High-efficiency Light-emitting Diodes Research Articles

Acceleration of radiative recombination for efficient perovskite LEDs

The increasing demands for more efficient and brighter thin-film light-emitting diodes (LEDs) in flat-panel display and solid-state lighting applications have promoted research into three-dimensional (3D) perovskites. These materials exhibit high charge mobilities and low quantum efficiency droop1–6, making them promising candidates for achieving efficient LEDs with enhanced brightness. To improve the efficiency of LEDs, it is crucial to minimize nonradiative recombination while promoting radiative recombination. Various passivation strategies have been used to reduce defect densities in 3D perovskite films, approaching levels close to those of single crystals3. However, the slow radiative (bimolecular) recombination has limited the photoluminescence quantum efficiencies (PLQEs) of 3D perovskites to less than 80% (refs. 1,3), resulting in external quantum efficiencies (EQEs) of LED devices of less than 25%. Here we present a dual-additive crystallization method that enables the formation of highly efficient 3D perovskites, achieving an exceptional PLQE of 96%. This approach promotes the formation of tetragonal FAPbI3 perovskite, known for its high exciton binding energy, which effectively accelerates the radiative recombination. As a result, we achieve perovskite LEDs with a record peak EQE of 32.0%, with the efficiency remaining greater than 30.0% even at a high current density of 100 mA cm−2. These findings provide valuable insights for advancing the development of high-efficiency and high-brightness perovskite LEDs.

Efficient Perovskite Nanograin Light-Emitting Diodes in Green-to-Blue Gamut with Co-Additive Engineering.

Perovskite nanograins exceeding the Bohr exciton diameter show great potential for high-performance light-emitting diodes (LEDs) owing to their bandgap homogeneity, spatial charge confinement, and nonlocal interaction. However, it is challenging to directly synthesize proper nanograins along with reduced crystal defects on functional substrate, and the corresponding high-efficiency perovskite LEDs (PeLEDs) have rarely been reported. In this study, crystallization modulation for perovskites with an effective co-additive system, including lithium bromide, p-fluorophenethylammonium bromide, and 18-crown-6, is performed. Furthermore, it is demonstrated that the proposed co-additive system can synergistically retard perovskite crystallization and reduce crystal defects. Consequently, high-quality perovskite nanograin solids (≈22.8nm) are obtained with a high photoluminescence quantum yield (≈88%). These superior optical properties contribute to developing efficient green PeLEDs with a champion external quantum efficiency (EQE) of 28.4% and an average EQE of 27.1%. The co-additive system can be universally applied to mixed-halide perovskite nanograin LED, presenting a maximum EQE of 24.4%, 21.6%, 17.5%, and 11.1% for the blue device at 496, 488, 478, and 472nm, respectively, along with a narrow spectral linewidth (17-14nm) and stable color. These results supplement the research on high-efficiency perovskite nanograin LEDs for multicolor displays and lighting.

High-Efficiency Pure-Red CsPbI3 Quantum Dot Light-Emitting Diodes Enabled by Strongly Electrostatic Potential Solvent and Sequential Ligand Post-treatment Process.

Efficient pure-red emission light-emitting diodes (LEDs) are essential for high-definition displays, yet achieving pure-red emission is hindered by challenges like phase segregation and spectral instability when using halide mixing. Additionally, strongly confined quantum dots (QDs) produced through traditional hot-injection methods face byproduct contamination due to poor solubility of metal halide salts in the solvent octadecene (ODE) at low temperatures. Herein, we introduced a novel method using a benzene-series strongly electrostatic potential solvent instead of ODE to prevent PbI2 intermediates and promote their dissolution into [PbI3]-. Increasing methyl groups on benzene yields precisely sized (4.4 ± 0.1 nm) CsPbI3 QDs with exceptional properties: a narrow 630 nm PL peak with photoluminescence quantum yield (PLQY) of 97%. Sequential ligand post-treatment optimizes optical and electrical performance of QDs. PeLEDs based on optimized QDs achieve pure-red EL (CIE: 0.700, 0.290) approaching Rec. 2020 standards, with an EQE of 25.2% and T50 of 120 min at initial luminance of 107 cd/m2.

