality nanocrystals. Meanwhile, the MoOx film owns an excellent transmittance, suitable valence band, good morphology and impressive hole-conductivity, demonstrating that the MoOx film could be used as a hole injection layer in QLEDs. Moreover, the rigid and flexible red QLEDs made by MoOx exhibit peak external quantum efficiencies of over 20%, representing a new record for the hole-conductive metal oxide based QLEDs. Most importantly, the MoOx QDs afford their QLEDs with a longer T95 lifetime than these devices made by PEDOT:PSS. As a result, we believe that the MoOx QDs could be used as efficient and stable hole injection materials used in QLEDs.

Phenethylammonium bromide interlayer for high-performance red quantum-dot light emitting diodes.

Interfacial modification is vital to boost the performance of colloidal quantum-dot light-emitting diodes (QLEDs). We introduce phenethylammonium bromide (PEABr) as an interlayer to reduce the trap states and exciton quenching at the interface between the emitting layer (EML) with CdSe/ZnS quantum-dots and the electron transport layer (ETL) with ZnMgO. The presence of PEABr separates the EML and the ETL and thus passivates the surface traps of ZnMgO. Moreover, the interfacial modification also alleviates electron injection, leading to more improved carrier injection balance. Consequently, the external quantum efficiency of the PEABr-based red QLED reached 27.6%, which outperformed those of the previously reported devices. Our results indicate that the halide ion salts are promising to balance charge carrier injection and reduce exciton quenching in the QLEDs.

Anomalous efficiency elevation of quantum-dot light-emitting diodes induced by operational degradation

Quantum-dot light-emitting diodes promise a new generation of high-performance and solution-processed electroluminescent light sources. Understanding the operational degradation mechanisms of quantum-dot light-emitting diodes is crucial for their practical applications. Here, we show that quantum-dot light-emitting diodes may exhibit an anomalous degradation pattern characterized by a continuous increase in electroluminescent efficiency upon electrical stressing, which deviates from the typical decrease in electroluminescent efficiency observed in other light-emitting diodes. Various in-situ/operando characterizations were performed to investigate the evolutions of charge dynamics during the efficiency elevation, and the alterations in electric potential landscapes in the active devices. Furthermore, we carried out selective peel-off-and-rebuild experiments and depth-profiling analyses to pinpoint the critical degradation site and reveal the underlying microscopic mechanism. The results indicate that the operation-induced efficiency increase results from the degradation of electron-injection capability at the electron-transport layer/cathode interface, which in turn leads to gradually improved charge balance. Our work provides new insights into the degradation of red quantum-dot light-emitting diodes and has far-reaching implications for the design of charge-injection interfaces in solution-processed light-emitting diodes.

Dipole-tunable interfacial engineering strategy for high-performance all-inorganic red quantum-dot light-emitting diodes

All-inorganic quantum dot (QD) light-emitting diodes (AI-QLEDs) with excellent stability received enormous interest in the past few years. Nevertheless, the vast energy offset and the high trap density at the NiOX/QDs interface limit hole injection leading to fluorescence quenching and hampering the performance. Here, we present self-assembled monolayers (SAMs) with phosphonic acid (PA) anchoring groups modifying NiOX hole transport layer (HTL) to tune energy level and passivate trap states. This strategy facilitates hole injection owning to the well-aligned energy level by interface dipole, downshifting the vacuum level, reducing the hole injection barrier from 0.94 eV to 0.28 eV. Meanwhile, it mitigates the interfacial recombination by passivating surface hydroxyl group (-OH) and oxygen vacancy (VO) traps in NiOX. The electron leakage from QDs toward NiOX HTL is significantly suppressed. The all-inorganic R-QLEDs exhibit one of the highest maximum luminance, external quantum efficiency and operational lifetime of 88980 cd m−2, 10.3 % and 335045 h (T50 @100 cd m−2), respectively. The as-proposed interface engineering provides an effective design principle for high-performance AI-QLEDs for future outdoor and optical projection-type display applications.

Ultralow Roll-Off Quantum Dot Light-Emitting Diodes Using Engineered Carrier Injection Layer.

Quantum dot (QD) light-emitting diodes (QLEDs) have attracted extensive attention due to their high color purity, solution-processability, and high brightness. Due to extensive efforts, the external quantum efficiency (EQE) of QLEDs has approached the theoretical limit. However, because of the efficiency roll-off, the high EQE can only be achieved at relatively low luminance, hindering their application in high-brightness devices such as near-to-eye displays and lighting applications. Here, this article reports an ultralow roll-off QLED that is achieved by simultaneously blocking electron leakage and enhancing the hole injection, thereby shifting the recombination zone back to the emitting QDs layer. These devices maintain EQE over 20.6% up to 1000 mA cm-2 current density, dropping only by ≈5% from the peak EQE of 21.6%, which is the highest value ever reported for the bottom-emitting red QLEDs. Furthermore, the maximum luminance of the optimal device reaches 320 000 cd m-2 , 2.7 times higher than the control device (Lmax : 128 000 cd m-2 ). A passive matrix (PM) QLED display panel with high brightness based on the optimized device structure is also demonstrated. The proposed approach advances the potential of QLEDs to operate efficiently in high-brightness scenarios.

