Efficient Light-emitting Diodes Research Articles

Controlled phase distribution of quasi-2D perovskite enables improved electroluminescence

Quasi-two-dimensional (quasi-2D) perovskites are increasingly explored for integration into light-emitting diodes (LEDs) as light-emissive layers. However, the quasi-2D perovskite films likely exhibit non-uniform dimensional phase distribution and irregular internal crystal structures. These characteristics are known to contribute to undesirable effects, including non-radiative recombination losses and radiative recombination in perovskites of various dimensions, impeding the realization of efficient electroluminescence and high color purity in LEDs. In this study, we present an investigation on the correlation between the dimensional distribution of quasi-2D perovskites and charge carrier behavior by modulating anti-solvent dripping during the film fabrication processes. We provide a comprehensive analysis of the impact of controlled dimensional distribution on charge injection and recombination processes associated with the performance of quasi-2D perovskite LEDs. Our work emphasizes the crucial role played by controlled dimensionality in quasi-2D perovskites in realizing efficient and stable perovskite-based LEDs.

Enhanced Efficiency and Stability of Sky Blue Perovskite Light-Emitting Diodes via Introducing Lead Acetate

Enhanced Efficiency and Stability of Sky Blue Perovskite Light-Emitting Diodes via Introducing Lead Acetate

Strategically constructed AlGaN doping barriers for efficient deep ultraviolet light-emitting diodes: erratum

We present an erratum to our Letter [Opt. Lett. 49, 2049 (2024)10.1364/OL.522212]. There is a careless omission of some references because our Letter is longer than the maximum allowed four pages. The missing references and their specific quote location are listed in the following. These corrections do not affect the data plotted in figures, discussion, or conclusion of the original Letter.

Efficient Large-Area (81 cm2) Ternary Copper Halides Light-Emitting Diodes with External Quantum Efficiency Exceeding 13% via Host-Guest Strategy.

Ternary copper (Cu) halides are promising candidates for replacing toxic lead halides in the field of perovskite light-emitting diodes (LEDs) toward practical applications. However, the electroluminescent performance of Cu halide-based LEDs remains a great challenge due to the presence of serious nonradiative recombination and inefficient charge transport in Cu halide emitters. Here, the rational design of host-guest [dppb]2Cu2I2 (dppb denotes 1,2-bis[diphenylphosphino]benzene) emitters and its utility in fabricating efficient Cu halide-based green LEDs that show a high external quantum efficiency (EQE) of 13.39% are reported. The host-guest [dppb]2Cu2I2 emitters with mCP (1,3-bis(N-carbazolyl)benzene) host demonstrate a significant improvement of carrier radiative recombination efficiency, with the photoluminescence quantum yield increased by nearly ten times, which is rooted in the efficient energy transfer and type-I energy level alignment between [dppb]2Cu2I2 and mCP. Moreover, the charge-transporting mCP host can raise the carrier mobility of [dppb]2Cu2I2 films, thereby enhancing the charge transport and recombination. More importantly, this strategy enables a large-area prototype LED with a record-breaking area up to 81 cm2, along with a decent EQE of 10.02% and uniform luminance. It is believed these results represent an encouraging stepping stone to bring Cu halide-based LEDs from the laboratory toward commercial lighting and display panels.

Blue Lead‐Free Perovskite Derivatives: Structural Diversity, Luminescence Properties and Light‐Emitting Diode Applications

AbstractHalide perovskite light‐emitting diodes (LEDs) have made remarkable advancements in both efficiency and stability. However, when compared to green and red LEDs, blue perovskite LEDs still lag behind in terms of efficiency and stability. Presently, efficient blue LEDs primarily rely on lead‐based perovskites, which goes against the environmentally friendly practices and restricts potential industrial applications. Consequently, there has been a surge of interest in academic research toward developing blue LEDs using lead‐free perovskites. This paper provides a comprehensive review of the structural diversity of lead‐free perovskite derivatives used for blue emission, encompassing Sn‐, Zr‐, Bi‐, Sb‐, Cu‐, Zn‐based halides as well as double perovskites. Various material synthesis techniques are discussed, such as nanocrystal preparation and film preparation. Additionally, the photoluminescence properties for different energy band structures are outlined, along with the luminescence mechanism involving energy transfer and strategies for enhancing luminous efficiency. The advancement in efficiency and stability of lead‐free perovskite LEDs is also examined in this review. Finally, the current challenges and future opportunities in advancing research on blue lead‐free perovskite derivatives and their potential application in LED technology is emphasized.

Efficient Green Spin Light-Emitting Diodes Enabled by Ultrafast Energy- and Spin-Funneling in Chiral Perovskites.

