ZnO Nanoparticle Electron Transport Layer 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.

Ultrathin Self-Powered Heavy-Metal-Free Cu-In-Se Quantum Dot Photodetectors for Wearable Health Monitoring.

Mechanically deformable photodetectors (PDs) are key device components for wearable health monitoring systems based on photoplethysmography (PPG). Achieving high detectivity, fast response time, and an ultrathin form factor in the PD is highly needed for next-generation wearable PPG systems. Self-powered operation without a bulky power-supply unit is also beneficial for point-of-care application. Here, we propose ultrathin self-powered PDs using heavy-metal-free Cu-In-Se quantum dots (QDs), which enable high-performance wearable PPG systems. Although the light-absorbing QD layer is extremely thin (∼40 nm), the developed PD exhibits excellent performance (specific detectivity: 2.10 × 1012 Jones, linear dynamic range: 102 dB, and spectral range: 250-1050 nm at zero bias), which is comparable to that of conventional rigid QD-PDs employing thick Pb-chalcogenide QD layers. This is attributed to material and device strategies─materials that include Cu-In-Se QDs, a MoS2-nanosheet-blended poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) hole transport layer, a ZnO nanoparticle electron transport layer, Ag and ITO electrodes, and an ultrathin form factor (∼120 nm except the electrodes) that enable excellent mechanical deformability. These allow the successful application of QD-PDs to a wearable system for real-time PPG monitoring, expanding their potential in the field of mobile bioelectronics.

A Study on the ZnO Thin Film Deposited by RF Sputtering Method as an Electron Transport Layer in Quantum Dot Light-Emitting Diodes

We report a highly efficient quantum dot light emitting diode (QLEDs) with a radio frequency (RF) sputtered ZnO thin film as an electron transport layer (ETL) instead of the conventional ZnO nanoparticles (NPs) by solution process. ZnO NPs have been used as a key material to improve the performance of QLEDs, but the charge imbalance in ZnO NPs resulting from fast electron injection, and their limited uniformity are significant disadvantages. In this study, ZnO layers were deposited by RF sputtering with various O2 partial pressures. All of the ZnO films showed preferential growth along the (002) direction, smooth morphology, and good optical transmittance. To test their feasibility for QLEDs, we fabricated devices with RF sputtered ZnO layers as an ETL, which has the inverted structure of ITO/RF sputtered ZnO/QDs/CBP/MoO3/Al. The optical/electrical characteristics of two devices, comprised of RF sputtered ZnO and ZnO NPs, were compared with each other. QLEDs with the sputtered ZnO ETL achieved a current efficiency of 11.32 cd/A, which was higher than the 8.23 cd/A of the QLEDs with ZnO NPs ETL. Next, to find the optimum ZnO thin film for highly efficient QLEDs, deposition conditions with various O2 partial pressures were tested, and device performance was investigated. The maximum current efficiency was 13.33 cd/A when the ratio of Ar/O2 was 4:3. Additional oxygen gas reduced the O vacancies in the ZnO thin film, which resulted in a decrease in electrical conductivity, thereby improving charge balance in the emission layer of the QLEDs. As a result, we provide a way to control the ZnO ETL properties and to improve device performance by controlling O2 partial pressure.

A Study on the ZnO Thin Film Deposited by RF Sputtering Method as an Electron Transport Layer in Quantum Dot Light-Emitting Diodes

We report a highly efficient quantum dot light emitting diode (QLEDs) with a radio frequency (RF) sputtered ZnO thin film as an electron transport layer (ETL) instead of the conventional ZnO nanoparticles (NPs) by solution process. ZnO NPs have been used as a key material to improve the performance of QLEDs, but the charge imbalance in ZnO NPs resulting from fast electron injection, and their limited uniformity are significant disadvantages. In this study, ZnO layers were deposited by RF sputtering with various O2 partial pressures. All of the ZnO films showed preferential growth along the (002) direction, smooth morphology, and good optical transmittance. To test their feasibility for QLEDs, we fabricated devices with RF sputtered ZnO layers as an ETL, which has the inverted structure of ITO/RF sputtered ZnO/QDs/CBP/MoO3/Al. The optical/electrical characteristics of two devices, comprised of RF sputtered ZnO and ZnO NPs, were compared with each other. QLEDs with the sputtered ZnO ETL achieved a current efficiency of 11.32 cd/A, which was higher than the 8.23 cd/A of the QLEDs with ZnO NPs ETL. Next, to find the optimum ZnO thin film for highly efficient QLEDs, deposition conditions with various O2 partial pressures were tested, and device performance was investigated. The maximum current efficiency was 13.33 cd/A when the ratio of Ar/O2 was 4:3. Additional oxygen gas reduced the O vacancies in the ZnO thin film, which resulted in a decrease in electrical conductivity, thereby improving charge balance in the emission layer of the QLEDs. As a result, we provide a way to control the ZnO ETL properties and to improve device performance by controlling O2 partial pressure.

