RESUMEN
The aging phenomenon is commonly observed in quantum-dot light emitting diodes (QLEDs), involving complex chemical or physical processes. Resolving the underlying mechanism of these aging issues is crucial to deliver reliable electroluminescent devices in future display applications. Here, we report a reversible positive aging phenomenon that the device brightness and efficiency significantly improve after device operation, but recover to initial states after long-time storage or mild heat treatment, which can be termed as warming-up effects. Steady and transient equivalent circuit analysis suggest that the radiative recombination current dramatically increases but electron leakage from the quantum dots (QDs) to hole transport layer becomes more accessible during the warming-up process. Further analysis discloses that the notable enhancement of device efficiency can be ascribed to the filling of shell traps in gradient alloyed QDs. This work reveals a distinct positive aging phenomenon featured with reversibility, and further guidelines would be provided to achieve stable QLED devices in real display applications.
RESUMEN
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.
RESUMEN
We report high-efficiency blue-violet quantum-dot-based light-emitting diodes (QD-LEDs) by using high quantum yield ZnCdS/ZnS graded core-shell QDs with proper surface ligands. Replacing the oleic acid ligands on the as-synthesized QDs with shorter 1-octanethiol ligands is found to cause a 2-fold increase in the electron mobility within the QD film. Such a ligand exchange also results in an even greater increase in hole injection into the QD layer, thus improving the overall charge balance in the LEDs and yielding a 70% increase in quantum efficiency. Using 1-octanethiol capped QDs, we have obtained a maximum luminance (L) of 7600 cd/m(2) and a maximum external quantum efficiency (ηEQE) of (10.3 ± 0.9)% (with the highest at 12.2%) for QD-LEDs devices with an electroluminescence peak at 443 nm. Similar quantum efficiencies are also obtained for other blue/violet QD-LEDs with peak emission at 455 and 433 nm. To the best of our knowledge, this is the first report of blue QD-LEDs with ηEQE > 10%. Combined with the low turn-on voltage of â¼2.6 V, these blue-violet ZnCdS/ZnS QD-LEDs show great promise for use in next-generation full-color displays.
RESUMEN
Brain-inspired electronics with synaptic functions hold significant promise for advancing artificial intelligent applications. In this study, we demonstrate the synaptic feature of quantum-dot light-emitting diodes (QLEDs), which can convert electrical pulses into synapse-like light signals (the brightness gradually increases as the electrical pulses are prolonged). These features are analogous to learning and forgetting in biological synapses. The enhancement of brightness can be attributed to the reduction of charge transfer from the quantum dots to ZnO electron transport layer and resistive switching effect. With an integrated complementary metal-oxide-semiconductor (CMOS) drive, arrayed synaptic QLEDs can simulate the visualization of brain-like learning processes, which can reduce the noise toward high image recognition rate (>95.0%) by deep neural networks. Our findings introduce a novel brain-inspired optoelectronic approach with potential applications in optical neuromorphic systems.
RESUMEN
Intrinsic or acquired resistance to chemical drugs severely limits their therapeutic efficacy in cancer treatment. Various intracellular antioxidant molecules, particularly glutathione (GSH), play a crucial role in maintaining intracellular redox homeostasis by mitigating the overproduced reactive oxygen species (ROS) due to rapid cell proliferation. Notably, these antioxidants also eliminate chemical-drug-induced ROS, eventually diminishing their cytotoxicity and rendering them less effective. In this study, we combined erastin, a GSH biosynthesis inhibitor, with 2'-deoxy-5-fluorouridine 5'-monophosphate sodium salt (FdUMP), an ROS-based drug, to effectively disrupt intracellular redox homeostasis and reverse chemotherapy resistance. Therefore, efficient ferroptosis and apoptosis were simultaneously induced for enhanced antitumor effects. Additionally, we employed small interfering RNA targeting PD-L1 (siPD-L1) as a third agent to block immune-checkpoint recognition by CD8+ T cells. The highly immunogenic cell peroxidates or damage-associated molecular patterns (DAMPs) induced by erastin acted synergistically with downregulated PD-L1 to enhance the antitumor effects. To codeliver these three drugs simultaneously and efficiently, we designed GE11 peptide-modified lipid nanoparticles (LNPs) containing calcium phosphate cores to achieve high encapsulation efficiencies. In vitro studies verified its enhanced cytotoxicity, efficient intracellular ROS induction and GSH/GPX4 downregulation, substantial lipid peroxidation product accumulation, and mitochondrial depolarization. In vivo, this formulation effectively accumulated at tumor sites and achieved significant tumor inhibition in subcutaneous colon cancer (CRC) mouse models with a maximum tumor inhibition rate of 83.89% at a relatively low dose. Overall, a strategy to overcome clinical drug resistance was verified in this study by depleting GSH and activating adaptive immunity.