High-efficiency InGaN red light-emitting diodes with external quantum efficiency of 10.5% using extended quantum well structure with AlGaN interlayers

In this study, we have demonstrated a high-efficiency InGaN red (625 nm) light-emitting diode (LED) with an external quantum efficiency (EQE) of 10.5% at a current density of 10 A/cm2. To achieve this, we introduced GaN cap layers on InGaN quantum wells and AlGaN interlayers. The introduction of these layers resulted in a red shift of the wavelength. The AlGaN interlayer caused band bending, while the GaN cap layer modulated the electron wavefunction, thus helping to achieve the wavelength red shift of the InGaN red LED with high EQE. This technology is crucial for the realization of discrete or monolithic full-color micro-LED displays.

Investigation into the Effects of Cross-Sectional Shape and Size on the Light-Extraction Efficiency of GaN-Based Blue Nanorod Light-Emitting Diode Structures

We investigated the effect of cross-sectional shape and size on the light-extraction efficiency (LEE) of GaN-based blue nanorod light-emitting diode (LED) structures using numerical simulations based on finite-difference time-domain methods. For accurate determination, the LEE and far-field pattern (FFP) were evaluated by averaging them over emission spectra, polarization, and source positions inside the nanorod. The LEE decreased as rod size increased, owing to the nanorods’ increased ratio of cross-sectional area to sidewall area. We compared circular, square, triangular, and hexagonal cross-sectional shapes in this study. To date, nanorod LEDs with circular cross sections have been mainly demonstrated experimentally. However, circular shapes were found to show the lowest LEE, which is attributed to the coupling with whispering-gallery modes. For the total emission of the nanorod, the triangular cross section exhibited the highest LEE. When the angular dependence of the LEE was calculated using the FFP simulation results, the triangular and hexagonal shapes showed relatively high LEEs for direction emission. The simulation results presented in this study are expected to be useful in designing high-efficiency nanorod LED structures with optimum nanorod shape and dimensions.

Partial Ligand Stripping from CsPbBr3 Nanocrystals Improves Their Performance in Light-Emitting Diodes.

Halide perovskite nanocrystals (NCs), specifically CsPbBr3, have attracted considerable interest due to their remarkable optical properties for optoelectronic devices. To achieve high-efficiency light-emitting diodes (LEDs) based on CsPbBr3 nanocrystals (NCs), it is crucial to optimize both their photoluminescence quantum yield (PLQY) and carrier transport properties when they are deposited to form films on substrates. While the exchange of native ligands with didodecyl dimethylammonium bromide (DDAB) ligand pairs has been successful in boosting their PLQY, dense DDAB coverage on the surface of NCs should impede carrier transport and limit device efficiency. Following our previous work, here, we use oleyl phosphonic acid (OLPA) as a selective stripping agent to remove a fraction of DDAB from the NC surface and demonstrate that such stripping enhances carrier transport while maintaining a high PLQY. Through systematic optimization of OLPA dosage, we significantly improve the performance of CsPbBr3 LEDs, achieving a maximum external quantum efficiency (EQE) of 15.1% at 516 nm and a maximum brightness of 5931 cd m-2. These findings underscore the potential of controlled ligand stripping to enhance the performance of CsPbBr3 NC-based optoelectronic devices.

Investigation of emission plane control in GaInN/GaN multiple-quantum shells for efficient nanowire-based LEDs.

Significant attention has been directed toward core-shell GaInN/GaN multiple-quantum shell (MQS) nanowires (NWs) in the context of high-efficiency micro light-emitting diodes (micro-LEDs). These independent three-dimensional NWs offer the advantage of reducing the impact of sidewall etching regions. Furthermore, the emitting plane on the sidewalls demonstrates either nonpolar or semipolar orientation, while the dislocation density is exceptionally low. In this study, we assessed how changes in the NW morphology are affected by GaInN/GaN superlattice (SL) structures grown at varying growth temperatures, as well as control of the emission plane via the p-GaN shell and emission sizes. The SL growth rate was enhanced at elevated growth temperatures, accompanied by the shrinkage of the (0001)-plane and expansion of the (11̄01)-plane on the NWs. The samples exhibited a higher light output when the SLs were grown at elevated temperatures compared to those grown with lower temperatures. A similar trend was observed for the samples with a gradual temperature transition during the growth. These findings indicate that the dimensions of the (0001)-plane can be controlled through SL growth, which in turn influences the emission properties of NW-LEDs. In addition, the emission properties of NW-LEDs with different growth time p-GaN shells and different emission sizes were investigated. Based on the NW-LED characteristics, it was revealed that the weak emission of the (0001)-plane was the dominant factor for the limited light output, and the most effective way to realize high efficiency devices is to suppress current injection into the apex or minimize the grown (0001)-plane region. Overall, it is one promising way to control the emission planes of NWs, which holds significant relevance for the potential application of NW-LEDs in the realm of micro-LEDs.