Influence of ZnO nanoparticles as electron transport material on the performance and stability of organic solar cells with sputtered Ag back electrodes

ZnO has been widely used as electron selective material in P3HT:PCBM organic solar cells with either conventional or inverted architecture in order to enhance the extraction of electrons and block the collection of holes at one electrode. In this work we investigate the influence of ZnO nanoparticles electron transport layer (ETL) on the performance and stability of P3HT:PCBM based organic solar cells with conventional architecture and magnetron sputtered back Ag contacts. Their stability in the dark and under real outdoor conditions was monitored by current-voltage measurements and impedance spectroscopy. The impedance spectra were taken as a function of applied bias under illumination in order to reveal more information about the degradation mechanisms taking place in the device.

Effect of Time-Dependent Characteristics of ZnO Nanoparticles Electron Transport Layer Improved by Intense-Pulsed Light Post-Treatment on Hole-Electron Injection Balance of Quantum-Dot Light-Emitting Diodes.

We investigated the effect of intense-pulsed light (IPL) post-treatment on the time-dependent characteristics of ZnO nanoparticles (NPs) used as an electron transport layer (ETL) of quantum-dot light-emitting diodes (QLEDs). The time-dependent characteristics of the charge injection balance in QLEDs was observed by fabrication and analysis of single carrier devices (SCDs), and it was confirmed that the time-dependent characteristics of the ZnO NPs affect the device characteristics of QLEDs. Stabilization of the ZnO NPs film properties for improvement of the charge injection balance in QLEDs was achieved by controlling the current density characteristics via filling of the oxygen vacancies by IPL post-treatment.

Polymer‐Modified ZnO Nanoparticles as Electron Transport Layer for Polymer‐Based Solar Cells

AbstractThe optimization of interfacial layer plays a critical role in the ultimate use of polymer‐based solar cells (PSCs). By introducing an insulating polymer, polystyrene (PS), into the ZnO nanoparticles (NPs) with large particle size, an electron transport layer (ETL) with a thickness of more than 130 nm is produced. The doping of PS not only improves the film quality of ZnO NPs to generate a denser, smoother, and more uniform ETL, but also increases the contact properties between the hydrophilic ZnO and hydrophobic active layer. In comparison to control devices, the power conversion efficiencies (PCEs), short circuit current densities, and fill factors of PSCs with the PS‐modified ETL for a typical fullerene system PTB7‐Th:PC71BM and, also, a nonfullerene system PBDB‐T:ITIC are increased, with PCEs from 8.49% to 9.54% and 10.03% to 11.05%, respectively. The reproducibility, mechanical endurance, and ambient stability of the PSCs with the PS‐modified ZnO NP ETL are significantly improved. The combination of the insulating polymer and ZnO NPs provides a simple, low‐cost way to realize the commercialization of high performance, flexible PSCs.

High-efficiency blue and white electroluminescent devices based on non-Cd I−III−VI quantum dots

Research direction of colloidal quantum dot (QD)-based LEDs (QLEDs), whose performance has substantially progressed over last two decades, has been oriented mostly to the fabrication of next-generation, high-color gamut display devices particularly based on Cd-containing QDs, while their extension to solid-state planar lighting application remains nearly unexplored. In this work, we report on all-solution-processed fabrication of group I–III–VI chalcogenide, non-Cd QDs-based high-efficiency white lighting electroluminescent (EL) devices. For this, using Zn–Cu–Ga–S (ZCGS) QD emitters having a high photoluminescence quantum yield (PL QY) of 80% a multilayered blue QLED consisting of poly(9-vinylcarbazole) hole transport layer (HTL) and Mg-alloyed ZnO nanoparticle electron transport layer (ETL) is first fabricated, showing a maximum external quantum efficiency (EQE) of 7.1%. Then, white QLEDs containing a mixture of blue ZCGS and yellow Cu–In–S QDs as a single emitting layer (EML) are constructed with the same HTL/ETL combination as above. White EL spectral distribution is facilely tunable simply by varying ZCGS-to-CIS QD content ratio in the EML of white EL device. The optimum white QLED not only generates the peak quantities of 2172 cd/m2 in luminance and 4.6% in EQE, corresponding to the record values ever reported in non-Cd white EL devices, but exhibits high color rendering index up to 82.