Asunto(s)
Antineoplásicos , Apoptosis , Antígeno B7-H1 , Regulación hacia Abajo , Ferroptosis , Nanopartículas , Ferroptosis/efectos de los fármacos , Animales , Humanos , Ratones , Nanopartículas/química , Antígeno B7-H1/metabolismo , Antígeno B7-H1/antagonistas & inhibidores , Apoptosis/efectos de los fármacos , Antineoplásicos/farmacología , Antineoplásicos/química , Regulación hacia Abajo/efectos de los fármacos , Especies Reactivas de Oxígeno/metabolismo , Lípidos/química , Proliferación Celular/efectos de los fármacos , Femenino , Ensayos de Selección de Medicamentos Antitumorales , Línea Celular Tumoral , LiposomasRESUMEN
FOLFOX regimen, composed of folinic acid, 5-fluorouracil (5-FU) and oxaliplatin (OXP), has been used as clinical standard therapeutic regimen in treatments of colorectal cancer (CRC) and esophageal squamous cell carcinoma (ESCC). To further improve its therapeutic outcomes, FOLFOX was combined with anti-PD-1 antibody to form an advanced chemo-immune combination strategy, which has been proven more efficient in controlling cancer progression and prolonging patients' survival in various clinical trials. However, bad tumor accumulation, relative high toxicity, numerous treatment cycles with high fees and low compliance as well as drug resistance seriously limit the prognosis of FOLFOX regimen. The "all-in-one" formulations, which could precisely delivery multidrug regimen into tumor sites and cells, showed a promising application prospect for targeted drug delivery as well as reducing side effects. However, the design and preparation of the "all-in-one" formulation with high drug encapsulation efficiencies for all drugs was still challenging. Herein, a lipid core-shell nanoparticle codelivery platform was designed for simultaneous encapsulation of variant FOLFOX composed of miriplatin (MiPt), 5-Fluoro-2'-deoxyuridine 5'-monophosphate (FdUMP), calcium folinate (CF) and PD-L1 siRNA (siPD-L1) with high efficiencies, and their synergistic anti-tumor mechanisms were studied, respectively. MiPt, a precursor of OXP, was validated capable of inducing efficient immunogenic cell death (ICD) in this work. Additionally, ICD-mediated release of damage associated molecular patterns functionalized synergistically with PD-L1 silence by siPD-L1 to overcome chemoresistance, reverse suppressive tumor microenvironment and recruit more CD8+ T cells. FdUMP, as the intracellular active form of 5-FU, could induce large amounts of reactive oxygen species to enhance the ICD. CF worked as the sensitizer of FdUMP. The enhanced long-term anti-tumor effect of the prepared "all-in-one" formulation compared to free drug regimen and other controls, was verified in heterotopic CRC mice models and ESCC mice models, providing new thoughts for researchers and showing a promising prospect of translation into clinical applications.
Asunto(s)
Protocolos de Quimioterapia Combinada Antineoplásica , Neoplasias Colorrectales , Neoplasias Esofágicas , Carcinoma de Células Escamosas de Esófago , Nanopartículas , Humanos , Animales , Ratones , Leucovorina/uso terapéutico , Antígeno B7-H1 , Neoplasias Colorrectales/patología , Linfocitos T CD8-positivos/patología , Fluorodesoxiuridilato/uso terapéutico , Fluorouracilo/uso terapéutico , Oxaliplatino , Lípidos/uso terapéutico , Línea Celular Tumoral , Inmunoterapia , Compuestos OrganoplatinosRESUMEN
To industrialize printed full-color displays based on quantum-dot light-emitting diodes, one must explore the degradation mechanism and improve the operational stability of blue electroluminescence. Here, we report that although state-of-the-art blue quantum dots, with monotonically-graded core/shell/shell structures, feature near-unity photoluminescence quantum efficiency and efficient charge injection, the significant surface-bulk coupling at the quantum-dot level, revealed by the abnormal dipolar excited state, magnifies the impact of surface localized charges and limits operational lifetimes. Inspired by this, we propose blue quantum dots with a large core and an intermediate shell featuring nonmonotonically-graded energy levels. This strategy significantly reduces surface-bulk coupling and tunes emission wavelength without compromising charge injection. Using these quantum dots, we fabricate bottom-emitting devices with emission colors varying from near-Rec.2020-standard blue to sky blue. At an initial luminance of 1000 cd m-2, these devices exhibit T95 operational lifetimes ranging from 75 to 227 h, significantly surpassing the existing records.
