Quenching of electroluminescence and charge trapping in high-efficiency Ge-implanted MOS light-emitting silicon diodes

Combined measurements of charge trapping and electroluminescence intensity as a function of injected charge and current have been carried out with the aim of clarifying the mechanisms of electroluminescence (EL) quenching in Ge-implanted ITO-SiO₂-Si light-emitting silicon diodes. Good correlation between the negative charge capture in traps of small effective capture cross-sections (σ_t1 ^e=1.7×10^-19 cm² and σ_t2 ^e=4.8×10^-20 cm²) located in SiO₂, and the quenching of the asymmetrical EL line with a maximum intensity at 400 nm has been observed. Similar correlation between the electron capture in traps with extremely small effective capture cross-section (σ_t3 ^e=5×10^-21 cm²) and the quenching of the EL line at 637 nm has been established. A quantitative model for the EL quenching has been developed, which takes into account the modification of the luminescent centers with subsequent electron capture at the newly generated traps. The model shows good agreement between simulation and experimental data. It also demonstrates that small effective capture cross-sections for electron charging during the EL quenching are determined by the probability of the luminescence centers (LCs) being disrupted, and enables one to estimate the Ge concentration associated with the EL at 400 nm. PACS 72.20.Jv; 73.40.Qv; 73.50.Gr     

Temperature‐dependent electroluminescence intensity in green and blue (In,Ga)N multiple‐quantum‐well diodes

The electroluminescence (EL) intensity has been investigated of green and blue (In,Ga)N multiple‐quantum‐well diodes grown on c ‐plane sapphire over a wide temperature range and as a function of current between 0.01 mA and 10 mA. The EL intensity of the green diode with p‐(Al,Ga)N electron blocking layer does not show low‐temperature quenching, especially at low injection levels, previously observed for the blue (In,Ga)N quantum‐well diodes. This finding rules out possi‐ bilities that the freeze‐out of holes at deep Mg acceptor levels and the failure of hole injections through the p‐(Al,Ga)N layer are directly responsible for the EL quenching at temperatures below 100 K. Variations of the EL efficiency with current level suggest that capture/escape efficiencies of injected carriers by the wells play an important role for the determination of EL external quantum efficiency. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Design and development of organic light emitting diodes

A highly luminescent thiophene based conjugated polymer, i.e., poly[2-(3-thienyl) ethanol butoxy carbonyl–methyl urethane] (PURET) has been used for fabricating polymeric light emitting diodes in the present investigations. PURET has been doped with varying amount of (4-dicyano methylene-2 methyl-6-(p-dimethyl amino styryl)-4H-pyran) dye. Enhanced electroluminescence (EL) and quantum efficiency has been observed by incorporating small amount of dye. An attempt has been made to understand the mechanism of charge transport, which helped in the understanding of the possible reasons for enhancement of EL emission as a function of dye concentration and allowed for further optimization of device performance. Based on capacitance–voltage (C–V) analysis it is proposed that the devices in the present investigations, may be modeled as a resistance and capacitor in parallel for the frequency range of 20 Hz–1 MHz. The enhancement in EL intensity and external quantum efficiency of PURET has been observed in addition of small amount of dye which is attributed to the trapping of excitons and enhanced probability electron–hole recombination in EL layer. In addition, voltage tunable color emission has also been observed. This is attributed to the charge transport among the various layers depending upon the applied voltage.     

