Highly stable and high power efficiency tandem organic light-emitting diodes with transition metal oxide-based charge generation layers

Tandem organic light-emitting diodes (OLEDs) have been studied to improve the long-term stability of OLEDs for 10 years. The key element in a tandem OLEDs is the charge generation layer (CGL), which provides electrons and holes to the adjacent sub-OLED units. Among different types of CGLs, n-doped electron transporting layer (ETL)/transition metal oxide (TMO)/hole transporting layer (HTL) has been intensively studied. Past studies indicate that this kind of CGL can achieve the desired efficiency enhancement, however, its long-term stability was reported not good and sometime even poor than a single OLED. This issue was not well addressed over the past 10 years. Here, for the first time, we found that this is caused by the unwanted diffusion of TMO into the underlying n-doped ETL layer and can be well resolved by introducing an additional diffusion suppressing layer (DSL) between them. Our finding will fully release the potential of TMO-based CGL in tandem OLEDs.     

A red tandem organic light-emitting diode based on organic photovoltaic-type charge generation layer

In this paper, a significant enhancement in current efficiency of a red tandem organic light-emitting diode (OLED), which is based on an organic photovoltaic-type charge generation layer (CGL) of fullerene carbon 60/copper (Ⅱ) phthalocyanine, is introduced. The CGL can absorb a part of photons, radiated from emission zone, then form excitons, which are dissociated into free charges. It induces in lower driven voltage and better efficiency of tandem OLED. Compared with single emitter-unit OLED and tandem OLED with bulk heterojunction CGL, the luminous efficiency boosts remarkably with increasing current density and shows rather slower roll-off. Our results demonstrate that the organic photovoltaic heterojunction, consists of two matched n- and p-type organic semiconductors, is a promising CGL for tandem OLEDs with high efficiency.     

Tandem organic light-emitting diodes with buffer- modified C60/ZnPc as charge generation layer

In this paper, a significant enhancement in current efficiency of the green tandem organic light-emitting diodes (TOLEDs) is demonstrated, which is based on a buffer-modified charge generation layer (CGL) of fullerene carbon (C60)/zinc-phthalocyanine (ZnPc). Al and MoO3 were used as the buffer-modified layers on both sides of the bilayer C60/ZnPc, respectively. Experimental results show that the inserted Al and MoO3 layers can effectively increase the electron extraction of the CGL for obtaining the device performance enhancement. Compared with that of the green TOLEDs without buffer-modified layers in CGL (37.3 cd?A-1), the current efficiency of the green TOLEDs is increased to 54.1 cd?A-1. Further study results find that the performance can also be improved by optimizing the thickness of Al in the CGL. The maximum current efficiency and maximum luminance of the green TOLEDs achieve 63.5 cd?A-1 and 17 873 cd?m-2, respectively, when the multilayer structure of the CGL is Al (3 nm)/C60 (5 nm)/ZnPc (5 nm)/MoO3 (3 nm).     

Tandem organic light-emitting diodes with buffer- modified C60/pentacene as charge generation layer

Buffer-modified C60/pentacene as charge generation layer (CGL) is investigated to achieve effective performance of charge generation. Undoped green electroluminescent tandem organic light-emitting diodes (OLEDs) with multiple identical emissive units and using buffer-modified C60/pentacene organic semiconductor heterojunction (OHJ) as CGL are demonstrated to exhibit better current density and brightness, compared with conventional single-unit devices. The current density and brightness both can be significantly improved with increasing the thickness of Al. However, excessive thickness of Al seriously decreases the transmittance of films and damages the interface. As a result, the maximum current efficiency of 1.43 cd.A-1 at 30 mA.cm-2 can be achieved for tandem OLEDs with optimal thickness of Al. These results clearly demonstrate that Cs2CO3/Al is an effective buffer for C60/pentacene-based tandem OLEDs.     

Design of white tandem organic light-emitting diodes for full-color microdisplay with high current efficiency and high color gamut

Microdisplays based on organic light-emitting diodes (OLEDs) have a small form factor, and this can be a great advantage when applied to augmented reality and virtual reality devices. In addition, a high-resolution microdisplay of 3000 ppi or more can be achieved when applying a white OLED structure and a color filter. However, low luminance is the weakness of an OLED-based microdisplay as compared with other microdisplay technologies. By applying a tandem structure consisting of two separate emission layers, the efficiency of the OLED device is increased, and higher luminance can be achieved. The efficiency and white spectrum of the OLED device are affected by the position of the emitting layer in the tandem structure and calculated via optical simulation. Each white OLED device with optimized efficiency is fabricated according to the position of the emitting layer, and red, green, and blue spectrum and efficiency are confirmed after passing through color filters. The optimized white OLED device with color filters reaches 97.8% of the National Television Standards Committee standard.     

