High-efficiency organic light-emitting diodes (OLEDs) with a mixed layer structure

Improved performance of organic light-emitting diodes (OLEDs) as obtained by a mixed layer was investigated. The OLEDs with a mixed layer which were composed of N,N′-diphenyl-N,N′-bis(1-napthyl-phenyl)-1,1′-biphenyl-4,4′-diamine (NPB), tris-(8-hydroxyquinolato) aluminum (Alq₃) and 4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4H-pyran (DCJTB) showed the highest brightness and efficiency, which reached 19048 cd/m² at 17 V and 4.3 cd/A at 10 mA/cm², respectively. The turn-on voltage of the device is 2.6 V. Its Commission Internationale del’Eclairage (CIE) coordinate is (0.497, 0.456) at 17 V, and the CIE coordinates of the device are largely insensitive to the driving voltages, which depicts stabilized yellow color.     

Highly efficient and stable organic light-emitting diode by balancing drift current of charge

Highly efficient and stable OLED device in which hole-drift current and electron-drift current are balanced was fabricated. Drift current characteristics according to the thickness of organic layer were examined using the device with ITO/m-MTDATA/NPB/Al structure that can only move the hole and the device with Al/LiF/Alq₃/LiF/Al structure that can only move the electron. Using the result of such examination, green device with balanced drift current was produced. Device with the structure of m-MTDATA (80 nm)/NPB (20 nm)/C-545T (3%) doped Alq₃ (5 nm)/Alq₃ (59 nm)/LiF (1 nm)/Al (200 nm) showed color purity of (0.309, 0.643) and high efficiency of 7.0 lm/W (14.4 cd/A). Most of light emission was observed inside the green emitting layer. Through the result of EL spectrum for the device also including red emitting layer, same result could be obtained. The device with balanced drift current also showed half life-time of 175 h for initial luminance of 3000 cd/m², which is more stable in comparison to the device without balanced drift current.     

Red organic light-emitting diodes with high efficiency,low driving voltage and saturated red color realized via two step energy transfer based on ADN and Alq3 co-host system

We demonstrated efficient red organic light-emitting diodes based on a wide band gap material 9,10-bis(2-naphthyl)anthracene (ADN) doped with 4-(dicyano-methylene)-2-t-butyle-6-(1,1,7,7-tetramethyl-julolidyl-9-enyl)-4H-pyran (DCJTB) as a red dopant and 2,3,6,7-tetrahydro-1,1,7,7,-tetramethyl-1H,5H,11H-10(2-benzothiazolyl)quinolizine-[9,9a,1gh]coumarin (C545T) as an assistant dopant. The typical device structure was glass substrate/ITO/4,4′,4″-tris(N-3-methylphenyl-N-phenyl-amino)triphenylamine (m-MTDATA)/N,N′-bis(naphthalene-1-yl)-N,N′-diphenyl-benzidine (NPB)/[ADN:Alq₃]:DCJTB:C545T/Alq₃/LiF/Al. It was found that C545T dopant did not by itself emit but did assist the energy transfer from the host (ADN) to the red emitting dopant via cascade energy transfer mechanism. The OLEDs realized by this approach significantly improved the EL efficiency. We achieved a significant improvement regarding saturated red color when a polar co-host emitter (Alq₃) was incorporated in the matrix of [ADN:Alq₃]. Since ADN possesses a considerable high electron mobility of 3.1 × 10⁻⁴ cm²  V⁻¹ s⁻¹, co-host devices with high concentration of ADN (>70%) exhibited low driving voltage and high current efficiency as compared to the devices without ADN. We obtained a device with a current efficiency of 3.6 cd/A, Commission International d’Eclairage coordinates of [0.618, 0.373] and peak λ_max = 620 nm at a current density of 20 mA/cm². This is a promising way of utilizing wide band gap material as the host to make red OLEDs, which will be useful in improving the electroluminescent performance of devices and simplifying the process of fabricating full color OLEDs.     

