Luminance enhancement of top-emitting blue organic light emitting diodes encapsulated with silicon nitride thin films by a double-layer nano-structure.

Even though it is in high demand to introduce a nano-structure (NS) light extraction technology on a silicon nitride to be used as a thin film encapsulation material for an organic light-emitting diode (OLED), only an industry-incompatible wet method has been reported. This work demonstrates a double-layer NS fabrication on the silicon nitride using a two-step organic vapor phase deposition (OVPD) of an industry-compatible dry process. The NS showed a wrinkle-like shape caused by coalescence of the nano-lenses. The NS integrated top-emitting OLED revealed 40 percent enhancement of current efficiency and improvement of the luminance distribution and color change according to viewing angle.

Metal oxide charge transfer complex for effective energy band tailoring in multilayer optoelectronics.

Metal oxides are intensively used for multilayered optoelectronic devices such as organic light-emitting diodes (OLEDs). Many approaches have been explored to improve device performance by engineering electrical properties. However, conventional methods cannot enable both energy level manipulation and conductivity enhancement for achieving optimum energy band configurations. Here, we introduce a metal oxide charge transfer complex (NiO:MoO3-complex), which is composed of few-nm-size MoO3 domains embedded in NiO matrices, as a highly tunable carrier injection material. Charge transfer at the finely dispersed interfaces of NiO and MoO3 throughout the entire film enables effective energy level modulation over a wide work function range of 4.47 - 6.34 eV along with enhanced electrical conductivity. The high performance of NiO:MoO3-complex is confirmed by achieving 189% improved current efficiency compared to that of MoO3-based green OLEDs and also an external quantum efficiency of 17% when applied to blue OLEDs, which is superior to 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile-based conventional devices.

Organic/Inorganic Hybrid Thin-Film Encapsulation Using Inkjet Printing and PEALD for Industrial Large-Area Process Suitability and Flexible OLED Application.

We present herein the first report of organic/inorganic hybrid thin-film encapsulation (TFE) developed as an encapsulation process for mass production in the display industry. The proposed method was applied to fabricate a top-emitting organic light-emitting device (TEOLED). The organic/inorganic hybrid TFE has a 1.5 dyad structure and was fabricated using plasma-enhanced atomic layer deposition (PEALD) and inkjet printing (IJP) processes that can be applied to mass production operations in the industry. Currently, industries use inorganic thin films such as SiNx and SiOxNy fabricated through plasma-enhanced chemical vapor deposition (PECVD), which results in film thickness >1 µm; however, in the present work, an Al2O3 inorganic thin film with a thickness of 30 nm was successfully fabricated using ALD. Furthermore, to decouple the crack propagation between the adjacent Al2O3 thin films, an acrylate-based polymer layer was printed between these layers using IJP to finally obtain the 1.5 dyad hybrid TFE. The proposed method can be applied to optoelectronic devices with various form factors such as rollables and stretchable displays. The hybrid TFE developed in this study has a transmittance of 95% or more in the entire visible light region and a very low surface roughness of less than 1 nm. In addition, the measurement of water vapor transmission rate (WVTR) using commercial MOCON equipment yielded a value of 5 × 10-5 gm-2 day-1 (37.8 °C and 100% RH) or less, approaching the limit of the measuring equipment. The TFE was applied to TEOLEDs and the improvement in optical properties of the device was demonstrated. The OLED panel was manufactured and operated stably, showing excellent consistency even in the actual display manufacturing process. The panel operated normally even after 363 days in air. The proposed organic/inorganic hybrid encapsulant manufacturing process is applicable to the display industry and this study provides basic guidelines that can serve as a foothold for the development of various technologies in academia and industry alike.

Identification of a multi-stack structure of graphene electrodes doped layer-by-layer with benzimidazole and its implication for the design of optoelectronic devices.

