The performance of solution-processed organic light emitting diodes (OLEDs) is often limited by non-uniform contacts. In this work, we introduce Ni-containing solution-processed metal oxide (MO) interfacial layers inserted between indium tin oxide (ITO) and poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) to improve the bottom electrode contact for OLEDs using the poly(p-phenylene vinylene) (PPV) derivative Super-Yellow (SY) as an emission layer. For ITO/Ni-containing MO/PEDOT:PSS bottom electrode structures we show enhanced wetting properties that result in an improved OLED device efficiency. Best performance is achieved using a Cu-Li co-doped spinel nickel cobaltite [(Cu-Li):NiCo2O4], for which the current efficiency and luminous efficacy of SY OLEDs increased, respectively, by 12% and 11% from the values obtained for standard devices without a Ni-containing MO interface modification between ITO and PEDOT:PSS. The enhanced performance was attributed to the improved morphology of PEDOT:PSS, which consequently increased the hole injection capability of the optimized ITO/(Cu-Li):NiCo2O4/PEDOT:PSS electrode.
As an attempt to further elucidate the operating voltage increase in InGaN-based light-emitting diodes (LEDs), the radiative and nonradiative current components are separately analyzed in combination with the Shockley diode equation. Through the analyses, we have shown that the increase in operating voltage is caused by phase space filling effect in high injection. We have also shown that the classical Shockley diode equation is insufficient to comprehensively explain the I-V curve of the LED devices since the transport and recombination characteristics of respective current components are bas…
In this work, performance and characteristics of AlGaN/AlGaN deep-ultraviolet light-emitting diodes (DUV LEDs) with varied number of quantum-well (QW) are investigated numerically. From our simulation, 1-QW structure give the best performance at low injection current. However, at higher injection current, 2-QWs structure give the largest power output due to its higher total radiative recombination rate and internal quantum efficiency (IQE) compared to other structures. The 2-QWs structure also has less serious efficiency droop at high current than 1-QW, which makes it an optimum structure for …
Carrier recombination and transport processes play key roles in determining the optoelectronic performances such as the efficiency droop and forward voltage in InGaN/GaN multiple-quantum-well (MQW) light-emitting diodes (LEDs). In this work, we investigate the dominant carrier transport and recombination processes inside and outside the MQW region as a function of injection current from a new point of view by separately examining the carrier energy loss. Analysis of the measurement results reveals that the carrier accumulation and subsequent spill-over from the MQW active region to the clad is…
Short wavelength ultraviolet (UV-C) light deactivates DNA of any germs, including multiresistive bacteria and viruses like COVID-19. Two-dimensional (2D) material-based UV-C light emitting diodes can potentially be integrated into arbitrary surfaces to allow for shadow-free surface disinfection. In this work, we perform a series of first-principles calculations to identify the core components of ultrathin LEDs based on hexagonal boron nitride (hBN). The electrons and holes are predicted to be confined in multiple quantum wells (MQWs) by combining hBN layers with different stacking orders. Vari…
Perovskite nanocrystal light-emitting diodes (LEDs) employing architecture comprising a ZnO nanoparticles electron-transport layer and a conjugated polymer hole-transport layer have been fabricated. The obtained LEDs demonstrate a maximum external-quantum-efficiency of 6.04%, luminance of 12998 Cd/m2 and stable electroluminescence at 519 nm. Importantly, such high efficiency and brightness have been achieved by employing solution processed transport layers, formamidinium lead bromide nanocrystals (CH(NH2)2PbBr3 NCs) synthesized at room-temperature and in air without the use of a Schlenk line, …
Organic Zener diodes with a precisely adjustable reverse breakdown from -3 V to -15 V without any influence on the forward current-voltage curve are realized. This is accomplished by controlling the width of the charge depletion zone in a pin-diode with an accuracy of one nanometer independently of the doping concentration and the thickness of the intrinsic layer. The breakdown effect with its exponential current voltage behavior and a weak temperature dependence is explained by a tunneling mechanism across the HOMO-LUMO gap of neigh- boring molecules. The experimental data are confirmed by a …
Based on the assumption that the contact barrier height determines the current flow in organic semiconductor-based electronic devices, charge injection at metal-organic (MO) interfaces has been extensively investigated, while space-charge conduction in organic bulk is generally overlooked. Recent theoretical modeling and simulation have pointed out that such a simplification is questionable due to the hopping nature of charge injection and hopping-related space-charge conduction. Here we show experimentally that charge transport in metal-organic diodes is complex interplay between injection-li…
Very thin (1.2-2.5nm) self-assembled organic dielectric monolayers have been integrated into organic thin-film diode to achieve electrical characteristics. These dielectrics are fabricated by self-assembling deposition, resulting in smooth, strongly adherent, thermally stable, organosiloxane thin films having interesting electrical capacitances (around 150 nF cm-2 at -3V) and insulating properties (leakage current densities around 10-5 A cm2 at -1V).