The roles of zinc selenide sandwiched between organic layers and its applications in white light-emitting diodes

In this paper, the roles of zinc selenide (ZnSe) sandwiched between organic layers, i.e. organic/ZnSe/aluminum quinoline (Alq₃), have been studied by varying device structure. A broad band emission was observed from ITO/poly(N-vinylcarbazole)(PVK)(80 nm)/ZnSe(120 nm)/ Alq₃(15 nm)/Al under electric fields and it combined the emissions from the bulk of PVK, ZnSe and Alq₃, however, emission from only Alq₃ was observed from trilayer device ITO/N,N^′-bis-(1-naphthyl)-N,N^′-diphenyl-1, 1^′-biphenyl-4, 4^′-diamine (NPB) (40 nm)/ZnSe(120 nm)/ Alq₃(15 nm)/Al. Consequently the luminescence mechanism in the ZnSe layer is suggested to be charge carrier injection and recombination. By thermal co-evaporating Alq₃ and 4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4H-pyran (DCJTB), we get white light emission with a Commission Internationale de l’E clairage (C.I.E) co-ordinates of (0.32, 0.38) from device ITO/PVK(80 nm)/ZnSe(120 nm)/ Alq₃:DCJTB(0.5 wt% DCJTB)(15 nm)/Al at 15 V and the device performs stably with increasing applied voltages.     

The effect of Ag layer thickness on the properties of WO3/Ag/MoO3 multilayer films as anode in organic light emitting diodes

Transparent conductive WO₃/Ag/MoO₃ (WAM) multilayer electrodes were fabricated by thermal evaporation and the effects of Ag layer thickness on the optoelectronic and structural properties of multilayer electrode as anode in organic light emitting diodes (OLEDs) were investigated using different analytical methods. For Ag layers with thickness varying between 5 and 20 nm, the best WAM performances, high optical transmittance (81.7%, at around 550 nm), and low electrical sheet resistance (9.75 Ω/cm²) were obtained for 15 nm thickness. Also, the WAM structure with 15 nm of Ag layer thickness has a very smooth surface with an RMS roughness of 0.37 nm, which is suitable for use as transparent conductive anode in OLEDs. The current density?voltage?luminance (J?V?L) characteristics measurement shows that the current density of WAM/PEDOT:PSS/TPD/Alq₃/LiF/Al organic diode increases with the increase in thickness of Ag and WO₃/Ag (15 nm)/MoO₃ device exhibits a higher luminance intensity at lower voltage than ITO/PEDOT:PSS/TPD/Alq₃/LiF/Al control device. Furthermore, this device shows the highest power efficiency (0.31 lm/W) and current efficiency (1.2 cd/A) at the current density of 20 mA/cm², which is improved 58% and 41% compared with those of the ITO-based device, respectively. The lifetime of the WO₃/Ag (15 nm)/MoO₃ device was measured to be 50 h at an initial luminance of 50 cd/m², which is five times longer than 10 h for ITO-based device.     

Influence of thickness of functional layer on performance of organic salt-doped OLED with ITO/PVK:PBD:TBAPF6/Al structure

The effect of thickness of functional layer on the electrical and electroluminescence (EL) properties of single-layer OLED with ITO/PVK:PBD:TBAPF₆/Al structure were investigated where indium tin oxide (ITO) was used as anode, poly(9-vinylcarbazole) (PVK) as polymeric host, 2-(4-biphenylyl)-5-phenyl-1,3,4-oxadiazole (PBD) as electron-transporting molecule, tetrabutylammonium hexafluorophosphate (TBAPF₆) as organic salt dopant and aluminium (Al) as cathode. A unique transition phenomenon at high bias voltage in the devices was observed and the transition was reversible. The transition voltage and turn on voltage decreased with the decrease of functional layer thickness. The turn on voltage was approximately 5.5 V and 6.5 V for 55-nm-thick and 95-nm-thick devices, respectively. However, the current efficiency of 95-nm-thick device was higher than the 55-nm-thick device. More interestingly, the Commission Internationale d’Eclairage (C.I.E.) coordinates of EL spectra of 95-nm-thick device at bias voltage ranging from 7 V to 13 V located in the white light region even without any dye doping. The PL and EL spectra were found completely different. PBD electromer was proposed to dominate the EL spectrum, but the contribution from PVK–PBD electroplex cannot be completely ruled out.     

An organic electroluminescent device made from a gadolinium complex

A gadolinium ternary complex, tris(1-phenyl-3-methyl-4-isobutyryl-5-pyrazolone) (phenanthroline) gadolinium [Gd(PMIP)₃(Phen)] was synthesized and used as a light emitting material in the organic electroluminescent (EL) devices. The triple layer device with a structure of indium tin oxide (ITO)/N,N′-diphenyl-N,N′-bis(3-methylphenyl)-1,1′-biphenyl-4,4′-diamine (TPD) (20 nm)/Gd(PMIP)₃(Phen) (80 nm)/2, 9-dimethyl-4, 7-diphenyl-1, 10-phenanthroline (bathocuproine or BCP) (20 nm)/Mg: Ag(200 nm)/Ag(100 nm) exhibited green emission peaking at 535 nm. A maximum luminance of 230 cd/m² at 17 V and a peak power efficiency of 0.02 lm/w at 9 V were obtained.     