Unveiling the luminescence property of Li2MgGeO4:Mn4+ featuring the tetrahedral crystallographic-site occupancy of Mn4.

Owing to the occupying tendency of Mn4+ at octahedral sites, doping Mn4+ activators in tetrahedral structures poses challenges and hence is seldom reported. In this work, tetrahedrally sited Mn4+ phosphors were studied. By combining X-ray diffraction (XRD) data with Rietveld refinement analysis, the location of Mn4+ was determined. It was found that by adding excessive raw MgO, the phosphor synthesis temperature can be improved, enhancing the crystallinity of the crystal and thus improving the emission performance of the phosphor. In addition, excessive raw MgO forms a second phase in an LMGO matrix, which does not change the doping site for Mn4+. The Tanabe-Sugano diagram of Mn4+ in the tetrahedral field and the energy-level diagram of these phosphors were constructed for the first time, and the excitation and emission mechanisms are discussed in detail. With 1.2-fold excess of raw MgO, the prepared sample (LMGO-Mn-1.2) shows the best luminescence, demonstrating red emissions peaked at 656 nm and affording an emission intensity enhancement of over 50 times compared to a stoichiometric LMGO:Mn4+ system. At 150 °C, LMGO-Mn-1.2 keeps 90% emission intensity compared to that at room temperature. Finally, a high-efficiency warm white light-emitting diode was built. This work provides new insights into the study of Mn4+-activated phosphors in a tetrahedron crystal field.

Phase distribution management for high-efficiency and bright blue perovskite light-emitting diodes

Quasi-two-dimensional (quasi-2D) perovskite materials have attracted significant attention for application in light-emitting diodes (PeLEDs) due to their unique optical characteristics and extraordinary performance. The inherent multi-quantum well structure will generate a strong quantum confinement effect which is beneficial for the blue emission. However, the efficiency and stability of the quasi-2D blue PeLEDs lag behind their red and green counterparts, which prevents the further commercial application of the PeLEDs. The performance of quasi-2D blue PeLEDs was limited on account of the inefficient phase distribution management, which causes an inefficient energy transfer and severe non-radiative recombination. Herein, we employ guanidine thiocyanate (GASCN) as the pre-deposited film at the bottom of the perovskite film to manage the phase distribution of the PBA2Csn−1PbnBr3n+1 quasi-2D perovskite film (where n is the number of [PbBr6]4- sheets, and PBA is phenylbutylammonium). The pre-deposited GASCN can not only inhibit the small n-phase (i.e., n = 1: PBA2PbBr4, and n = 2: PBA2CsPb2Br7) but also avoid the undesired emission redshift from the over-growth of the large n-phase as well as passivate defects of the quasi-2D perovskite film, which accelerates energy transfer efficiently, strengthens the carrier transport, and enhances the luminous efficiency. As a result, the optimized device demonstrated the highest external quantum efficiency (EQE) of 16.40% and a maximum luminance of 8290 cd m−2. This strategy provides a new pathway to accurately manage phase distribution of quasi-2D perovskite achieving the high efficiency in blue PeLEDs.