Optical properties of benzimidazole (BI)-doped layer-by-layer graphene differ significantly from those of intrinsic graphene. Our study based on transmission electron microscopy and X-ray photoelectron spectroscopy depth profiling reveals that such a difference stems from its peculiar stratified geometry formed in situ during the doping process. This work presents an effective thickness and optical constants that can treat these multi-stacked BI-doped graphene electrodes as a single equivalent medium. For verification, the efficiency and angular emission spectra of organic light-emitting diodes with the BI-doped graphene electrode are modeled with the proposed method, and we demonstrate that the calculation matches experimental results in a much narrower margin than that based on the optical properties of undoped graphene.

Surface wrinkle formation by liquid crystalline polymers for significant light extraction enhancement on quantum dot light-emitting diodes.

We propose an optimal outcoupling structure of a quantum-dot light-emitting diode (QLED) and present material properties based on numerical calculations via the ray-tracing method, in which light extraction properties are obtained according to the surface wrinkles on a substrate. After analyzing the designed microstructure elements, the optimal model was derived and applied to the QLEDs; consequently, the outcoupling efficiency enhanced by 31%. The liquid crystalline polymer forming the random surface wrinkles not only achieves an excellent light extraction through plasma crosslinking but also facilitates large-area processes. We propose an optical design rule for high-efficiency QLED design by analyzing the electro-optical efficiency, emission spectrum, and angular radiation pattern of the optical device.

Thin-film transistor-driven vertically stacked full-color organic light-emitting diodes for high-resolution active-matrix displays.

Thin-film transistor (TFT)-driven full-color organic light-emitting diodes (OLEDs) with vertically stacked structures are developed herein using photolithography processes, which allow for high-resolution displays of over 2,000 pixels per inch. Vertical stacking of OLEDs by the photolithography process is technically challenging, as OLEDs are vulnerable to moisture, oxygen, solutions for photolithography processes, and temperatures over 100 °C. In this study, we develop a low-temperature processed Al2O3/SiNx bilayered protection layer, which stably protects the OLEDs from photolithography process solutions, as well as from moisture and oxygen. As a result, transparent intermediate electrodes are patterned on top of the OLED elements without degrading the OLED, thereby enabling to fabricate the vertically stacked OLED. The aperture ratio of the full-color-driven OLED pixel is approximately twice as large as conventional sub-pixel structures, due to geometric advantage, despite the TFT integration. To the best of our knowledge, we first demonstrate the TFT-driven vertically stacked full-color OLED.

Color-tunable organic light-emitting diodes with vertically stacked blue, green, and red colors for lighting and display applications.

We demonstrate independently and simultaneously controlled color-tunable organic light-emitting diodes (OLEDs) with vertically stacked blue, green, and red elements. The blue, green, and red elements were placed at the bottom, middle, and top positions, respectively, forming color-tunable OLEDs. The independently driven blue, green, and red elements in the color-tunable OLEDs exhibited low driving voltages of 5.3 V, 3.0 V, and 4.6 V, as well as high external quantum efficiencies of 11.1%, 10.9%, and 9.6%, respectively, at approximately 1000 cd/m2. Each element in the color-tunable OLEDs showed high-purity blue, green, and red colors with little parasitic emission owing to the delicately designed device structure resultant from optical simulations. The color-tunable OLEDs could produce any colors inside the triangle formed with blue (0.136, 0.261), green (0.246, 0.697), and red (0.614, 0.386) Commission Internationale de l'éclairage (CIE) 1931 color coordinates. In addition, the correlated color temperatures (CCTs) of white colors in the color-tunable OLED can be easily changed from the warm white to the cool white by controlling the red, green, and blue emissions simultaneously. The white colors in the color-tunable OLED have the CIE 1931 color coordinate of (0.304, 0.351), with a CCT of 6289 K and (0.504, 0.440), with a CCT of 2407K at the driving voltage of 5 V (blue), 2.8 V (green), 4.4 V (red), and 4.6 V (blue), 3 V (green), 5 V (red), respectively. Furthermore, the white color in the color-tunable OLED exhibited a high color rendering index (~88.7) due to vertically stacked three color system. Moreover, we successfully fabricated a large-sized, 14 × 12 pixel array of the color-tunable OLEDs to demonstrate lighting and display applications, respectively.