RESUMEN
The light extraction efficiency in organic light-emitting devices (OLEDs) is enhanced by up to 2.6 times when a close-packed, hemispherical transparent polymer microlens array (MLA) is molded on the light-emitting surface of a top-emitting device. The microlens array helps to extract the waveguided optical emission in the organic layers and the transparent top electrode, and can be manufactured in large area with low cost.
RESUMEN
As the development of artificial intelligence (AI) technology, the deep-learning (DL)-based Virtual Reality (VR) technology, and DL technology are applied in human-computer interaction (HCI), and their impacts on modern film and TV works production and audience psychology are analyzed. In film and TV production, audiences have a higher demand for the verisimilitude and immersion of the works, especially in film production. Based on this, a 2D image recognition system for human body motions and a 3D recognition system for human body motions based on the convolutional neural network (CNN) algorithm of DL are proposed, and an analysis framework is established. The proposed systems are simulated on practical and professional datasets, respectively. The results show that the algorithm's computing performance in 2D image recognition is 7-9 times higher than that of the Open Pose method. It runs at 44.3 ms in 3D motion recognition, significantly lower than the Open Pose method's 794.5 and 138.7 ms. Although the detection accuracy has dropped by 2.4%, it is more efficient and convenient without limitations of scenarios in practical applications. The AI-based VR and DL enriches and expands the role and application of computer graphics in film and TV production using HCI technology theoretically and practically.
RESUMEN
Blue quantum dot (QD) light emitting diode (QLED) developments are far lagging behind the red and green ones as it becomes difficult to balance charge injection and photo stability than the latter. Here, we introduced a combination of a low band energy shell with better surfactants, which largely meet both abovementioned requirements. Our simulation pinpoints that it is the exposed Se on the QD surface, which causes non-radiative relaxations. By adding tributyl phosphine (TBP), which is a good ligand to Se, we recover photoluminescence quantum yield (PLQY) from less than 8.0% up to above 85.0%. The corresponding external quantum efficiency (EQE) of QLEDs increases from 3.1% to 10.1%. This demonstrates that the low bandgap shell with effective surfactant passivation is a promising strategy to enhance QLED performance.
RESUMEN
The tissue-specific targeted delivery and efficient cellular uptake of siRNAs are the main obstacles to their clinical application. Antibody-siRNA-conjugates (ARCs) can deliver siRNA by exploiting the targeting property of antibodies like antibody-drug conjugates (ADCs). However, the effective conjugation of antibodies and siRNAs and the release of siRNAs specifically at target sites have posed challenges to the development of ARCs. In this study, the successful conjugation of antibodies and siRNAs was achieved using a multifunctional peptide as a linker, composed of a cell-penetrating peptide (CPP) and a substrate peptide (SP), which is highly expressed in solid tumors. The resulting antibody-multifunctional peptide (SP-CPP)-siRNA system delivered the siRNA to target tumor cells by the specific binding of the antibody. Once the enzymes on the tumor cell surface hydrolyzed the substrate peptide linker, siRNA-CPP was released from ARCs. The released siRNA-CPP entered the targeted cells via the cellular penetrating ability of CPP, resulting in improved siRNA-mediated gene silencing efficiency, verified both in vitro and in vivo. After intravenous administration, the designed ARCs achieved approximately 66.7% EGFP (Enhanced Green Fluorescent Protein) downregulation efficiency in nude mice xenografted with the HCT116-EGFP tumor model. The proposed system provides a prospective choice for ARC production and the safe and efficient delivery of siRNAs.