Color-tunable organic light-emitting devices using a thin N,N′-bis-(1-naphthyl)-N,N′-diphenyl-1,1′-biphenyl-4,4′-diamine layer at heterojunction interface

Novel types of multilayer color-tunable organic light-emitting devices (OLEDs) with the structure of indium tin oxide (ITO)/N,N′-bis-(1-naphthyl)-N,N′-diphenyl-1,1′-biphenyl-4,4′-diamine (NPB)/aluminum (III)bis(2-methyl-8-quinolinato)4-phenylphenolato (BAlq)/tris-(8-hydroxyquinolate)-aluminum (Alq₃)/Mg:Ag were fabricated. By inserting a thin layer with different thickness of a second NPB layer at the heterojunction interface of BAlq/Alq₃, the emission zone of devices shifted greatly and optoelectronic characteristics underwent large variation. Although BAlq was reported as a very good hole-blocking and blue-light-emission material, results of measurements in this paper suggested that a certain thickness of NPB layer between BAlq and Alq₃ plays an important role to modify device characteristics, which can act as recombination-controlling layer in the multilayer devices. It also provides a simple way to fabricate color-tunable OLEDs by just changing the thickness of this “recombination-controlling” layer rather than doping by co-evaporation.     

Model and simulation on the efficiencies of microcavity OLEDs

This paper presents simple calculation models of the external quantum efficiency and power efficiency for the microcavity OLEDs. The models take into account the energy spatial distribution of the device and provide a rough estimate of the efficiencies for the planar surface emitting devices, by which the integrating sphere and monochrometer were saved. The external quantum efficiency and luminous current efficiency from the structures of glass/DBR/ITO/NPB/Alq: C545T/Alq/LiF/Al and glass/ITO/NPB/Alq: C545T/Alq/LiF/Al were calculated based on these models and the measured data. Comparing with conventional OLED, the external quantum efficiency and luminous current efficiency of the MOLED were improved 3.1% and 8% at low current density (< 10 mA/cm², corresponding to the display brightness range), respectively.     

Ohmic contact and space-charge-limited current in molybdenum oxide modified devices

The effect of indium-tin oxide (ITO) surface treatment on hole injection of devices with molybdenum oxide (MoO₃) as a buffer layer on ITO was studied. The Ohmic contact is formed at the metal/organic interface due to high work function of MoO₃. Hence, the current is due to space charge limited when ITO is positively biased. The hole mobility of N, N′-bis-(1-napthyl)-N, N′-diphenyl-1, 1′biphenyl-4, 4′-diamine (NPB) at various thicknesses (100–400 nm) has been estimated by using space-charge-limited current measurements. The hole mobility of NPB, 1.09×10⁻⁵ cm²/V s at 100 nm is smaller than the value of 1.52×10⁻⁴ cm²/V s at 400 nm at 0.8 MV/cm, which is caused by the interfacial trap states restricted by the surface interaction. The mobility is hardly changed with NPB thickness for the effect of interfacial trap states on mobility which can be negligible when the thickness is more than 300 nm.     

1.53 μm electroluminescence from ErF3-doped organic light-emitting diodes

Near-infrared (NIR) organic light-emitting devices (OLEDs) are demonstrated by employing erbium fluoride (ErF₃)-doped tris-(8-hydroxyquinoline) aluminum (Alq₃) as the emitting layer. The device structure is ITO/N,N′-di-1-naphthyl-N,N′-diphenylbenzidine (NPB)/Alq₃: ErF₃/2,2′,2″-(1,3,5-phenylene)tris(1-phenyl-1H-benzimidazole) (TPBI)/Alq₃/Al. Room-temperature electroluminescence around 1530 nm is observed due to the ⁴I_13/2–⁴I_15/2 transition of Er³⁺. Full width at half maximum (FWHM) of the electroluminescent (EL) spectrum is ～50 nm. NIR EL intensity from the ErF₃-based device is ～4 times higher than that of Er(DBM)₃Phen-based device at the same current. Alq₃–ErF₃ composite films are investigated by the measurements of X-ray diffraction (XRD), absorption, photoluminescence (PL) and PL decay time. Electron-only devices are also fabricated. The results indicate that energy transfer mechanism and charge trapping mechanism coexist in the NIR EL process.     