Mechanistic Understanding of Improved Performance of Graphene Cathode Inverted Organic Light-Emitting Diodes by Photoemission and Impedance Spectroscopy.

Modification of multilayer graphene films was investigated for a cathode of organic light-emitting diodes (OLEDs). By doping the graphene/electron transport layer (ETL) interface with Li, the driving voltage of the OLED was reduced dramatically from 24.5 to 3.2 V at a luminance of 1000 cd/m2. The external quantum efficiency was also enhanced from 3.4 to 12.9%. Surface analyses showed that the Li doping significantly lowers the lowest unoccupied molecular orbital level of the ETL, thereby reducing the electron injection barrier and facilitating electron injection from the cathode. Impedance spectroscopy analyses performed on electron-only devices (EODs) revealed the existence of distributed trap states with a well-defined activation energy, which is successfully described by the Havriliak-Negami capacitance functions and the temperature-independent frequency dispersion parameters. In particular, the graphene EOD showed a unique high-frequency feature as compared to the indium tin oxide one, which could be explained by an additional parallel capacitance element.

Overcoming the efficiency limit of organic light-emitting diodes using ultra-thin and transparent graphene electrodes.

We propose an effective way to enhance the out-coupling efficiencies of organic light-emitting diodes (OLEDs) using graphene as a transparent electrode. In this study, we investigated the detrimental adsorption and internal optics occurring in OLEDs with graphene anodes. The optical out-coupling efficiencies of previous OLEDs with transparent graphene electrodes barely exceeded those of OLEDs with conventional transparent electrodes because of the weak microcavity effect. To overcome this issue, we introduced an internal random scattering layer for light extraction and reduced the optical absorption of the graphene by reducing the number of layers in the multilayered graphene film. The efficiencies of the graphene-OLEDs increased significantly with decreasing the number of graphene layers, strongly indicating absorption reduction. The maximum light extraction efficiency was obtained by using a single-layer graphene electrode together with a scattering layer. As a result, a widened angular luminance distribution with a remarkable external quantum efficiency and a luminous efficacy enhancement of 52.8% and 48.5%, respectively, was achieved. Our approach provides a demonstration of graphene-OLED having a performance comparable to that of conventional OLEDs.

Unraveled Face-Dependent Effects of Multilayered Graphene Embedded in Transparent Organic Light-Emitting Diodes.

With increasing demand for transparent conducting electrodes, graphene has attracted considerable attention, owing to its high electrical conductivity, high transmittance, low reflectance, flexibility, and tunable work function. Two faces of single-layer graphene are indistinguishable in its nature, and this idea has not been doubted even in multilayered graphene (MLG) because it is difficult to separately characterize the front (first-born) and the rear face (last-born) of MLG by using conventional analysis tools, such as Raman and ultraviolet spectroscopy, scanning probe microscopy, and sheet resistance. In this paper, we report the striking difference of the emission pattern and performance of transparent organic light-emitting diodes (OLEDs) depending on the adopted face of MLG and show the resolved chemical and physical states of both faces by using depth-selected absorption spectroscopy. Our results strongly support that the interface property between two different materials rules over the bulk property in the driving performance of OLEDs.

Stable angular emission spectra in white organic light-emitting diodes using graphene/PEDOT:PSS composite electrode.

In this work, we suggest a graphene/ poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) composite as a transparent electrode for stabilizing white emission of organic light-emitting diodes (OLEDs). Graphene/PEDOT:PSS composite electrodes have increased reflectance when compared to graphene itself, but their reflectance is still lower than that of ITO itself. Changes in the reflectance of the composite electrode have the advantage of suppressing the angular spectral distortion of white emission OLEDs and achieving an efficiency of 16.6% for white OLEDs, comparable to that achieved by graphene-only electrodes. By controlling the OLED structure to compensate for the two-beam interference effect, the CIE color coordinate change (Δxy) of OLEDs based on graphene/PEDOT:PSS composite electrodes is 0.018, less than that based on graphene-only electrode, i.e.,0.027.