Phosphorescent Dye Sensitized Quantum-Dot Light-Emitting Diodes with 37% External Quantum Efficiency.

Exciton harvesting is of paramount importance for quantum-dot light-emitting diodes (QLEDs). Direct exciton harvesting by quantum dots (QDs) emitting layer suffers from poor hole injection due to the low conduction bands and valence bands of QDs, leading to unbalanced electron-hole injection and recombination. To address this issue, here we report an exciton sensitizing approach, where excitons form on a phosphorescent dye doped layer which then transfer their energies to adjacent QDs layer for photon emission. Due to the very efficient exciton formation and energy transfer processes, higher device performance could be achieved. To demonstrate the above strategy, red QLEDs with a phosphorescent dye Iridium (III) bis (2 - methyldibenzo - [f, h] quinoxaline) (acetylacetonate), Ir(MDQ)2 (acac) doped hole transporting layer were fabricated and studied. At a doping concentration of 10wt.%, the best device achieves record high current efficiency, power efficiency and external quantum efficiency of 37.3cd A-1 , 41.0lm W-1 and 37.0%, respectively. Simultaneously, the efficiency roll-off characteristic was greatly improved that 35.0% EQE can be well remained at high luminance level of 450 000cd m-2 . Moreover, the devices also exhibit good stability and reproducibility. This article is protected by copyright. All rights reserved.

Enhancing performance of inverted quantum-dot light-emitting diodes based on a solution-processed hole transport layer via ligand treatment

The performance of inverted quantum-dot light-emitting diodes (QLEDs) based on solution-processed hole transport layers (HTLs) has been limited by the solvent-induced damage to the quantum dot (QD) layer during the spin-coating of the HTL. The lack of compatibility between the HTL's solvent and the QD layer results in an uneven surface, which negatively impacts the overall device performance. In this work, we develop a novel method to solve this problem by modifying the QD film with 1,8-diaminooctane to improve the resistance of the QD layer for the HTL’s solvent. The uniform QD layer leads the inverted red QLED device to achieve a low turn-on voltage of 1.8 V, a high maximum luminance of 105 500 cd/m2, and a remarkable maximum external quantum efficiency of 13.34%. This approach releases the considerable potential of HTL materials selection and offers a promising avenue for the development of high-performance inverted QLEDs.

Single, Double and ETL-Sandwiched PVPy Interlayer Effect on Charge Injection Balance and Performance of Inverted Quantum Dot Light-Emitting Diodes.

A desire to achieve optimal electron transport from the electron transport layer (ETL) towards the emissive layer (EML) is an important research factor for the realization of high performance quantum dot light-emitting diodes (QD-LEDs). In this paper, we study the effect of a single, double, and electron transport layer sandwiched Poly(4-vinylpyridine) (PVPy here on) on the charge injection balance and on the overall device performance of InP-based red quantum dot light emitting diodes (red QD-LEDs). The results showed general improvement of device characteristic performance metrics such as operational life with incorporation of a PVPy interlayer. The best performance was observed at a lower concentration of PVPy (@ 0.1 mg/mL) in interlayer with continual worsening in performance as PVPy concentration in the interlayer increased in other fabricated devices. The AFM images obtained for the different materials reported improved surface morphology and overall improved surface properties, but decreased overall device performance as PVPy concentration in interlayer was increased. Furthermore, we fabricated two special devices: in the first special device, a single 0.1 mg/mL PVPy sandwiched between two ZnO ETL layers, and in the second special device, two 0.1 mg/mL PVPy interlayers were inter-sandwiched between two ZnO ETL layers. Particular emphasis was placed on monitoring the maximum obtained EQE and the maximum obtained luminance of all the devices. The first special device showed better all-round improved performance than the second special device compared to the reference device (without PVPy) and the device with a single 0.1 mg/mL PVPy interlayer stacked between ZnO ETL and the emissive layer.