异质结堆叠发光层红色磷光有机发光二极管

本文采用主客体交错结构的发光层,即发光层是 由多组主体材料CBP和客体材料Ir(piq)₂(acac)异质结堆叠构成的。为了改善器件的性能 ,分别优化 了单主体层和单客体层的厚度。研 究表明,单主体层厚度为3~4 nm,单客体层厚度为0.3 nm时,器件能够获得的最大电流效率为3.92 cd/A,色纯度 和发光稳 定性俱佳,1mA工作电流下的CIE色坐标为(0.669,0.308),当工作电流从0.1 mA变化 到1mA,色度坐标的变化值(Δ(x,y)) 仅为(0.004,0.002)。所采用的 主客体交错发光层的制备方法,工艺简单,且因为能分别调整主客体层的厚度而改善因客体 分子聚集或因长程偶极子间相互作用对发光效率的影响,为非掺杂磷光有机发光二极管的制 备提供了思路。     

High efficiency p-i-n organic light-emitting diodes with a novel n-doping layer

This study demonstrated p-i-n organic light-emitting diodes (OLEDs) incorporating a novel n-doping transport layer which is comprised of cesium iodide (CsI) doped into tris-(8-hydroxyquinoline) aluminum (Alq₃) as n-doping electron transport layer (n-ETL) and a p-doping hole transport layer (p-HTL) which includes molybdenum oxide (MoO₃) doped into 4,4′,4″-tris[2-naphthyl(phenyl)amino] triphenylamine (2-TNATA). The device with a 15 wt.% CsI-doped Alq₃ layer shows a turn on voltage of 2.4 V and achieves a maximum power efficiency of to 4.67 lm/W as well, which is significantly improved compared to these (3.6 V and 3.21 lm/W, respectively) obtained from the device with un-doped Alq₃. This improvement is attributed to an increase in the number of electron carriers in the transportation layer leading to an efficient charge balance in the emission zone. A possible mechanism behind the improvement is discussed based on X-ray photoelectron spectroscopy (XPS).     

Effect of bulk and planar heterojunctions based charge generation layers on the performance of tandem organic light-emitting diodes

Tandem organic light-emitting diodes (OLEDs) were fabricated using organic planar and bulk heterojunctions based charge generation layers (CGLs), which were composed of cobalt phthalocyanine (CoPc) and fullerene (C₆₀). The electroluminescent (EL) characteristics of these two kinds of devices were systematically studied. The results showed that, compared to the corresponding devices with planar heterojunction (PHJ) based CGL, the tandem OLEDs with bulk heterojunction (BHJ) based CGL exhibited a dramatic improvement of performance. By investigating the electrical characteristics of CGLs, it was found that more hetero-interfaces introduced in the BHJ blend were beneficial for generating more interfacial dipoles and charge carriers, and the optimized charge transport pathways were favorable to promote both electron and hole mobilities. As a result, the improved charge carrier balance led to the efficiency enhancement of device performance. The results demonstrated the advantageous effect of BHJ blend film for the rational design of CGLs on the realization of high OLEDs performance.     

Optimization for tandem organic light-emitting diodes based on Firpic

A series of single-unit and tandem blue phosphorescent organic light-emitting diodes (OLEDs) were prepared by adjusting the concentration of dopant based on the structure of ITO/NPB/EL unit/Alq₃/Cs₂CO₃/Al. The results show that tandem device with doping concentration of 10 wt% has appropriate energy transfer, which achieves the best performance with a maximum current efficiency of 3.4 cd·A^?1. Further study found that current efficiency and power efficiency of the tandem OLED adding BCP as hole blocking layer (HBL) can achieve 7.85 cd·A^?1 and 0.72 lm·W^?1, respectively. It is 2.88 times and 1.57 times larger than those of sing-unit devices, and green peak is restrained effectively.     

Dibenzofuran derivative as high triplet energy host material for high efficiency in deep blue phosphorescent organic light-emitting diodes

A high efficiency deep blue phosphorescent organic light-emitting diodes was developed using an weak electron transport type high triplet energy host material with dibenzofuran and phosphine oxide units. The host material showed a high triplet energy of 3.01 eV and was effective as the host material for deep blue phosphorescent organic light-emitting diodes. The device performances could be optimized by managing the doping concentration of phosphorescent dopants and a high quantum efficiency of 25.9% with a color coordinate of (0.14, 0.22) was achieved.     

High triplet energy n-type dopants for high efficiency in phosphorescent organic light-emitting diodes

High triplet energy n-type dopants, lithium 2-(oxazol-2-yl)phenolate (LiOx) and lithium 2-(1-methyl-imidazol-2-yl)phenolate (LiIm), were synthesized as n-type doping materials for phosphorescent organic light-emitting diodes and the effect of the n-type doping materials on the electron mobility and device performances of the phosphorescent organic light-emitting diodes was investigated. The LiOx and LiIm n-type dopants were effective to increase the electron mobility of electron transport materials and improve the quantum efficiency of green and blue phosphorescent organic light-emitting diodes.     