电极处势垒对新结构器件电子输运的影响

在新结构薄膜电致发光器件中,电极处的势垒的高度决定电子的注入数量.在电极界面处插入不同的薄膜材料,可以改变势垒的高度,并对电子注入数量和器件的发光亮度产生影响.通过拟合计算得到ZnO/SiO,ITO/SiO的界面势垒高度分别为0.51和1.87eV. 关键词：     

Evidence for the changes in hole injection mechanism with a CoPc hole injection layer

The hole injection in hole-only devices with the structures of Al/N,N′-bis(1-naphthyle)-N,N′-diphenyl-1,1′-biphenyl-4,4′-diamine (NPB)/ITO and Al/NPB/cobalt phthalocyanine (CoPc)/ITO were analyzed. With the combined analysis of current density–voltage and impedance measurement, the charge injection mechanism based on the injection limited current model was investigated. The NPB single layer device shows Richardson–Schottky type thermionic emission in the entire applied bias range. On the other hand, the device with the CoPc hole injection layer shows thermionic emission until the applied bias reaches 3.7 V. Increasing the bias further, Fowler–Nordheim tunneling dominates the charge injection. The changes of hole injection mechanism were discussed by evaluating the energy level changes with internal field distributions.     

Correlation of charge trapping and electroluminescence in highly efficient Si-based light emitters

In this paper we report on recent results on charge trapping and electroluminescence (EL) from Ge rich SiO₂ layers. Thermally grown 80 nm thick SiO₂ layers were implanted with Ge ions at energies of 30–50 keV to peak concentrations of 1–6 at%. Subsequently rapid thermal annealing was performed at 1000°C for 6, 30 and 150 s under a nitrogen atmosphere in order to form luminescence centers. A combination of capacitance–voltage (CV) and current–voltage (IV) methods was used for the investigation of the trapping properties. It was found that at electric fields <8 MV/cm electron trapping dominates while at higher electric fields which are typically required for the EL operation of the devices positive charge trapping occurs. It is assumed, that the trapping sites which are responsible for the trapping of the positive charge are in strong relation to the defects causing the luminescence.     

Correlation between defect-related electroluminescence and charge trapping in Gd-implanted SiO<Subscript>2</Subscript> layers

When amorphous silica is bombarded with energetic ions, various types of defects are created as a consequence of ion-solid interaction (oxygen deficient centers (ODC), non-bridging oxygen hole centers (NBOHC), E^′-centers, etc.). Luminescent peaks from oxygen deficiency centers at 2.7 eV, non-bridging oxygen hole centers at 1.9 eV and defect centers with emission at 2.07 eV were observed by changing the concentration of implanted Gd³⁺ ions. Charge trapping in Gd-implanted SiO₂ layers was induced using constant current electron injection to study the electroluminescence intensity with dependence on the applied voltage change. The process of electron trap generation during high field carrier injection results in an increase of the electroluminescence from non-bridging oxygen hole centers. Direct correlation between electron trapping and the quenching of the electroluminescence at 2.07 eV and 2.7 eV was observed with variation of the implanted Gd concentration. PACS 78.60.i; 72.20.Jv; 78.20.-e     

Exciton–dopant and exciton–charge interactions in electronically doped OLEDs

The electronic dopants, like tetrafluorocyanoquinodimethane (F₄–TCNQ) molecules, used for p-doping of hole transport layers in organic light-emitting diodes (OLEDs) are found to quench the electroluminescence (EL) if they diffuse into the emissive layer. We observed EL quenching in OLED with F₄-TCNQ doped N,N′-diphenyl-N′N′-bis(1-naphthyl)-1,1′-biphenyl-4,4′-diamine hole transport layer at large dopant concentrations, >5%. To separate the effects of exciton–dopant quenching, from exciton–polaron quenching we have intentionally doped the emissive layer of (8-tris-hydroxyquinoline) with three acceptors (A) of different electron affinities: F₄-TCNQ, TCNQ, and C₆₀, and found that C₆₀ is the strongest EL-quencher, while F₄-TCNQ is the weakest, contrary to intuitive expectations. The new effects of charge transfer and usually considered energy transfer from exciton to neutral (A) and charged acceptors (A⁻) are compared as channels for non-radiative Ex–A decay. At high current loads the EL quenching is observed, which is due to decay of Ex on free charge carriers, hole polarons P⁺. We consider contributions to Ex–P⁺ interaction by short-range charge transfer and describe the structure of microscopic charge transfer (CT)-processes responsible for it. The formation of metastable states of ‘charged excitons’ (predicted and studied by Agranovich et al. Chem. Phys. 272 (2001) 159) by electron transfer from a P to an Ex is pointed out, and ways to suppress non-radiative Ex–P decay are suggested.     