Highly Efficient Top‐Emitting Quantum‐Dot Light‐Emitting Diodes with Record‐Breaking External Quantum Efficiency of over 44.5%

AbstractTop‐emitting (TE) quantum‐dot light‐emitting diodes (QLEDs) can exhibit higher light outcoupling efficiency (OCE) compared to bottom‐emitting (BE) QLEDs due to the eliminated substrate mode and enhanced microcavity effect. In this study, TE QLEDs with an OCE of over 45% are realized by simultaneously optimizing the thicknesses of both indium‐zinc‐oxide (IZO) phase tuning layers and IZO top transparent electrodes. To reduce the resistance, the IZO top electrodes are equipped with an auxiliary metal electrode. Consequently, the red QLEDs demonstrate a high external quantum efficiency (EQE) of 38.2%. Furthermore, by applying a scattering layer on the IZO top electrode, the red QLEDs demonstrate record‐breaking efficiencies of EQE 44.5%, power efficiency 92.2 lm W−1, and current efficiency 93.7 cd A−1. The proposed device architecture and optimization strategy contribute to a new design scheme for the preparation of highly efficient QLEDs for displays and lighting applications.

ZnO/silica quasi core/shell nanoparticles as electron transport materials for high-performance quantum-dot light-emitting diodes

Quantum dot light-emitting diodes (QLEDs) are considered as the ideal candidate for next-generation displays, solid-state lighting, and optical communication applications. Although the efficiency of QLEDs has been significantly improved to the level comparable to that of organic light-emitting diodes in recent years, simultaneously achieving high efficiency and high brightness still remains challenging for QLEDs. In this work, we report a facile and effective electron-transport-layer interface control strategy of incorporating 3-aminopropyl triethoxysilane (APTES) into a ZnO nanocrystal-solution to enhance charge injection balance and suppress interfacial exciton quenching via in-situ formation of ZnO/organic silica (hereinafter referred to as ZnO/SiO2) quasi core/shell nanoparticles in the solution, enabling red QLEDs to exhibit a maximum luminance intensity of 261,700 cd m−2, a peak external quantum efficiency (EQE) of 19.0%, and low efficiency roll-off at high luminance (an EQE up to 16.8% remained at a brightness of 200, 000 cd m−2). Our results demonstrate that substituting quasi core/shell-structured ZnO/SiO2 nanoparticles for traditional ZnO nanocrystals as electron transport materials is a simple and effective means of fabricating QLEDs with both high efficiency and high luminance, which is expected to facilitate the development of QLED technology toward practical applications in lighting, displays and optical communication.

Hole-transport-layer-free CdSe/ZnS core/shell red quantum-dot light-emitting diodes sensitized by TADF polymers

Energy transfer and charge transport in the thermally activated delayed fluorescence polymer doped quantum-dots were investigated. A high EQE of 18.1% was demonstrated for the first time in the quantum-dot red LEDs without any hole transport layers.

Investigation of quantum dots light emitting diodes with different transition metal oxide as charge injection layers

In this paper, various transition metal oxides serve as charge injection layers being prepared by solution process for the fabrication of quantum dot light emitting diodes (QLEDs) is demonstrated. Magnesium doped zinc oxide (MgZnO) nanoparticles is used as electron injection and transport layer, copper oxide (CuO x ), nickel oxide (NiO x ), cobalt oxide (CoO x ) and molybdenum oxide (MoO x ) are used as hole injection layer (HIL) for the comparison with Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate), PEDOT:PSS. The fabricated red QLEDs with PEDOT:PSS possess highest maximum luminance of 88,713 cd/m 2 and current efficiency of 4.96 cd/A, whereas QLEDs with MoO x and NiO x HILs demonstrate lower turn on voltage of 1.5V and 2.1V and maintain decent maximum luminance of 59,699 and 64,244 cd/m 2 , respectively. The sub-bandgap turn-on voltage of QLED with MoO x can be attributed to thermal-assisted energy up-conversion effect due to its lower series resistance. • Various solution process metal oxides are used as QLEDs charge injection layers. • QLEDs with NiO x and MoO x HILs demonstrate lower turn on and forward voltage. • MoO x device achieve a sub-bandgap turn-on voltage of 1.5 V for red QLEDs.

Surface engineering of ZnO nanoparticles with diethylenetriamine for efficient red quantum-dot light-emitting diodes

SummaryDue to the outstanding electron injection/transport capability of ZnO nanoparticles (NPs), quantum-dot light-emitting diodes (QLEDs) are commonly constructed by employing a hybrid device structure with ZnO electron-transporting layer and organic hole-transporting layer. However, the emission quenching of quantum dots and excessive electron injection induced by ZnO NPs also limits the device efficiency and operational stability. Here, diethylenetriamine (DETA) molecules as the ligands are introduced to modify the surface of ZnO NPs, which not only passivate the surface defects of ZnO but also suppress the overwhelming electron injection in the QLED. As a result, the device based on the DETA-modified ZnO NPs exhibits a peak external quantum efficiency of 23.7%, corresponding to an enhancement factor of 129% in comparison with that of the device with as-synthesized ZnO as the electron-transporting layer. The easy and feasible strategy may also be applicable to other photoelectric devices, such as solar cells and photodetectors.