A nanoporous polymer film as a diffuser as well as a light extraction component for top emitting organic light emitting diodes with a strong microcavity structure.

To improve the viewing angle characteristic as well as the light extraction effect of strong microcavity devices, we fabricated a nanoporous polymer film (NPF) as a scattering medium as well as a light extraction component. We designed two types of organic light emitting diodes (OLEDs) with a strong microcavity effect by changing the thickness of the hole transport layer (HTL; e.g., 30 nm and 60 nm) to investigate two different scattering effects of the NPF. Very interestingly, we could observe a significant enhancement of the external quantum efficiency (EQE) for each device (30 nm thick HTL: 18.0%, 60 nm thick HTL: 31.6%) when we attached a NPF formed on a 125 µm thick PET film coated with the NPF. Furthermore, the NPF successfully suppressed the viewing angle dependence to realize ideal angular emission even in the two extreme microcavity conditions although they are still different from that of a Lambertian distribution.

Flexion bonding transfer of multilayered graphene as a top electrode in transparent organic light-emitting diodes.

Graphene has attracted considerable attention as a next-generation transparent conducting electrode, because of its high electrical conductivity and optical transparency. Various optoelectronic devices comprising graphene as a bottom electrode, such as organic light-emitting diodes (OLEDs), organic photovoltaics, quantum-dot LEDs, and light-emitting electrochemical cells, have recently been reported. However, performance of optoelectronic devices using graphene as top electrodes is limited, because the lamination process through which graphene is positioned as the top layer of these conventional OLEDs is a lack of control in the surface roughness, the gapless contact, and the flexion bonding between graphene and organic layer of the device. Here, a multilayered graphene (MLG) as a top electrode is successfully implanted, via dry bonding, onto the top organic layer of transparent OLED (TOLED) with flexion patterns. The performance of the TOLED with MLG electrode is comparable to that of a conventional TOLED with a semi-transparent thin-Ag top electrode, because the MLG electrode makes a contact with the TOLED with no residue. In addition, we successfully fabricate a large-size transparent segment panel using the developed MLG electrode. Therefore, we believe that the flexion bonding technology presented in this work is applicable to various optoelectronic devices.

Exciton dissociation and charge-transport enhancement in organic solar cells with quantum-dot/N-doped CNT hybrid nanomaterials.

The incorporation of InP quantum-dot/N-doped multiwalled carbon nanotube (QD:NCNT) nanohybrids in the active layer of poly(3-hexylthiophene)/indene-C60 bisadduct (P3HT/ICBA) bulk-heterojuction solar cells enhances V(OC) and J(SC) . The QDs encourage exciton dissociation by promoting electron transfer, while the NCNTs enhance the transport of the separated electrons and eventual charge collection. Such a synergistic effect successfully improves the power conversion efficiency (PCE) from 4.68% (reference cells) to 6.11%.

Position-controlled ZnO nanoflower arrays grown on glass substrates for electron emitter application.

The electron emission of position-controlled grown ZnO nanoflowers was investigated for application in cold cathode electron emission devices. ZnO nanoflower arrays, composed of several nanoneedles with sharp tips, were grown selectively on a conducting glass substrate using a chemical solution deposition method. The morphology and position of the ZnO nanoflowers were controlled by preparing polymethylmethacrylate submicron patterns using electron-beam lithography. Without the patterns, in contrast, vertical ZnO nanoneedles were randomly grown on the substrates with high density. Several samples prepared at the same conditions exhibited almost the same nanoflower morphology and field emission characteristics. Comparison of the field emission characteristics of the ZnO nanoflower arrays and ZnO nanoneedles showed that the arrays had excellent electron emission characteristics, with a low turn-on electric field of 0.13 V µm(-1) at 0.1 µA cm(-2) and a high emission current density of 0.8 mA cm(-2) in an applied electric field of 9.0 V µm(-1). Furthermore, light-emitting devices made using ZnO nanoflower arrays demonstrated strong light emission, and micropixels for display application were clearly displayed.