Effect of thickness variation of hole injection and hole blocking layers on the performance of fluorescent green organic light emitting diodes

In this paper we present the effect of thickness variation of hole injection and hole blocking layers on the performance of fluorescent green organic light emitting diodes (OLEDs). A number of OLED devices have been fabricated with combinations of hole injecting and hole blocking layers of varying thicknesses. Even though hole blocking and hole injection layers have opposite functions, yet there is a particular combination of their thicknesses when they function in conjunction and luminous efficiency and power efficiency are maximized. The optimum thickness of CuPc (Copper(II) phthalocyanine) layer, used as hole injection layer and BCP (2,9 dimethyl-4,7-diphenyl-1,10-phenanthroline) used as hole blocking layer were found to be 18 nm and 10 nm respectively. It is with this delicate adjustment of thicknesses, charge balancing is achieved and luminous efficiency and power efficiency were optimized. The maximum luminous efficiency of 3.82 cd/A at a current density of 24.45 mA/cm² and maximum power efficiency of 2.61 lm/W at a current density of 5.3 mA/cm² were achieved. We obtained luminance of 5993 cd/m² when current density was 140 mA/cm². The EL spectra was obtained for the LEDs and found that it has a peaking at 524 nm of wavelength.     

Change of the dominant luminescent mechanism with increasing current density in molecularly doped organic light-emitting devices

We have fabricated and measured a series of electroluminescent devices with the structure of ITO/TPD/Eu(TTA)₃phen (x):CBP/BCP/ALQ/LiF/Al, where x is the weight percentage of Eu(TTA)₃phen (from 0% to 6%). At very low current density, carrier trapping is the dominant luminescent mechanism and the 4% doped device shows the highest electroluminescence (EL) efficiency among all these devices. With increasing current density, Förster energy transfer participates in EL process. At the current density of 10.0 and 80.0 mA/cm², 2% and 3% doped devices show the highest EL efficiency, respectively. From analysis of the EL spectra and the EL efficiency-current density characteristics, we found that the EL efficiency is manipulated by Förster energy transfer efficiency at high current density. So we suggest that the dominant luminescent mechanism changes gradually from carrier trapping to Förster energy transfer with increasing current density. Moreover, the conversion of dominant EL mechanism was suspected to be partly responsible for the EL efficiency roll-off because of the lower EL quantum efficiency of Förster energy transfer compared with carrier trapping.     

Electrical characterization of impurity-free disordering-induced defects in n-GaAs using native oxide layers

Defects created in rapid thermally annealed n-GaAs epilayers capped with native oxide layers have been investigated using deep-level transient spectroscopy (DLTS). The native oxide layers were formed at room temperature using pulsed anodic oxidation. A hole trap H0, due to either interface states or injection of interstitials, is observed around the detection limit of DLTS in oxidized samples. Rapid thermal annealing introduces three additional minority-carrier traps H1 (E_V+0.44 eV), H2 (E_V+0.73 eV), and H3 (E_V+0.76 eV). These hole traps are introduced in conjunction with electron traps S1 (E_C-0.23 eV) and S2 (E_C-0.45 eV), which are observed in the same epilayers following disordering using SiO₂ capping layers. We also provide evidence that a hole trap whose DLTS peak overlaps with that of EL2 is present in the disordered n-GaAs layers. The mechanisms through which these hole traps are created are discussed. Capacitance–voltage measurements reveal that impurity-free disordering using native oxides of GaAs produced higher free-carrier compensation compared to SiO₂ capping layers. Received: 12 March 2002 / Accepted: 15 July 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +61-2/6125-0381, E-mail: pnk109@rsphysse.anu.edu.au     