Electron transport phenomena at the interface of Al electrode and heavily doped degenerate ZnO nanoparticles in quantum dot light emitting diode

ZnO nanoparticles (NPs) of 4–5 nm, widely adopted as an electron transport layer (ETL) in quantum dot light emitting diodes (QD-LEDs), were synthesized using the solution-precipitation process. It is notable that synthesized ZnO NPs are highly degenerate intrinsic semiconductors and their donor concentration can be increased up to ND = 6.9 × 1021 cm–3 by annealing at 140 °C in air. An optical bandgap increase of as large as 0.16–0.33 eV by degeneracy is explained well by the Burstein–Moss shift. In order to investigate the influence of intrinsic defects of ZnO NP ETLs on the performance of QD-LED devices without a combined annealing temperature between ZnO NP ETLs and the emissive QD layer, pre-annealed ZnO NPs at 60 °C, 90 °C, 140 °C, and 180 °C were spin-coated on the annealed QD layer without further post-annealing. As the annealing temperature increases from 60 °C to 180 °C, the defect density related to oxygen vacancy (VO) in ZnO NPs is reduced from 34.4% to 17.8%, whereas the defect density of interstitial Zn (Zni) is increased. Increased Zni reduces the width (W) of the depletion region from 0.21 to 0.12 nm and lowers the Schottky barrier (ФB) between ZnO NPs and the Al electrode from 1.19 to 0.98 eV. We reveal for the first time that carrier conduction between ZnO NP ETLs and the Al electrode is largely affected by the concentration of Zni above the conduction band minimum, and effectively described by space charge limited current and trap charge limited current models.

High-Efficiency Light-Emitting Diodes Based on Formamidinium Lead Bromide Nanocrystals and Solution Processed Transport Layers

Perovskite nanocrystal light-emitting diodes (LEDs) employing architecture comprising a ZnO nanoparticles electron-transport layer and a conjugated polymer hole-transport layer have been fabricated. The obtained LEDs demonstrate a maximum external-quantum-efficiency of 6.04%, luminance of 12998 Cd/m2 and stable electroluminescence at 519 nm. Importantly, such high efficiency and brightness have been achieved by employing solution processed transport layers, formamidinium lead bromide nanocrystals (CH(NH2)2PbBr3 NCs) synthesized at room-temperature and in air without the use of a Schlenk line, and a procedure based on atomic layer deposition to insolubilize the NC film. The obtained NCs show a photoluminescence quantum yield of 90% that is retained upon film fabrica-tion. The results show that perovskite NC LEDs can achieve high-performance without the use of transport layers deposited through evapo-ration in ultra-high-vacuum.

Correlating annealing temperature of ZnO nanoparticle electron transport layer with performance of inverted polymer solar cells

We fabricated inverted polymer solar cells (PSCs) with the structure of ITO/ZnO NPs/Active layer/MoO3/Ag, in which ZnO NPs act as electron transport layer (ETL), poly{4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b0]-dithiophene-2,6-diyl-alt-3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophene-4,6-diy (PTB7) as donor and [6,6]-phenyl-C71-butyric-acidmethyl-ester (PC71BM) as accepter. It is found that the temperature employed during the annealing process of ZnO NPs has significant impact on the efficiency of the resulted PSCs. The optimized PSC with ZnO NPs annealed at 150 °C based on PTB7:PC71BM (1:1.5 w/w) exhibited a power-conversion efficiency of 7.37% with open-circuit voltage (Voc) of 0.722 V, short-circuit current density (Jsc) of 15.38 mA cm−2, and fill factor (FF) of 66.4%. The effects of the annealing temperature on photovoltaic performances were further illustrated with transmission spectrum, atomic force microscopy, X-ray diffraction and PL spectra, meanwhile electrical performance were illustrated with conductivity. Our result indicated that the improved efficiency is due to the optimized ETL/active layer interface, the enhanced transparency and electron transport of the ETLs. As its facile preparation process, this kind of ETL is compatible with roll-to-roll manufacturing of larger area flexible PSCs.

High-efficiency red electroluminescent device based on multishelled InP quantum dots.