Advanced Design of a III‐Nitride Light‐Emitting Diode via Machine Learning

AbstractGallium nitride (GaN)‐based light‐emitting diodes (LEDs) have obtained great market success in the past 20 years. However, the traditional research paradigm, i.e., experimental trial‐and‐error method, no longer adapts to the industry development. In this work, an efficient approach is demonstrated to design and optimize GaN‐based LED structures via machine learning (ML). By using the dataset of GaN‐based LED structures over the past decade to train four typical ML models, it is found that the convolutional neural network (CNN) provides the most accurate prediction, with a root mean square error (RMSE) of 1.03% for internal quantum efficiency (IQE) and 11.98 W cm−2 for light output power density (LOPD). Based on the CNN model, 1) the feature importance analysis is adopted to reveal the critical features for LED performance; 2) the predicted trends of IQE and LOPD match well with the physical mechanism, being consistent with the experimental and simulation results; and 3) a high‐throughput screening is demonstrated to predict the properties of over 20 000 structures within seconds to obtain high efficiency LED structures. This ML‐based LED design method enables direct guiding of the LED structure optimization in terms of key parameter selection during manufacturing and greatly accelerates the development cycle of GaN‐based LEDs.

Charge injection engineering at organic/inorganic heterointerfaces for high-efficiency and fast-response perovskite light-emitting diodes

The development of advanced perovskite emitters has considerably improved the performance of perovskite light-emitting diodes (LEDs). However, the further development of perovskite LEDs requires ideal device electrical properties, which strongly depend on its interfaces. In perovskite LEDs with conventional p-i-n structures, hole injection is generally less efficient than electron injection, causing charge imbalance. Furthermore, the popular hole injection structure of NiOx/poly(9-vinylcarbazole) suffers from several issues, such as weak interfacial adhesion, high interfacial trap density and mismatched energy levels. In this work, we insert a self-assembled monolayer of [2-(9H-carbazol-9-yl)ethyl]phosphonic acid between the NiOx and poly(9-vinylcarbazole) layers to overcome these challenges at the organic/inorganic heterointerfaces by establishing a robust interface, passivating interfacial trap states and aligning the energy levels. We successfully demonstrate blue (emission at 493 nm) and green (emission at 515 nm) devices with external quantum efficiencies of 14.5% and 26.0%, respectively. More importantly, the self-assembled monolayer also gives rise to devices with much faster response speeds by reducing interfacial capacitance and resistance. Our results pave the way for developing more efficient and brighter perovskite LEDs with quick response, widening their potential application scope.

Dual-functionalized poly(ethylene oxide) for interface modification and addition of rubidium-doped CsPbBr3 perovskite composite emission layer to enhance brightness of perovskite light-emitting diodes

Metal halide perovskite as an emitter has extremely high color purity, but the generally poor morphology of the perovskite layer restricts the performance of the emitter. The additive of a suitable polymer can greatly boost the uniformity of the spin-coated perovskite film. The all-inorganic perovskite layer deposited by the solution method has a multi-crystalline structure. Besides, there are a lot of defects and grain boundaries on the surface, and the carriers will undergo non-radiative recombination at these defects. In this study, Cs1-xRbxPbBr3 was prepared by introducing Rb+ cations with smaller ionic radius to partially replace Cs+ cations, and combined with poly(ethylene oxide) (PEO) and (1,3,5-benzinetriyl)tris(1-phenyl-1-H-benzimidazole) (TPBi) blended composite film as the light-emitting layer, that can increase the film coverage and radiative recombination efficiency of the perovskite film. The polymer PEO was introduced as a buffer layer deposited on the poly-TPD hole transport layer (HTL) to to enhance the hydrophilicity and passivate the poly-TPD HTL/perovskites interface in order to obtain high-efficiency perovskite light-emitting diodes. By adjusting the concentration of the PEO buffer layer, the champion luminance and external quantum efficiency are 25650 cd/m2 and 0.844 %, respectively.

High-Efficiency and Emission-Tunable Inorganic Blue Perovskite Light-Emitting Diodes Based on Vacuum Deposition.