The influence of exciton behavior on luminescent characteristics of organic light-emitting diodes

We used N,N′-bis-(1-naphthyl)-N,N′-1-diphenyl-1,1′-biphenyl-4,4′-diamine (NPB), 4,4′-N,N′-dicarbazole-biphenyl (CBP) and tris(8-hydroxyquinoline) aluminum (Alq₃) to fabricate tri-layer electroluminescent (EL) device (device structure: ITO/NPB/CBP/Alq₃/Al). In photoluminescence (PL) spectra of this device, the emission from NPB shifted to shorter wavelength accompanying with the decrease of its emission intensity and moreover the emission intensity of Alq₃ increased relatively with the increase of reverse bias voltage. The blue-shifted emission and the decrease in emission intensity of NPB were attributed to the polarization and dissociation of NPB excitons under reverse bias voltage. The increase of emission intensity of Alq₃ benefited from the recombination of electrons (produced by the dissociation of NPB exciton) and holes (injected from the Al cathode).     

Influence of the thickness of N,N′-Bis(naphthalene-1-yl)-N,N′-bis(phenyl) benzidine layer on the performance of organic light-emitting diodes

We investigated the influence of the thickness of hole-transport layer, N,N′-biphenyl-N,N′-bis(1-naphthyl)-(1,1′-biphenyl)-4,4′-diamine (NPB), on the performance of the typical bi-layer organic light-emitting diodes (OLEDs). It was found that both the current efficiency and the power efficiency of bi-layer OLEDs were improved when the thickness of the hole-transport layer varied from 30 to 120 nm. By investigating the hole-injection efficiency of ITO/NPB contact with various thicknesses of NPB film, we found that the hole-injection efficiency was reduced with the thickness of NPB layer increasing from 60 to 180 nm, which improved the injected carriers balance in devices and increased the efficiency of the bi-layer OLEDs.     

Charge carriers bulk recombination instead of electroplex emission after their tunneling through hole-blocking layer in OLEDs

Charge carriers bulk recombination instead of forming electroplex after their tunneling through a hole-blocking layer, i.e. 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (BCP), in organic electroluminescence (EL) device ITO/poly-(N-vinyl-carbazole)(PVK)/BCP/tris(8-hydroxyquinoline) aluminum (Alq₃)/Al is reported. By changing the thickness of BCP layer, one can find that high electric fields enhance the tunneling process of holes accumulated at the PVK/BCP interface into BCP layer instead of forming “electroplex emission” as reported earlier in literatures. Our experimental data show that charge carriers bulk recombination takes place in both PVK layer and BCP layer, and even in Alq₃ layer when BCP layer is thin enough. Further, it is suggested that PVK is the origin of the emission shoulder at 595 nm in the EL spectra of trilayer device ITO/PVK/BCP/Alq₃/Al.     

Ca/Alq3 hybrid cathode buffer layer for the optimization of organic solar cells based on a planar heterojunction

Use of efficient anode cathode buffer layer (CBL) is crucial to improve the efficiency of organic photovoltaic cells. Here we show that using a double CBL, Ca/Alq₃, allows improving significantly cell performances. The insertion of Ca layer facilitates electron harvesting and blocks hole collection, leading to improved charge selectivity and reduced leakage current, whereas Alq₃ blocks excitons. After optimisation of this Ca/Alq₃ CBL using CuPc as electron donor, it is shown that it is also efficient when SubPc is substituted to CuPc in the cells. In that case we show that the morphology of the SubPc layer, and therefore the efficiency of the cells, strongly depends on the deposition rate of the SubPc film. It is necessary to deposit slowly (0.02 nm/s) the SubPc films because at higher deposition rate (0.06 nm/s) the films are porous, which induces leakage currents and deterioration of the cell performances. The SubPc layers whose formations are kinetically driven at low deposition rates are more uniform, whereas those deposited faster exhibit high densities of pinholes.     