Carbene-metal-amide type photoemitters based on CF$_3$-substituted carbazolate ligands show sky-blue to deep-blue photoluminescence from charge-transfer excited states. They are suitable for incorporation into organic light-emitting diodes (OLEDs) by thermal vapour deposition techniques, either embedded within a high-triplet-energy host, or used host-free. We report high-efficiency OLEDs with emission ranging from yellow to blue (Commission Internationale de l'Éclairage (CIE) coordinates from [0.35, 0.53] to [0.17, 0.17]). The latter show a peak electroluminescence external quantum efficiency …
Spectroscopic Signature of Local Alloy Fluctuations in InGaN/GaN Multi-Quantum-Disk Light Emitting Diode Heterostructures and Its Impact on the Optical Performance
Blue light-emitting diodes (LEDs) consisting of a buried n+-p+ GaN tunnel junction, (In,Ga)N multiple quantum wells (MQWs) and a n+-GaN top layer are grown on single-crystal Ga-polar n+-GaN bulk wafers by plasma-assisted molecular beam epitaxy. The (In,Ga)N MQW active regions overgrown on the p+-GaN show chemically abrupt and sharp interfaces in a wide range of compositions and are seen to have high structural and optical properties as verified by X-ray diffraction and spatially resolved cathodoluminescence measurements. The processed LEDs reveal clear rectifying behavior with a low contact an…
Spin-spin interactions in organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) are pivotal because radiative recombination is largely determined by triplet-to-singlet conversion, also called reverse intersystem crossing (RISC). To explore the underlying process, we apply a spin-resonance spectral hole-burning technique to probe electroluminescence. We find that the triplet exciplex states in OLEDs are highly spin-polarized and show that these states can be decoupled from the heterogeneous nuclear environment as a source of spin dephasing and can even b…
Electrically Detected Magnetic Resonance (EDMR) was used to study a series of multilayer organic devices based on aluminum (III) 8-hydroxyquinoline. These devices were designed to identify the micoscopic origin of different spin dependent process, i.e. hopping and exciton formation. EDMR is demonstrated to probe molecular orbitals of charge, and thus indirectly explore interfaces, exciton formation, charge accumalation and electric fields in operating organic based devices.
The application of solution-processable graphene oxide (GO) as hole injection layer in organic light-emitting diodes (OLEDs) is demonstrated. High luminance of over 53,000 cd m-2 is obtained at only 10 V. The results will unlock a route of applying GO in flexible OLEDs and other electrode applications.
A self-consistent, mean-field model of charge-carrier injection and unipolar transport in an organic semiconductor diode is developed utilizing the effective transport energy concept and taking into account a realistic density-of-states distribution as well as the presence of trap states in an organic material. The consequences resulting from the model are discussed exemplarily on the basis of an indium tin oxide/organic semiconductor/metallic conductor structure. A comparison of the theory to experimental data of a unipolar indium tin oxide/poly-3-hexyl-thiophene/Al device is presented.
