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.

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.

Area-selective external light extraction for metal bus equipped large area transparent organic light-emitting diodes.

Area-selective external light extraction films based on wrinkle structured films were applied to large transparent organic light-emitting diodes (TOLEDs) with auxiliary metal buses. To be specific, on the external surface of the glass, we selectively formed a wrinkle structured film, which was aligned to the auxiliary metal electrodes. The wrinkle-structured film was patterned using a photo-mask and UV curing, which has the same shape of the auxiliary metal electrodes. With this area-selective film, it was possible to enhance the external quantum efficiencies of the bottom and top emissions TOLEDs by 15.7% and 15.1%, respectively, without significant loss in transmittance. Widened angular luminance distributions were also achieved in both emissions directions.

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.

A randomly nano-structured scattering layer for transparent organic light emitting diodes.

A random scattering layer (RSL) consisting of a random nano-structure (RNS) and a high refractive index planarization layer (HRI PL) is suggested and demonstrated as an efficient internal light-extracting layer for transparent organic light emitting diodes (TOLEDs). By introducing the RSL, a remarkable enhancement of 40% and 46% in external quantum efficiency (EQE) and luminous efficacy (LE) was achieved without causing deterioration in the transmittance. Additionally, with the use of the RSL, the viewing angle dependency of EL spectra was reduced to a marginal degree. The results were interpreted as the stronger influence of the scattering effect over the microcavity. The RSL can be applied widely in TOLEDs as an effective light-extracting layer for extracting the waveguide mode of confined light at the indium tin oxide (ITO)/OLED stack without introducing spectral changes in TOLEDs.

Random nanostructure scattering layer for suppression of microcavity effect and light extraction in OLEDs.

In this study, we investigated the effect of a random nanostructure scattering layer (RSL) on the microcavity and light extraction in organic light emitting diodes (OLEDs). In the case of the conventional OLED, the optical properties change with the thickness of the hole transporting layer (HTL) because of the presence of a microcavity. However, OLEDs equipped with the an RSL showed similar values of external quantum efficiency and luminous efficacy regardless of the HTL thickness. These phenomena can be understood by the scattering effect because of the RSL, which suppresses the microcavity effect and extracts the light confined in the device. Moreover, OLEDs with the RSL led to reduced spectrum and color changes with the viewing angle.

Light extraction from organic light emitting diodes using chemically etched glass substrates.

We have manufactured highly efficient OLED devices fabricated on chemically etched glass substrates. The external quantum efficiency of the OLED devices with the etched glass substrates was increased by 5-27% in comparison with the reference flat glass substrate. Surface morphology, such as indented patterns, significantly affected the external luminance efficiency. A clean surface and the presence of smooth bent edges of indented patterns were found to be important for improving the external luminous efficacy.