The fabrication of perovskite light-emitting diodes (PeLEDs) with vacuum deposition shows great potential and commercial value in realizing large-area display panel manufacturing. However, the electroluminescence (EL) performance of vacuum-deposited PeLEDs still lags behind the counterparts fabricated by solution process, especially in the field of blue PeLEDs. Here, the fabrication of high-quality CsPbBr3- x Clx film through tri-source co-evaporation is reported to achieve high photoluminescence quantum yield (PLQY). Compared with the conventional traditional dual-source co-evaporation, the tri-source co-evaporation method allows for freely adjustable elemental ratios, enabling the introduction of the lattice-matched Cs4 Pb(Br/Cl)6 phase with the quantum-limited effect into the inorganic CsPb(Br/Cl)3 emitter. By adjusting the phase distribution, the surface defects of the emitter can be effectively reduced, leading to better blue emission and film quality. Further, the effects of Cs/Pb ratio and Br/Cl ratio on the PLQY and carrier recombination dynamics of perovskite films are investigated. By optimizing the deposition rate of each precursor source, spectrally stable blue PeLEDs are achieved with tunable emission ranging from 468 to 488nm. Particularly, the PeLEDs with an EL peak at 488nm show an external quantum efficiency (EQE) of 4.56%, which is the highest EQE value for mixed-halide PeLEDs fabricated by vacuum deposition.

Photophysical dynamics of excitons in polyaniline nanotubes with enhanced resistance against exciton quenching for applications in flexible high-efficiency PLEDs

The development of a high-efficiency polymer light-emitting diode is strongly hindered by injected charge carriers in the emissive polymer layer. But real-time identification of the interactions that quench the photoluminescence is extremely difficult owing to the complex photophysics of polymers involved in it. Here, we have synthesized the polyaniline nanotubes to study interactions at the nanoscale within the emissive layer. Acid doping of PAni helped us to quantify the processes that suppress the emission, e.g., Förster resonance energy transfer (FRET) and charge transfer (CT). We have developed a material design perspective by demonstrating how an effective increase in conjugation length of PAni nanochain through 1D nanostructure growth can avoid the undesired emission quenching due to exciton quenching by the polarons. We have demonstrated how this approach helped us to preserve up to 95 % of the emission, which would otherwise be lost by exciton-polaron quenching interaction. Exploration of this new strategy could be a way forward for both fundamental and application aspects to enhance the emission efficiency of the conducting conjugate polymers and emissive layers in flexible polymer light-emitting diodes (PLEDs).

Dual-function ligand surface control to achieve high efficiency and brightness perovskite quantum dots LED devices

Metal halide perovskite quantum dots (QDs) have significant potential for application in light-emitting diodes (LED) owing to their superior optical properties. However, the dynamic instability of traditional oleic acid/amine ligands has a considerable impact on the optical and chemical properties of the surface. Additionally, one of its insulating qualities restricts the practical application of electroluminescent devices. In this case, the dual-function ligand DDA-MeS can passivate surface defects while also stabilizing chelation on QDs surface. As a result, the electrical performance of green QDs-LED devices is greatly enhanced, the external quantum efficiency is raised to 10.18%, the maximum brightness is also boosted to 8025 cd/m2, and the turn-on voltage is decreased to 2.5 V. This work also provides a novel strategy for the development of green LED devices with dual-function ligands that can be highly effective and bright.

High External Quantum Efficiency Light-Emitting Diodes Enabled by Advanced Heterostructures of Type-II Nanoplatelets

Colloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts. Unlike traditional type-II NPLs such as CdSe/CdTe, CdTe/CdSe, and CdSe/CdSexTe1-x core/crown heterostructures, here the proposed advanced heterostructure reaps the benefits of having two type-II transition channels, resulting in a high quantum yield (QY) of 83% and a long fluorescence lifetime of 73.3 ns. These type-II transitions were confirmed experimentally by optical measurements and theoretically using electron and hole wave function modeling. Computational study shows that the multi-crowned NPLs provide a better-distributed hole wave function along the CdTe crown, while the electron wave function is delocalized in the CdSe core and CdSe crown layers. As a proof-of-concept demonstration, NPL-LEDs based on these multi-crowned NPLs were designed and fabricated with a record high external quantum efficiency (EQE) of 7.83% among type-II NPL-LEDs. These findings are expected to induce advanced designs of NPL heterostructures to reach a fascinating level of performance, especially in LEDs and lasers.

High Color-Purity and Efficient Pure-Blue Perovskite Light-Emitting Diodes Based on Strongly Confined Monodispersed Quantum Dots.