Reactivation of damaged rare earth luminescence centers in ion-implanted metal–oxide–silicon light emitting devices

Charge trapping and quenching of electroluminescence (EL) in SiO₂ layers implanted by Ge and rare earth (RE) ions during hot electron injection were investigated. In case of the SiO₂:Ge layer the EL quenching is caused by the transformation of the luminescent defects (Ge–Si or Ge–Ge) to optically inactive centers during hot electron excitation, whereas the EL from rare earth centers is quenched due to the electron trapping by RE-centers or their surroundings, but not due to their optical deactivation. Therefore, the flash lamp post-injection annealing releasing trapped electrons reactivates RE centers and increases the operating time of metal–oxide–silicon light emitting devices (MOSLEDs). PACS 72.20.Jv; 73.40.Qv; 73.50.Gr     

Surface electroluminescence phenomena correlated with trapping parameters of insulating polymers

Electroluminescence (EL) phenomena are closely linked to the space charge and degradation in insulating polymers, and dominated by the luminescence and trap centers. EL emission has been promising in defining the onset of electrical aging and in the investigation of dissipation mechanisms. Generally, polymeric degradation reveals the increment of the density of luminescence and trap centers, so a fundamental study is proposed to correlate the EL emission of insulating polymers and their trapping parameters. A sensitive photon counting system is constructed to detect the weak EL. The time- and phase-resolved EL characteristics from different polymers (LDPE, PP and PTFE) are investigated with a planar electrode configuration under stepped ac voltage in vacuum. In succession, each sample is charged with exposing to multi-needle corona discharge, and then its surface potential decay is continuously recorded at a constant temperature. Based on the isothermal relaxation current theory, the energy level and density of both electron and hole trap distribution in the surface layer of each polymer is obtained. It is preliminarily concluded that EL phenomena are strongly affected by the trap properties, and for different polymers, its EL intensity is in direct contrast to its surface trap density, and this can be qualitatively explained by the trapping and detrapping sequence of charge carriers in trap centers with different energy level.     

Optimal thickness of hole transport layer in doped OLEDs

Current-voltage (I–V) and electroluminescence (EL) characteristics of organic light-emitting devices with N,N’-Di-[(1-naphthalenyl)-N,N’-diphenyl]-(1,1’-biphenyl)-4,4’-diamine (NPB) of various thicknesses as the hole transport layer, and tris(8-hydroxyquinoline)aluminum (Alq₃) selectively doped with 4-(dicyanomethylene)-2-methyl-6-(p-dimethylaminostyryl)-4H-pyran (DCM) as the electron transport layer, have been investigated. A trapped charge induced band bend model is proposed to explain the I–V characteristics. It is suggested that space charge changes the injection barrier and therefore influences the electron injection process in addition to the carrier transport process. Enhanced external quantum efficiency of the devices due to the electron blocking effect of an inserted NPB layer is observed. The optimal thickness of the NPB layer is experimentally determined to be 12±3 nm in doped devices, a value different from that for undoped devices, which is attributed to the electron trap effect of DCM molecules. This is consistent with the result that the proportion of Alq₃ luminescence in the total electroluminescence (EL) spectra increases with NPB thickness up to 12 nm under a fixed bias. PACS 72.80.Le; 85.60.Jb     

Trapping centers and their distribution in Tl2Ga2Se3S layered single crystals

Thermally stimulated current (TSC) measurements with current flowing perpendicular to the layers were carried out on Tl₂Ga₂Se₃S layered single crystals in the temperature range of 10-260 K. The experimental data were analyzed by using different methods, such as curve fitting, initial rise and isothermal decay methods. The analysis revealed that there were three trapping centers with activation energies of 12, 76 and 177 meV. It was concluded that retrapping in these centers was negligible, which was confirmed by the good agreement between the experimental results and the theoretical predictions of the model that assumes slow retrapping. The capture cross section and the concentration of the traps have been also determined. An exponential distribution of electron traps was revealed from the analysis of the TSC data obtained at different light illumination temperatures. This experimental technique provided values of 10 and 88 meV/decade for the traps distribution related to two different trapping centers.     