We report on the synthesis of highly fluorescent red-emitting InP quantum dots (QDs) and their application to the fabrication of a high-efficiency QD-light-emitting diode (QLED). The core/shell heterostructure of the QDs is elaborately tailored toward a multishelled structure with a composition-gradient ZnSeS intermediate shell and an outer ZnS shell. Using the resulting InP/ZnSeS/ZnS QDs as an emitting layer, all-solution-processible red InP QLEDs are fabricated with a hybrid multilayered device structure having an organic hole transport layer (HTL) and an inorganic ZnO nanoparticle electron transport layer. Two HTLs of poly(9-vinlycarbazole) or poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,4'-(N-(4-sec-butylphenyl))diphenyl-amine), whose hole mobilities are different by at least three orders of magnitude, are individually applied for QLED fabrication and such HTL-dependent device performances are compared. Our best red device displays exceptional figures of merit such as a maximum luminance of 2849 cd/m2, a current efficiency of 4.2 cd/A, and an external quantum efficiency of 2.5%.

Highly Efficient, Color-Reproducible Full-Color Electroluminescent Devices Based on Red/Green/Blue Quantum Dot-Mixed Multilayer.

Over the past few years the performance of colloidal quantum dot-light-emitting diode (QLED) has been progressively improved. However, most of QLED work has been fulfilled in the form of monochromatic device, while full-color-enabling white QLED still remains nearly unexplored. Using red, green, and blue quantum dots (QDs), herein, we fabricate bichromatic and trichromatic QLEDs through sequential solution-processed deposition of poly(9-vinlycarbazole) (PVK) hole transport layer, two or three types of QDs-mixed multilayer, and ZnO nanoparticle electron transport layer. The relative electroluminescent (EL) spectral ratios of constituent QDs in the above multicolored devices are found to inevitably vary with applied bias, leading to the common observation of an increasing contribution of a higher-band gap QD EL over low-band gap one at a higher voltage. The white EL from a trichromatic device is resolved into its primary colors through combining with color filters, producing an exceptional color gamut of 126% relative to National Television Systems Committee (NTSC) color space that a state-of-the-art full-color organic LED counterpart cannot attain. Our trichromatic white QLED also displays the record-high EL performance such as the peak values of 23,352 cd/m(2) in luminance, 21.8 cd/A in current efficiency, and 10.9% in external quantum efficiency.

Enhancement of the power conversion efficiency for inverted organic photovoltaic devices due to the localized surface plasmonic resonant effect of Au nanoparticles embedded in ZnO nanoparticles

The absorption spectra and input photon-to-converted current efficiency curves showed that Au nanoparticles increased the plasmonic broadband light absorption, thereby enhancing the short-circuit current density of the inverted organic photovoltaic (OPV) cells with a Au–ZnO nanocomposite electron transport layer (ETL). The power conversion efficiency of the inverted OPV cell fabricated with a Au–ZnO nanocomposite ETL was higher by 40% than that of the inverted OPV cell fabricated with a ZnO nanoparticle ETL, which could be attributed to the enhanced photon absorption in the active layer due to the localized surface plasmonic resonance of the Au nanoparticles.

Effect of CH3NH3PbI3thickness on device efficiency in planar heterojunction perovskite solar cells

Recent advances in the development of perovskite solar cells based on CH3NH3PbI3 have produced devices with power conversion efficiencies of >15%. While initial work in this area assumed that the perovskite-based cells required a mesoporous TiO2 support, many recent reports have instead focused on the development of planar heterojunction structures. A better understanding of how both cell architecture and various design parameters (e.g., perovskite thickness and morphology) affect cell performance is needed. Here, we report the fabrication of perovskite solar cells based on a ZnO nanoparticle electron transport layer, CH3NH3PbI3 light absorber, and poly(3-hexylthiophene) (P3HT) hole transport layer. We show that vapor-phase deposition of the PbI2 precursor film produces devices with performances equivalent to those prepared using entirely solution-based techniques, but with very precise control over the thickness and morphology of the CH3NH3PbI3 layer. Optimization of the layer thickness yielded devices with efficiencies of up to 11.3%. The results further demonstrate that a delicate balance between light absorption and carrier transport is required in these planar heterojunction devices, with the thickest perovskite films producing only very low power conversion efficiencies.

Stable and efficient quantum-dot light-emitting diodes based on solution-processed multilayer structures

Researchers demonstrate solution-processed light-emitting diodes based on a quantum-dot emissive layer between an organic hole-transport layer and an electron-transport layer of ZnO nanoparticles. The device achieves a luminance of 68,000 cd m−2 and power efficiencies of up to 8.2 lm W−1.