Here, we develop an in situ photoluminescence (PL) system to monitor the nucleation and growth of perovskite nanocrystals and control the monomer supply rate to achieve strongly confined and monodispersed quantum dots (QDs) with average size of 3.4 nm. Pure-blue (460 nm wavelength) CsPbBr3 QDs with near unity PL quantum yield and narrow size distribution (small size dispersion of 9.6%) were thus produced. Light-emitting diodes (LEDs) based on these QDs were prepared by using an all-solution processing route, which showed narrow electroluminescence with full width at half-maximum of 20 nm and a high color purity of 97.3%. The device also had a high external quantum efficiency of 10.1%, maximum luminance of 11 610 cd m-2, and continuous operation lifetime of 21 h at the initial luminance of 102 cd m-2, corresponding to the state-of-art for pure-blue perovskite LEDs.

Enhancing light extraction efficiency of GaN-based light-emitting diodes with reticulated photonic crystals

We have proposed reticulated photonic crystals (PhCs) on the top surface of conventional light-emitting diodes (LEDs) to increase the light extraction efficiency (LEE). The rigorous electromagnetic simulations based on the three-dimensional finite-difference time-domain method were carried out to investigate the optical properties of reticulated PhCs LEDs and mechanisms of reticulated PhCs improving the LEE of LEDs. Results from these simulations showed that more than 115% enhancement of LEE had been achieved for LEDs with reticulated PhCs period of 200 nm and depth of 200 nm. This study provides an innovative approach to the creation of high-efficiency LEDs of the upcoming generation.

Structure of V-defects in long wavelength GaN-based light emitting diodes

The V-defect is a naturally occurring inverted hexagonal pyramid structure that has been studied in GaN and InGaN growth since the 1990s. Strategic use of V-defects in pre-quantum well superlattices or equivalent preparation layers has enabled record breaking efficiencies for green, yellow, and red InGaN light emitting diodes (LEDs) utilizing lateral injection of holes through the semi-polar sidewalls of the V-defects. In this article, we use advanced characterization techniques such as scattering contrast transmission electron microscopy, high angle annular dark field scanning transmission electron microscopy, x-ray fluorescence maps, and atom probe tomography to study the active region compositions, V-defect formation, and V-defect structure in green and red LEDs grown on (0001) patterned sapphire and (111) Si substrates. We identify two distinct types of V-defects. The “large” V-defects are those that form in the pre-well superlattice and promote hole injection, usually nucleating on mixed (Burgers vector b=±a±c) character threading dislocations. In addition, “small” V-defects often form in the multi-quantum well region and are believed to be deleterious to high-efficiency LEDs by providing non-radiative pathways. The small V-defects are often associated with basal plane stacking faults or stacking fault boxes. Furthermore, we show through scattering contrast transmission electron microscopy that during V-defect filling, the threading dislocation, which runs up the center of the V-defect, will “bend” onto one of the six {101¯1} semi-polar planes. This result is essential to understanding non-radiative recombination in V-defect engineered LEDs.

Efficient and Bright Deep-Red Light-Emitting Diodes based on a Lateral 0D/3D Perovskite Heterostructure.

Bright and efficient deep-red light-emitting diodes (LEDs) are important for applications in medical therapy and biological imaging due to the high penetration of deep-red photons into human tissues. Metal-halide perovskites have potential to achieve bright and efficient electroluminescence due to their favorable optoelectronic properties. However, efficient and bright perovskite-based deep-red LEDs have not been achieved yet, due to either Auger recombination in low-dimensional perovskites or trap-assisted nonradiative recombination in 3D perovskites. Here, a lateral Cs4PbI6/FAxCs1- xPbI3 (0D/3D) heterostructure that can enable efficient deep-red perovskite LEDs at very high brightnessis demonstrated. The Cs4PbI6 can facilitate the growth of low-defect FAxCs1- xPbI3, and act as low-refractive-index grids, which can simultaneously reduce nonradiative recombination and enhance light extraction. This device reaches a peak external quantum efficiency of 21.0% at a photon flux of 1.75×1021 m-2 s-1, which is almost two orders of magnitude higher than that of reported high-efficiency deep-red perovskite LEDs. Theses LEDs are suitable for pulse oximeters, showing an error <2% of blood oxygen saturation compared with commercial oximeters.