Modeling of transient electroluminescence overshoot in bilayer organic light-emitting diodes using rate equations

When a voltage pulse is applied under forward biased condition to a spin-coated bilayer organic light-emitting diode (OLED), then initially the electroluminescence (EL) intensity appearing after a delay time, increases with time and later on it attains a saturation value. At the end of the voltage pulse, the EL intensity decreases with time, attains a minimum intensity and then it again increases with time, attains a peak value and later on it decreases with time. For the OLEDs, in which the lifetime of trapped carriers is less than the decay time of the EL occurring prior to the onset of overshoot, the EL overshoot begins just after the end of voltage pulse. The overshoot in spin-coated bilayer OLEDs is caused by the presence of an interfacial layer of finite thickness between hole and electron transporting layers in which both transport molecules coexist, whereby the interfacial energy barrier impedes both hole and electron passage. When a voltage pulse is applied to a bilayer OLED, positive and negative space charges are established at the opposite faces of the interfacial layer. Subsequently, the charge recombination occurs with the incoming flux of injected carriers of opposite polarity. When the voltage is turned off, the interfacial charges recombine under the action of their mutual electric field. Thus, after switching off the external voltage the electrons stored in the interface next to the anode cell compartment experience an electric field directed from cathode to anode, and therefore, the electrons move towards the cathode, that is, towards the positive space charge, whereby electron–hole recombination gives rise to luminescence. The EL prior to onset of overshoot is caused by the movement of electrons in the electron transporting states, however, the EL in the overshoot region is caused by the movement of detrapped electrons. On the basis of the rate equations for the detrapping and recombination of charge carriers accumulated at the interface expressions are derived for the transient EL intensity I, time t_m and intensity I_m corresponding to the peak of EL overshoot, total EL intensity I_t and decay of the intensity of EL overshoot. In fact, the decay prior to the onset of EL overshoot is the decay of number of electrons moving in the electron transporting states. The ratio I_m/I_s decreases with increasing value of the applied pulse voltage because I_m increases linearly with the amplitude of applied voltage pulse and I_s increases nonlinearly and rapidly with the increasing amplitude of applied voltage pulse. The lifetime τ_t of electrons at the interface decreases with increasing temperature whereby the dependence of τ_t on temperature follows Arrhenius plot. This fact indicates that the detrapping involves thermally-assisted tunneling of electrons. Using the EL overshoot in bilayer OLEDs, the lifetime of the charge carriers at the interface, recombination time of charge carriers, decay time of the EL prior to onset of overshoot, and the time delay between the voltage pulse and onset time of the EL overshoot can be determined. The intense EL overshoot of nanosecond or shorter time duration may be useful in digital communication, and moreover, the EL overshoot gives important information about the processes involving injection, transport and recombination of charge carriers. The criteria for appearance of EL overshoot in bilayer OLEDs are explored. A good agreement is found between the theoretical and experimental results.     

Bright electroluminescent devices with tunable spectra obtained by strictly controlling the doping concentration of electron injection sensitizer

In this paper, we report an efficient strategy to design bright blue and blue-green electroluminescent (EL) devices by slightly doping tris(8-hydroxyquinoline) aluminum (Alq₃) into N,N′-diphenyl-N,N′-bis(1-naphthyl)-1,1′-diphenyl-4,4′-diamine (NPB) as the light-emitting layer (EML). Bright EL devices with tunable spectra were obtained by strictly controlling the doping concentration of Alq₃. With increasing current density, EL efficiencies of these devices increase first and then decrease gradually after reaching the maximum. Analyzing the current density-voltage (J−V) characteristics of hole-only and electron-only devices, we found the presence of Alq₃ molecules in EML not only facilitates the injection of electrons from hole block layer (HBL) into EML but also stays the transport of holes in EML, thus causing significant enhancement of EL efficiency and brightness due to improved carriers balance and broadening of recombination zone. More interestingly, the doping concentration of Alq₃ strongly influences the injection and transport processes of electrons, thus determining the distribution of holes and electrons on NPB and Alq₃ molecules.     