We investigate the charge-transfer interfaces between metal and redox arylamine molecular films through studying the current-voltage characteristics of single-layer organic diodes with the aid of anode interfacial engineering method. The diode turn-on voltage is shown to be highly sensitive to the arylamine/metal charge-transfer interfaces and thus can serve as a probe in detecting such organic/metal interfaces. We show that the diode electrical performance could be tuned through engineering the arylamine/metal interfaces via controlling the factors of anode work function, arylamine substitute…
We present a comprehensive model to analyze, quantitatively, and predict the process of degradation of organic light-emitting diodes (OLEDs) considering all possible degradation mechanisms, i.e., polaron, exciton, exciton-polaron interactions, exciton-exciton interactions, and a newly proposed impurity effect. The loss of efficiency during degradation is presented as a function of quencher density, the density and generation mechanisms of which were extracted using a voltage rise model. The comprehensive model was applied to stable blue phosphorescent OLEDs (PhOLEDs), and the results showed th…
We propose making light emitting diodes out of inverse spin valves. The proposed diodes rely on the spin-dependent electron transport of inverse spin valves that are layered structures of a ferromagnetic half-metal sandwiched between two non-magnetic metals. Under a bias, a giant spin-dependent chemical potential difference between spin-up and spin-down electrons is created. Thus, the inverse spin valves are possible to emit light when electrons in higher chemical potential go to the lower chemical potential. The advantages of this type of light emitting diodes include tunableness and less dem…
Singlet-polaron and triplet-polaron annihilation mechanisms are the most detrimental exciton quenching processes that lower the efficiency of organic light-emitting diodes (OLEDs) at high current densities, causing so-called efficiency roll-off in these devices. These exciton loss mechanisms are also the critical obstacles towards the realization of electrically pumped organic semiconductor lasers, which require very high current densities to reach threshold. Herein, under a relatively large external magnetic field, we demonstrate that the efficiency roll-off at high current densities in europ…
We have succeeded in growing ferromagnetic metals (Co, Fe, and NiFe)/ Al2O3/ AlGaAs heterostructures with homogeneous and flat interfaces. The electro-luminescence (EL) from the light emitting diode (LED) consisting of the metal/insulator/semiconductor (MIS) structure depends on the magnetization direction of the ferromagnetic electrode at room temperature. This fact shows that a spin-injection from the ferromagnetic metal to the semiconductor is achieved. The spin-injection efficiency is estimated to be the order of 1 % at room temperature.
Cavity polaritons have been shown these last years to exhibit a rich variety of non-linear behaviors which could be used in new polariton based devices. Operation in the strong coupling regime under electrical injection remains a key step toward a practical polariton device. We report here on the realization of a polariton based light emitting diode using a GaAs microcavity with doped Bragg mirrors. Both photocurrent and electroluminescence spectra are governed by cavity polaritons up to 100 K.
In this paper, we aim to understand the apparent characteristics of IQE and I-V curve in AlGaInP and InGaN LED devices. For the analysis, we separate the current into radiative current and non-radiative current component by using the information of IQE. We carefully analyze each current component by ideality factor, S parameter, and the modified Shockley diode equation which is suitable for LED device. Through the analyses, it has been found that the characteristics of respective current components are basically similar for both samples while the physical origin of the potential drop induced b…
The magnetic field effects on the carrier mobilities and recombination in tri-(8-hydroxyquinoline)-aluminum (Alq3) based light-emitting diodes have been measured by the method of transient electroluminescence. It is confirmed that the magnetic field has no effect on the electron and hole mobilities in Alq3 layers and can decrease the electron-hole recombination coefficient. The results imply that the dominant mechanism for the magnetic field effects in Alq3 based light-emitting diodes is the interconversion between singlet e-h pairs and triplet e-h pairs modulated by the magnetic field when th…
The present work is focused on theoretical and experimental study of localised levels in organic materials suitable for light-emitting devices and field effect transistors by means of thermal techniques. In our work we focused on low molecular compounds as well as on polymers, especially of two classes of materials: oxadiazoles and quinoxalines. Both organic compounds are well know as electron transport materials in OLEDs.