Asunto(s)
Péptidos de Penetración Celular , Inmunoconjugados , Animales , Línea Celular Tumoral , Ratones , Ratones Desnudos , Estudios Prospectivos , ARN Interferente PequeñoRESUMEN
Colloidal quantum dot (QD) emitters show great promise in the development of next-generation displays. Although various solution-processed techniques have been developed for nanomaterials, high-resolution and uniform patterning technology amicable to manufacturing is still missing. Here, we present large-area, high-resolution, full-color QD patterning utilizing a selective electrophoretic deposition (SEPD) technique. This technique utilizes photolithography combined with SEPD to achieve uniform and fast fabrication, low-cost QD patterning in large-area beyond 1,000 pixels-per-inch. The QD patterns only deposited on selective electrodes with precisely controlled thickness in a large range, which could cater for various optoelectronic devices. The adjustable surface morphology, packing density and refractive index of QD films enable higher efficiency compared to conventional solution-processed methods. We further demonstrate the versatility of our approach to integrate various QDs into large-area arrays of full-color emitting pixels and QLEDs with good performance. The results suggest a manufacture-viable technology for commercialization of QD-based displays.
RESUMEN
The low efficiency and fast degradation of devices from ink-jet printing process hinders the application of quantum dot light emitting diodes on next generation displays. Passivating the trap states caused by both anion and cation under-coordinated sites on the quantum dot surface with proper ligands for ink-jet printing processing reminds a problem. Here we show, by adapting the idea of dual ionic passivation of quantum dots, ink-jet printed quantum dot light emitting diodes with an external quantum efficiency over 16% and half lifetime of more than 1,721,000 hours were reported for the first time. The liquid phase exchange of ligands fulfills the requirements of ink-jet printing processing for possible mass production. And the performance from ink-jet printed quantum dot light emitting diodes truly opens the gate of quantum dot light emitting diode application for industry.
RESUMEN
The operating lifetime of blue quantum-dot light-emitting diodes (QLED) is currently a short slab for this emerging display technology. To pinpoint the origin of device degradation, here we apply multiple techniques to monitor the electric-field distribution and space-charge accumulation across the multilayered structure before and after lifetime tests. Evident by charge-modulated electro-absorption and capacitance-voltage characteristics, the excited electrons in blue quantum dots (QD) are prone to cross the type II junction between the QD emission layer and the electron-transporting layer (ETL) due to the offset of conduction band minimum, leading to space-charge accumulation and operating-voltage rise in the ETL. Therefore, unlike those very stable red devices, of which the lifetime is primarily limited by the slow degradation of hole-transporting layer, the poor lifetime of blue QLED originates from the fast degradation at the QD-ETL junction. Materials engineering for efficient electron injection is prerequisite for the boost of operating lifetime.
RESUMEN
For the state-of-the-art quantum dot light-emitting diodes, while the ZnO nanoparticle layers can provide effective electron injections into quantum dots layers, the hole transporting materials usually cannot guarantee sufficient hole injection owing to the deep valence band of quantum dots. Developing proper hole transporting materials to match energy levels with quantum dots remains a great challenge to further improve the device efficiency and operation lifetime. Here we demonstrate high-performance quantum dot light-emitting diodes with much extended operation lifetime using quantum dots with tailored energy band structures that are favorable for hole injections. These devices show a T95 operation lifetime of more than 2300 h with an initial brightness of 1000 cd m-2, and an equivalent T50 lifetime at 100 cd m-2 of more than 2,200,000 h, which meets the industrial requirement for display applications.
RESUMEN
A solution-processed molybdenum oxide (MoO x) as the hole injection layer (HIL) by doctor-blade coating was developed to improve the efficiency and lifetime of red-emitting quantum-dot light-emitting diodes (QD-LEDs). It has been demonstrated that by adding isopropyl alcohol into the MoO x precursor during the doctor-blade coating process, the morphology, composition, and the surface electronic structure of the MoO x HIL could be tailored. A high-quality MoO x film with optimized charge injection was obtained, based on which all-solution-processed highly efficient red-emitting QD-LEDs were realized by using a low-cost doctor-blade coating technique under ambient conditions. The red QD-LEDs exhibited the maximum current efficiency and external quantum efficiency of 16 cd/A and 15.1%, respectively. Moreover, the lifetime of red devices initializing at 100 cd/m2 was 3236 h under ambient conditions, which is about twice as long as those with a conventional poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) HIL. Large-area QD-LEDs with 4 in. emitting areas were fabricated with blade coating as well, which exhibit a high efficiency of 12.1 cd/A for red emissions. Our work paves a new way to the realization of efficient large-area QD-LEDs, and the processing and findings from this work can be expanded into next-generation lighting and flat-panel displays.