Stable efficiency roll-off in blue phosphorescent organic light-emitting diodes by host layer engineering

The device characteristics of blue phosphorescent organic light-emitting diodes (PHOLEDs) with mixed host structure were investigated by changing the combination and the composition of host materials in emissive layer. The distributed recombination zone and balanced charge carrier injection within emissive layer were achieved through mixed host optimization with a hole transport-type and an electron transport-type host materials, therefore the device performances were greatly enhanced, with external quantum and power efficiencies of 21.8% and 53 lm/W. Moreover, mixed host blue PHOLEDs exhibited a extremely low stable efficiency roll-off with quantum efficiencies of 20.3% and 18.6% at a luminance of 1000 and 10,000 cd/m².     

Transparent Al/WO3/Au film as anode for high efficiency organic light-emitting diodes

A transparent Al/WO₃/Au anode is introduced to fabricate high efficiency organic light-emitting devices (OLEDs). By optimizing the thicknesses of each layers of the Al/WO₃/Au structure, the transmittance of Al(7 nm)/WO₃(3 nm)/Au(13 nm) has reached over 55%. Concerning the performance of OLEDs using the optimized anode, the electroluminescence (EL) current efficiency and brightness are enhanced and the EL spectrum is greatly narrowed as compared to the OLEDs using indium-tin-oxide (ITO) as the anode. The results indicate that the metal/metal oxide/metal transparent electrode is a good structure for the anode of high performance OLEDs. In addition, Al/WO₃/Au can function as a composite transparent electrode for top-emitting OLEDs.     

Solution-processed hexaazatriphenylene hexacarbonitrile as a universal hole-injection layer for organic light-emitting diodes

The use of 1,4,5,8,9,11-hexaazatriphenylene hexacarbonitrile (HAT-CN) thin layers, particularly the solution-processed type, as an efficient hole-injection layer (HIL) for organic optoelectronic devices is demonstrated herein. Among the solvents commonly used for solution processing, 2-propanone was found to selectively dissolve HAT-CN, allowing the fabrication of a rigid film. The alignment of the electronic energy levels of the solution-processed HAT-CN and thermally polymerized 2,7-disubstituted fluorene-based triaryldiamine (VB-FNPD) species was evaluated using ultraviolet photoelectron spectroscopy. The results revealed that the lowest unoccupied molecular orbital of HAT-CN and the highest occupied molecular orbital of VB-FNPD were very close to the Fermi level, which facilitated charge transfer at the interface and improved hole injection. The utilization of HAT-CN as HIL resulted in a dramatic enhancement of the performance of solution-processed red, green, and blue organic light-emitting diodes. The external quantum efficiency, current efficiency, and power efficiency of the HAT-CN-based devices were higher than or almost similar to those of optimized poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-based devices. Because of the efficient carrier-injection capability and the capacity to prevent interfacial mixing and erosion during fabrication, solution-processed HAT-CN is promising as a novel alternative to conventional PEDOT:PSS HILs.     

Phosphorescent dye-doped hole transporting layer for organic light-emitting diodes

Hole transport materials are critical to the performance of organic light-emitting diodes (OLEDs). While 1,1-bis(di-4-tolylaminophenyl)cyclohexane (TAPC) with a high triplet energy is widely used for high efficiency phosphorescent OLEDs, devices using TAPC as a hole transport layer (HTL) have a short operating lifetime due to the build-up of trapped charges at the TAPC/emitting layer (EML) interface during device operation. In this work, to solve the operating stability problem, instead of using conventional HTLs, we use a(fac-tris(2-phenylpyridine)iridium (III))(Ir(ppy)₃) doped layer as an HTL to replace the conventional HTLs. Because of the hole injecting and transporting abilities of the phosphorescent dye, holes can be directly injected into the emitting layer without an injection barrier. OLEDs based on a phosphorescent dye-doped HTL show significant improvement in operational stability without loss of efficiency.     

Simplified phosphorescent organic light-emitting diodes with a WO3-doped wide bandgap organic charge transport layer

The effects of p-type doping of wide bandgap ambipolar 4,4′-N,N′-dicarbazolebiphenyl (CBP) with WO₃ were investigated through detailed electrical device characterization. It was found that, to achieve effective doping for improved hole injection and transport, the doping level should be greater than 20 mol% and the doped layer should be at least 10 nm thick. A large downward shift of the Fermi level in WO₃-doped CBP causes band bending and depletion at the doped/undoped CBP interface, resulting in an additional energy barrier which hampers hole transport. Simplified green phosphorescent organic light-emitting diodes (PhOLEDs) with CBP as the hole transport and host material were fabricated. With a WO₃-doped hole transport layer, the PhOLEDs attained brightness of 11,163 cd/m² at 20 mA/cm², and exhibited an improved reliability under constant-current stressing as compared to undoped PhOLEDs.     