Enhanced photosensitivity of InGaZnO-TFT with a CuPc light absorption layer

A copper phthalocyanine (CuPc) organic semiconductor is capped onto an amorphous indium–gallium–zinc-oxide (InGaZnO) thin film transistor (TFT) to enhance the photosensitivity of InGaZnO-TFT. The CuPc organic semiconductor is served as a light absorption layer and forms a p–n junction with the InGaZnO film. After 60 s white light illumination, light responsivity (R) of InGaZnO-TFT with a CuPc light absorption layer reaches a value of 148.5 A/W at a gate-source voltage (V_GS) of 20 V, which is much larger than that (31.2 A/W) of the conventional InGaZnO-TFT. The results are attributed to the following mechanism. First, a CuPc layer is employed as the light absorption layer. Second, CuPc/InGaZnO p–n junction enables the injection of electron into InGaZnO film. Our results indicate that using CuPc as light absorption layer is an effective approach to improve the photosensitivity of InGaZnO-TFT.     

Enhancing properties of organic light-emitting diodes with LiF inside the hole transport layer

A new device has been made by inserting thin LiF layer in N,N′-diphenyl-N,N′-bis(1-napthyl–phenyl)-1, 1′-biphenyl-4,4′-diamine (NPB), which has a configuration of ITO/NPB(20 nm)/LiF(0.5 nm)/NPB(20 nm)/Alq₃(60 nm)/LiF(0.5 nm)/Al. Compared with normal device, the device inserted LiF layer inside NPB (HTL) can improve its performance. The luminance and efficiency is about 1.4 and 1.3 folds high of the conventional structure, respectively. The suggestion mechanism is that the LiF in the NPB layer can block holes of NPB, and balance the holes and electrons. Consequently, there are more excitons formed to boost the diode’s luminance and efficiency. And it may offer some valuable references for OLED’s structure.     

Diffusion study of multi-organic layers in OLEDs by ToF-SIMS

A model organic light-emitting diodes (OLEDs) with structure of tris(8-hydroxyquinoline) aluminum (Alq₃)/N,N′-diphenyl-N,N′-bis[1-naphthy-(1,1′-diphenyl)]-4,4′-diamine (NPB)/indium tin oxide (ITO)-coated glass was fabricated for diffusion study by ToF-SIMS. The results demonstrate that ToF-SIMS is capable of delineating the structure of multi-organic layers in OLEDs and providing specific molecular information to aid deciphering the diffusion phenomena. Upon heat treatment, the solidity or hardness of the device was reduced. Complicated chemical reaction might occur at the NPB/ITO interface and results in the formation of a buffer layer, which terminates the upper diffusion of ions from underlying ITO.     

Ultraviolet photoelectron spectroscopy investigation of interface formation in an indium-tin oxide/fluorocarbon/organic semiconductor contact

It has been demonstrated that hole-injection in organic light-emitting devices (OLEDs) can be enhanced by inserting a UV-illuminated fluorocarbon (CF_x) layer between indium-tin oxide (ITO) and organic hole-transporting layer (HTL). In this work, the process of interface formation and electronic properties of the ITO/CF_x/HTL interface were investigated with ultraviolet photoelectron spectroscopy. It was found that UV-illuminated fluorocarbon layer decreases the hole-injection barrier from ITO to α-napthylphenylbiphenyl diamine (NPB). Energy level diagrams deduced from the ultraviolet photoelectron spectroscopy (UPS) spectra show that the hole-injection barrier in ITO/UV-treated CF_x/NPB is the smallest (0.46 eV), compared to that in the ITO/untreated CF_x/NPB (0.60 eV) and the standard ITO/NPB interface (0.68 eV). The improved current density-voltage (I-V) characteristics in the UV-treated CF_x-coated ITO contact are consistent with its smallest barrier height.     

Spectral studies of thin films based on poly(N-vinylcarzole) and red dopant

Organic light-emitting diodes were fabricated with a structure of indium-tin-oxide (ITO)/poly(N-vinylcarzole)(PVK):4-(dicyanom-ethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4H-pyran (DCJTB)/8-tris-hydroxyquinoline aluminum (Alq₃)/lithium fluoride (LiF)/Al. The energy transfer from PVK to Alq₃ then to DCJTB and the charge trapping processes were investigated by employing the photoluminescence (PL) and electroluminescence (EL) spectra. With increasing thickness of the Alq₃ layer, the PL and EL emission from PVK were decreased gradually, which indicated that the effective energy transfer occurred from PVK to Alq₃ and then from Alq₃ to DCJTB. At the same time, we found that the exciton recombination zone could be adjusted by controlling the Alq₃ layer thickness and the applied voltages. The effects of different DCJTB concentrations on the optical and electrical characteristics of the devices were investigated, and an obvious red-shift was observed with the DCJTB dopant concentrations increasing in the PL and EL spectra.