RESUMEN
To improve the performance of inverted polymer solar cells based on a ternary blend of polymerthieno [3,4-b] thiophene/benzodithiophene (PTB7), [6,6]-phenyl C71-butyric acid methyl ester (PC71BM) and indene-C60-bisadduct (ICBA), a two-layer structure of zinc oxide (ZnO) and Al-doped zinc oxide (AZO) nanoperticles is used to improve electron extraction. Comparing to ZnO, AZO has lower work function and thus provides larger built-in potential across the organic heterojunction, resulting in more efficient photo-current extraction and larger open circuit voltages. Optimum devices with ZnO/AZO nanoparticles show enhancement of both short circuit current and open circuit voltage, leading to a power conversion efficiency (PCE) of 8.85%. The argument of energy level buffering and surface morphology is discussed in the paper. Finally, using a trilayer electron transporting unit of ZnO/AZO/PFN, the interface dipole between the organic active layer and AZO is introduced. The PCE is further enhanced to 9.17%.
RESUMEN
We report full-color quantum-dot-based light-emitting diodes (QLEDs) with high efficiency and long-lifetime by employing high quantum-yield core/shell QDs with thick shells. The increased shell thickness improves the confinement of excitons in the QD cores, and helps to suppress Auger recombination and Förster resonant energy transfer among QDs. Along with optimizing the QD emitting layer thickness and hole transport materials, we achieved significant improvements in device performance as a result of increasing the QD shell thickness to above 5 nm. By using poly[9,9-dioctylfluorene-co-N-[4-(3-methylpropyl)]-diphenylamine] (TFB) as a HTL with a 38 nm thick QD layer, these QLEDs show maximum current efficiencies of 18.9 cd A-1, 53.4 cd A-1, and 2.94 cd A-1, and peak external quantum efficiencies (EQEs) of 10.2%, 15.4%, and 15.6% for red, green, and blue QLEDs, respectively, all of which are well maintained over a wide range of luminances from 102 to 104 cd m-2. To the best of our knowledge, this is the first report of blue QLEDs with ηEQE > 15%. Most importantly, these devices also possess long lifetimes with T70 (the time at which the brightness is reduced to 70% of its initial value) of 117 h (red, with an initial luminance of 8000 cd m-2), 84 h (green, 6000 cd m-2) and 47 h (blue, 420 cd m-2). With further optimization of QD processing and device structures, these LEDs based on thick-shell QDs show great promise for use in next-generation full-color displays and lighting devices.
RESUMEN
Colloidal nanoplatelets (NPLs) have recently been introduced as semiconductor emissive materials for the fabrication of quantum dot light-emitting diodes (QLED) on account of their ultra-narrow photoluminescence (PL) linewidth. In this paper, we report a multilayer all solution-processed green QLED based on colloidal CdSe/CdS core/shell NPLs with a narrow PL full-width-at-half-maximum (FWHM) of 12 nm. Our characterization results reveal that this kind of NPL containing QLED exhibit a low operating voltage of 2.25 V and a maximum luminance up to 33 000 cd m(-2), and peak external quantum efficiency (EQE) of 5%, corresponding to 12.5 cd A(-1) in luminance efficiency. Particularly, these devices show ultra-high color purity for electroluminescence (EL) with FWHM of 14 nm. As extremely narrow EL and ultra-pure color is highly attractive in the applications of LED industries, this work signifies the unique potential application of one new class of colloidal core/shell NPLs in achieving bright and efficient LEDs with superior color saturation.
RESUMEN
A highly efficient inverted polymer solar cell (PSC) has been successfully demonstrated by using a ZnO nanoparticle (NP) and poly[(9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctyfluorene)] (PFN) bilayer structure as an effective electron collecting layer. This ZnO/PFN bilayer structure is designed to combine the advantages of both ZnO and PFN, based on the performance comparison of ZnO-only, PFN-only, and ZnO/PFN bilayer devices in our work. ZnO NPs can serve as an efficient electron transport and buffer layer for reduced series resistance, while the PFN interlayer can improve the energy level alignment of devices through the formation of an interfacial dipole. With the enhanced electron extraction induced by the ZnO/PFN bilayer structure and PTB7:ICBA:PC71BM ternary system, the corresponding inverted PSC device shows a high PCE of 9.3%, which is more than a 15% improvement compared to the ZnO- or PFN-only devices.