Using an embedded nanocomposite layer to increase color-conversion efficiency of organic light-emitting diodes

Down-conversion white organic light-emitting diodes (WOLEDs) have a significant advantage in generating stabilized white-light emissions, but still have room for further improvement in terms of color-conversion efficiency. We demonstrated that TiO₂ nanoparticles mixed with fluorescent dyes could be used to increase the absorption of dyes and thus boost the efficiency of color-conversion. WOLEDs with a nanocomposite color-conversion layer achieved high efficiencies of 12.3% (22.9 cd/A and 22.5 lm/W) and stable white-light emission. In addition, the EL spectra with different viewing angles are close to the ideal Lambertain curve. These outcomes indicate that the nanocomposite-based color-conversion possesses great potential for use in display and lighting applications.     

MoO3 as a cathode buffer layer for enhancing the efficiency in white organic light-emitting diodes

Molybdenum trioxide(MoO 3)as a cathode buffer layer is inserted between LiF and Al to improve the efficiency of white organic light-emitting diodes(OLEDs)in this paper.By changing the MoO 3 thickness,a higher current efficiency of 5.79 cd/A is obtained at a current density of 160 mA/cm2 for the device with a 0.8 nm-thick MoO 3 layer as the cathode buffer layer,which is approximately two times greater than that of the device without MoO 3.The mechanism for improving the device efficiency is discussed.Moreover,at a voltage of 13 V,the device with a 0.8 nm-thick MoO 3 layer achieves a higher luminance of 22370 cd/m2,and the Commission Internationale de I,Eclairage(CIE)color coordinate of the device with 1 nm-thick MoO 3 layer is(0.33,0.34),which shows the best color purity.Simple electron-only devices are tested to confirm the impact of the MoO 3 layer on the carrier injection.     

Low driving voltage white organic light-emitting diodes with high efficiency and low efficiency roll-off

Single emission layer white organic light-emitting diodes (WOLEDs) showing high color stability, low turn-on voltage, high efficiency and low efficiency roll-off by incorporating iridium(III) bis[(4,6-difluo-rophenyl)-pyridinato-N,C2] (FIrpic) and bis(2-phenylbenzothiazolato) (acetylacetonate)iridium(III) (Ir(BT)₂(acac)) phosphors dyes have been demonstrated. Our WOLEDs without any out-coupling schemes as well as n-doping strategies show low operating voltages, low turn-on voltage (defined for voltage to obtain a luminance of 1 cd/m²) of 2.35 V, 79.2 cd/m² at 2.6 V, 940.5 cd/m² at 3.0 V and 10 300 cd/m² at 4.0 V, respectively, and achieve a current efficiency of 40.5 cd/A, a power efficiency of 42.6 lm/W at a practical brightness of 1000 cd/m², and a low efficiency roll-off 14.7% calculated from the maximum efficiency value to that of 5000 cd/m². Such improved properties are attributed to phosphors assisted carriers transport for achieving charge carrier balance in the single light-emitting layer (EML). Meanwhile the host–guest energy transfer and direct exciton formation process are two parallel pathways serve to channel the overall excitons to dopants, greatly reduced the unfavorable energy losses.     

Efficient single layer RGB phosphorescent organic light-emitting diodes

We report efficient single layer red, green, and blue (RGB) phosphorescent organic light-emitting diodes (OLEDs) using a “direct hole injection into and transport on triplet dopant” strategy. In particular, red dopant tris(1-phenylisoquinoline)iridium [Ir(piq)₃], green dopant tris(2-phenylpyridine)iridium [Ir(ppy)₃], and blue dopant bis(3,5-difluoro-2-(2-pyridyl)phenyl-(2-carboxypyridyl)iridium [FIrpic] were doped into an electron transporting 1,3,5-tris(N-phenylbenzimidazole-2-yl)benzene (TPBi) host, respectively, to fabricate RGB single layer devices with indium tin oxide (ITO) anode and LiF/Al cathode. It is found that the maximum current efficiencies of the devices are 3.7, 34.5, and 6.8 cd/A, respectively. Moreover, by inserting a pure dopant buffer layer between the ITO anode and the emission layer, the efficiencies are improved to 4.9, 43.3, and 9.8 cd/A, respectively. It is worth noting that the current efficiency of the green simplified device was as high as 34.6 cd/A, even when the luminance was increased to 1000 cd/m² at an extremely low applied voltage of only 4.3 V. A simple accelerated aging test on the green device also shows the lifetime decay of the simplified device is better than that of a traditional multilayered one.