Despite widespread interest, ultrathin and highly flexible light-emitting devices that can be seamlessly integrated and used for flexible displays, wearables, and as bioimplants remain elusive. Organic light-emitting diodes (OLEDs) with $μ$m-scale thickness and exceptional flexibility have been demonstrated but show insufficient stability in air and moist environments due to a lack of suitable encapsulation barriers. Here, we demonstrate an efficient and stable OLED with a total thickness of $\approx$12 $μ$m that can be fully immersed in water or cell nutrient media for weeks without suffering…
The fabrication of single-carrier organic diodes from a series of sixteen molecular materials is reported. We experimentally demonstrate how the molecular structure affects the film morphology, and how the film morphology influences the diode performance. The compounds, with moderate molecular size and dendritic structures, are shown to be more favorable for good device performance than those small molecules with symmetry structures. The device turn-on voltage is found to be strongly dependent on the molecular first oxidation potentials. Independent of different anode materials, no obvious int…
The quantum efficiency of double hetero-junction light-emitting diodes (LEDs) can be significantly enhanced at low current density by tailoring the spatial profile of dopants to suppress Shockley-Read-Hall (SRH) recombination. To demonstrate this effect we model, design, grow, fabricate, and test a GaInAsP LED ($λ\approx$ 1330nm) with an unconventional dopant profile. Compared against that of our control design, which is a conventional $n^+$-$n$-$p^+$ double hetero-junction LED, the dopant profile near the $n$-$p^+$ hetero-structure of the new design displaces the built-in electric field in su…
Fabrication and optical characteristics of a spin light-emitting-diode (spin-LED) having dual spin-injection electrodes with anti-parallel magnetization configuration are reported. Alternating a current between the two electrodes using a PC-driven current source has led us to the observation of helicity switching of circular polarization at the frequency of 1 kHz. Neither external magnetic fields nor optical delay modulators were used. Sending dc-currents to both electrodes with appropriate ratio has resulted in continuous variation of circular polarization between the two opposite helicity, i…
The use of a thin mixed layer consisting of an inert diluent material and a light emitting material between the hole-transport layer and electron-transport layer of organic light-emitting diodes leads to an increase in the external quantum efficiency. The efficiency improvement is highly dependent on the thickness of the diluted light-emitting layer and driving current. Significant improvement seen at low current densities is explained in terms of effective hole confinement by the mixed layer while a modest decreases in efficiency at higher current densities may be attributed to luminescence q…
We report high luminance organic light-emitting diodes by use of acid functionalized multi-walled carbon nanotube (o-MWCNTs) as efficient hole injector electrodes with a simple and solution processable device structure. At only 10 V, the luminance can reach nearly 50,000 cd/m2 with an external quantum efficiency over 2% and a current efficiency greater than 21 cd/A. The investigation of hole-only devices shows that the mechanism for hole injection is changed from injection limited to bulk limited because of the higher effective work function of the anode modified by the o-MWCNTs. We expect the…
Electroluminescence in organic light emitting diode (OLED) materials occurs via the recombination of excitonic electrons-hole pairs Only the singlet excitons of commonly used OLED materials, e.g., Aluminum trihydroxyquinoline (AlQ$_3$), decay radiatively, limiting the external quantum efficiency to a maximum 25%. Thus 75% of the energy is lost due to the triplet bottleneck for radiative recombination. We consider molecules derived from AlQ$_3$ which bypass the triplet bottleneck by designing structures which contain strong spin-orbit coupling. As a first stage of this work, groundstate energie…
Concentration quenching is a major impediment to efficient organic light-emitting devices. We herein report on Organic Light-Emitting Diodes (OLEDs) based on a fluorescent amorphous red-emitting starbust triarylamine molecule (4-di(4'-tert-butylbiphenyl-4-yl)amino-4'-dicyanovinylbenzene, named FVIN), exhibiting a very small sensitivity to concentration quenching. OLEDs are fabricated with various doping levels of FVIN into Alq3, and show a remarkably stable external quantum efficiency of 1.5% for doping rates ranging from 5% up to 40%, which strongly relaxes the technological constraints on th…
White light emitting diodes based on III-nitride InGaN/GaN quantum wells currently offer the highest overall efficiency for solid state lighting applications. Although current phosphor-converted white LEDs have high electricity-to-light conversion efficiencies, it has been recently pointed out that the full potential of solid state lighting could be exploited only by color mixing approaches without employing phosphor-based wavelength conversion. Such an approach requires direct emitting LEDs of different colors, in particular in the green/yellow range ov the visible spectrum. This range, howev…
A numerical method based on the transfer matrix technique is developed to calculate the luminescence spectra of complex layered structures with photon recycling. Using this method we show a strong dependence of the emission spectra on the optical eigenmode structure of the device. The enhancement of the photon recycling and the LED external efficiency can be achieved by placing the active regions inside single or coupled microcavities.