多层结构的阴极修饰层对有机电致发光器件的性能改善

为提高有机电致发光器件（OLEDs）的阴极电子注入效率,我们设计了新型的阴极杂化修饰层,其结构为Bphen∶LiF/Al/MoO₃,将其应用到器件ITO/NPB/Alq₃/Al中,参考器件的电子注入层选用传统材料LiF。实验研究表明,与传统的阴极修饰层LiF相比,基于这种杂化结构的阴极修饰层非常有效。测试了器件的电致发光光谱（EL谱）,其峰值位于534 nm,发光来自于Alq₃,实验中我们可以观察到明亮的绿色发光。将其与传统参考器件的EL谱进行对比,在电流密度40 mA·cm-2下,两个器件的电致发光光谱是一致的。在0～100 mA·cm-2范围内,对器件的EL谱进行了测试。实验结果表明,随着电流密度的增加,器件的发光增强,但是EL谱的形状和谱峰的位置是固定不变的。与参考器件对比,基于杂化修饰层的器件的发光性能更好。研究表明,杂化修饰层的最佳参数为Bphen∶LiF(5 nm; 6%)/Al(1 nm)/MoO₃(5 nm),在测试范围内,器件的最大电流效率和最大功率效率分别为4.28 cd·A-1和2.19 lm·W-1,相比参考器件提高了25.5%和23.7%。器件的电流密度-电压特性曲线表明阴极杂化修饰层可以增强电子的注入,使器件中的载流子更加平衡,从而提高了器件的发光性能。从两个角度对器件效率的增强进行了理论方面的论证。一方面利用阴极杂化修饰层的作用机制来解释。在HML中,LiF能填充Bphen的电子陷阱,增强电流的注入,同时HML也能限制空穴的传输,减小空穴电流。另一方面从电荷平衡因子的角度,HML增强了电子的注入,使得器件的电荷平衡因子增大,空穴和电子的平衡性更好。实验研究表明,阴极杂化修饰层很好地增强了器件的效率。     

Electroluminescence study on electron hole plasma in strained SiGe epitaxial layers

The electroluminescence (EL) of thick fully strained SiGe layers is investigated in order to clarify the recombination mechanisms. In the investigated temperature range of 20–80 K and for SiGe thickness of 70–450 nm an electron–hole plasma (EHP) is observed even at low current densities of 1 Acm⁻². In SiGe-based quantum devices the EHP condition is expected to be attained at even lower injection levels. We used the band filling model for EHP to extract the renormalized gap of SiGe in dependence on the plasma density by performing a line shape analysis of EL spectra. The results were compared with the theoretical prediction. Based on this analysis as well as on measurements and modelling of the spectral photocurrent and the external quantum efficiency, we were able to evaluate parameters of recombination transitions for EHP in SiGe. Above 200 K there is an important contribution to EL from the silicon regions. For a better evaluation of the SiGe contribution, we compared EL of SiGe diodes with EL of pure silicon diodes.     

Low field DC investigation of hot carrier trapping in silicon dioxide films

The experimental method used in this work is based upon the idea of nonavalanche injection of carriers heated by direct electric field. The structure consisted of an n-channel MOS transistor and two p-n junctions. The process of charge injection in this structure was investigated by studying the dependence of gate current on heating voltage. The trapping properties of the SiO₂ film were studied by monitoring the charging of the film during injection of electrons. The capture cross-sections, the trap centre concentrations and the dependence of the capture cross section on the electric field for fields between 1 MV/cm and 2.5 MV/cm were determined.