In the present work we study the effect of nitrogen (N) and fluorine (F) doping in the electronic properties of ZrO$_2$ by using \emph{ab initio} electronic structure calculations. Our calculations show the importance of on-site Coulomb correlation in estimating the correct band gap of ZrO$_2$. The N and F doping provide hole and electron type impurity states in the band gap closer to the top of the valance band and bottom of the conduction band, respectively. The formation of such impurity states may be exploited in fabricating a $p$-$n$ junction expected to be useful in making an ultraviolet…
We investigate the effect of the p-type top contact on the optoelectronic characteristics of light emitting diodes (LEDs) based on (In,Ga)N/GaN nanowire (NW) ensembles grown by molecular beam epitaxy on Si substrates. We compare devices fabricated with either Ni/Au or indium tin oxide (ITO) top contact. The NW-LEDs with ITO exhibit a number density of NWs emitting electroluminescence about ten times higher, significantly lower turn-on voltage and series resistance, and a relative external quantum efficiency more than one order of magnitude higher than the sample with Ni/Au. These results show …
Planar light-emitting diodes (LEDs) fabricated within a single high-mobility quantum well are demonstrated. Our approach leads to a dramatic reduction of radiative lifetime and junction area with respect to conventional vertical LEDs, promising very high-frequency device operation. Devices were fabricated by UV lithography and wet chemical etching starting from p-type modulation-doped AlGaAs/GaAs heterostructures grown by molecular beam epitaxy. Electrical and optical measurements from room temperature down to 1.8 K show high spectral purity and high external efficiency. Time-resolved measurem…
The recombination of charges is an important process in organic photonic devices because the process influences the device characteristics such as the driving voltage, efficiency and lifetime. By combining the dipole trap theory with the drift-diffusion model, we report that the stationary dipole moment (μ0) of the dopant is a major factor determining the recombination mechanism in the dye-doped organic light emitting diodes when the trap depth (ΔEt) is larger than 0.3 eV where any de-trapping effect becomes negligible. Dopants with large μ0 (e.g., homoleptic Ir(III) dyes) induce large charge …
Detection of the degree of circular polarization of the electroluminescence of a light-emitting diode fitted with a spin injecting contact (a spin-LED) allows for a direct determination of the spin polarization of the injected carriers. Here, we compare the detection efficiency of (Al,Ga)As spin-LEDs fitted with a (Zn,Be,Mn)Se spin injector in top- and side-emission configuration. In contrast with top emission, we cannot detect the electrical spin injection in side emission from analysing the degree of circular polarization of the electroluminescence. To reduce resonant optical pumping of quan…
Quantifying the spin-spin interactions which influence electronic transitions in organic semiconductors is crucial for understanding their magneto-optoelectronic properties. By combining a theoretical model for three spin interactions in the coherent regime with pulsed electrically detected magnetic resonance experiments on MEH-PPV diodes, we quantify the spin-coupling within complexes comprising three spin-half particles. We determine that these particles form triplet-exciton:polaron pairs, where the polaron:exciton exchange is over 5 orders of magnitude weaker (less than 170 MHz) than that w…
Electrically driven single-photon emitting devices have immediate applications in quantum cryptography, quantum computation and single-photon metrology. Mature device fabrication protocols and the recent observations of single defect systems with quantum functionalities make silicon carbide (SiC) an ideal material to build such devices. Here, we demonstrate the fabrication of bright single photon emitting diodes. The electrically driven emitters display fully polarized output, superior photon statistics (with a count rate of $>$300 kHz), and stability in both continuous and pulsed modes, all a…
Polarization engineered interband tunnel junctions (TJs) are integrated in nanowire ultraviolet (UV) light emitting diodes (LEDs). A ~6V reduction in turn-on voltage is achieved by the integration of tunnel junction at the base of polarization doped nanowire UV LEDs. Moreover, efficient hole injection into the nanowire LEDs leads to suppressed efficiency droop in TJ integrated nanowire LEDs. The combination of both reduced bias voltage and increased hole injection increases the wall plug efficiency in these devices. More than 100 microwatts of UV emission at ~310 nm is measured with external q…
InGaN/GaN tunnel junction contacts were grown on top of an InGaN/GaN blue (450 nm) light emitting diode wafer using plasma assisted molecular beam epitaxy. The tunnel junction contacts enable low spreading resistance n-GaN top contact layer thereby requiring less top metal contact coverage on the surface. A voltage drop of 5.3 V at 100 mA, forward resistance of 2 x 10-2 ohm cm2 and a higher light output power are measured in tunnel junction LED. A low resistance of 5 x 10-4 ohm cm2 was measured in a MBE grown tunnel junction on GaN PN junction device, indicating that the tunnel junction LED de…
We report on the unambiguous detection of Auger electrons by electron emission spectroscopy from a cesiated InGaN/GaN light emitting diode (LED) under electrical injection. Electron emission spectra were measured as a function of the current injected in the device. The appearance of high energy electron peaks simultaneously with an observed drop in electroluminescence efficiency shows that hot carriers are being generated in the active region (InGaN quantum wells) by an Auger process. A linear correlation was measured between the high energy emitted electron current and the "droop current" - t…
we investigated the magneto-electroluminescence (MEL) in tri-(8-hydroxyquinoline)-aluminum based organic light-emitting diodes (OLEDs) through the steady-state and transient method simultaneously. The MELs show the great different behaviors when we turn the driving condition from a constant voltage to a pulse voltage. For devices driven by the constant voltage, the MELs are similar with the literature data; for devices driven by the pulse voltage, the MELs are quite different, they firstly increase to a maximum then decrease as the magnetic field increases continuously. Negative MELs can be se…
The low efficiency of metal halide perovskite light-emitting diodes (PeLEDs) with blue emission block their potential applications in large-area full-color displays and solid-state lighting. A delicate control over the entire electroluminescence process is indispensable to overcome the efficiency limitations of blue PeLEDs. Here, we demonstrate an efficient device architecture to synergistically reduce the energetic losses during electron-photon conversion and boost the extraction of trapped light in the device. An interfacial nucleation seeding scheme is proposed to control the crystallizatio…
p-Conjugated materials, including small molecules and polymers, are attracting substantial attention as novel gain media in semiconductor lasers; they offer many potential advantages not achievable with conventional inorganic semiconductors: simple processing, low cost, easy tuneability of the spectrum, and large-area integration on flexible substrates. Optically pumped lasing action in various small molecular and polymeric p-conjugated materials has been demonstrated using several resonator configurations. However, electrically pumped organic semiconductor lasers, i.e., organic injection or d…
The kinetics of the charge carrier recombination in dye molecule-doped multilayer organic light-emitting diodes (OLEDs) was quantified by transient electroluminescence (EL). Three sets of dye molecules, such as derivatives of naphthalimide and stilbene, were used as dopants in light-emission layer. Although the devices show almost the same EL spectra for each set of molecules, they show very different EL efficiency. The difference in EL efficiency was attributed to the difference in charge carrier recombination, as revealed by transient EL. The recombination coefficient (γ) was determined from…
White organic light-emitting diodes (OLEDs) are ultra-thin, large-area light sources made from organic semiconductor materials. Over the last decades, much research has been spent on finding the suitable materials to realize highly efficient monochrome and white OLEDs. With their high efficiency, color-tunability, and color-quality, white OLEDs are emerging to become one of the next generation light sources. In this review, we discuss the physics of a variety of device concepts that are introduced to realize white OLEDs based on both polymer and small molecule organic materi als. Owing to the …
We demonstrate highly efficient spin injection at low and room temperature in an AlGaAs/GaAs semiconductor heterostructure from a CoFe/AlOx tunnel spin injector. We use a double-step oxide deposition for the fabrication of a pinhole-free AlOx tunnel barrier. The measurements of the circular polarization of the electroluminescence in the Oblique Hanle Effect geometry reveal injected spin polarizations of at least 24% at 80K and 12% at room temperature.
This work reports our effort on understanding the efficiency roll-off in blue phosphorescent organic light-emitting diodes (OLEDs), based on a blue phosphorescence from bis(3,5-difluoro-2-(2-pyridyl)phenyl-(2-carboxypyridyl)- iridium (FIrpic) doped in 4,4-N,N-dicarbazole-biphenyl (CBP) host. The performance of a set of blue phosphorescent OLEDs with different FIrpic dopant concentrations was analyzed. Phosphorescent OLEDs, having a 30 nm thick pure FIrpic emissive layer, with a high luminous efficiency of 7.76 cd/A at 100 mA/cm2 was obtained. Theoretical calculation, based on the density funct…