Introducing molecular chirality into perovskite crystal structures has enabled the control of carrier spin states, giving rise to circularly polarized luminescence (CPL) in thin films and circularly polarized electroluminescence (CPEL) in LEDs. Spin-LEDs can be fabricated either through a spin-filtering layer enabled by chiral-induced spin selectivity or a chiral emissive layer. The former requires a high degree of spin polarization and a compatible spinterface for efficient spin injection, which might not be easily integrated into LEDs. Alternatively, a chiral emissive layer can also generate circularly polarized electroluminescence, but the efficiency remains low and the fundamental mechanism is elusive. In this work, we report an efficient green LED based on quasi-two-dimensional (quasi-2D) chiral perovskites as the emitting layer (EML), where CPEL is directly produced without separate carrier spin injection. The optimized chiral perovskite thin films exhibited strong CPL at 535 nm with a photoluminescence quantum yield (PLQY) of 91% and a photoluminescence dissymmetry factor (glum) of 8.6 × 10-2. Efficient green spin-LEDs were successfully demonstrated, with a large EL dissymmetry factor (gEL) of 7.8 × 10-2 and a maximum external quantum efficiency (EQE) of 13.5% at room temperature. Ultrafast transient absorption (TA) spectroscopic study shows that the CPEL is generated from a rapid energy transfer accompanied by spin transfer from 2D to 3D perovskites. Our study not only demonstrates a reliable approach to achieve high performance spin-LEDs but also reveals the fundamental mechanism of CPEL with an emissive layer of chiral perovskites.

Microcavity enhancement vs Auger recombination in variable thickness type-II superlattices in resonant cavity mid-infrared light emitting diodes

In this study, we investigate the tradespace between the improvement of mid-infrared light-emitting diode efficiency through microcavity enhancement vs reduction of Auger recombination for different W-superlattice thicknesses. Several sample designs are modeled and then grown and fabricated to test the tradespace at different W-superlattice thicknesses down to the quantum well limit. In a half-cavity, with a single reflector from the top metal contact, intermediate thickness W-superlattices gave the highest efficiencies, outperforming those in the W-quantum well limit across the entire measured current range. Experimentally, we report wallplug efficiencies of 0.4% for a room temperature 3.2 μm device. W-superlattices of intermediate thickness were also found to be optimal for a full-cavity device with a bottom distributed Bragg reflector added. The resonant full cavity did strongly improve the peak spectral radiance, with a measured increase of four to five times for a 3.6 μm device, and a value that is >250 times larger than previously reported.

Exploration of the optical characteristics in sol-gel synthesized europium-doped zinc oxide thin films for potential optoelectronic use: a comprehensive characterization approach

Abstract In this study, we present our findings on the spin coated pure Zinc-Oxide (ZnO) nanowire arrays and Europium doped ZnO (Eu3+: ZnO) nanostructure thin films. These arrays were grown on soda lime (silica) coated glass substrate. We conducted a comprehensive analysis of the structural and optical properties of the as-synthesized nanostructures. The characterization techniques included x-ray Diffraction, FESEM Analysis, Raman Spectroscopy, Photoluminescence and UV–vis Analysis. The XRD findings indicate the incorporation of Europium (Eu3+) into the ZnO crystalline lattice, potentially replacing Zn2+ ions. This doping with Europium (Eu3+) led to a reduction in crystalline size, as determined by Scherrer’s equation decreasing from 48 nm to 28 nm demonstrates a decrease in defects within the films. Raman Shift analysis revealed changes in the optical properties of films with inclusion of Europium in host matrix. Photoluminescence studies demonstrated a distinctive 5D0 to 7F2 transition arising from the Eu3+ ions, observed at approximately 612 nm. We have thoroughly examined the optical characteristics of both Europium-doped and pure ZnO thin films through a systematic study. The optical properties were assessed by analyzing the absorption spectra (220–600 nm) and transmission spectra within the wavelength range of 200 to 1200 nm. The film exhibited an impressive 80% transparency, particularly noteworthy for window layer application. The refractive index (n), extinction coefficient (k) and all other associated parameters were found to be impacted by the doping of Europium. The refractive index dispersion relation has been explored using a single oscillator model. Furthermore, the non-linear optical susceptibility (χ 3) and non-linear refractive index were computed using semi-empirical relationships based on the linear optical parameters. The Europium (Eu3+) doping in ZnO led to an increase in the χ 3 value elevating it from 4.07 × 10–1° to 5.91 × 10–1° e.s.u. These findings suggest that Europium-doped ZnO nanostructures have the potential to be a promising platform for the development of efficient multispectral light-emitting diodes (LED’s) and optical devices.

Efficient pure-red perovskite light-emitting diodes with strong passivation via ultrasmall-sized molecules.

Perovskite light-emitting diodes (PeLEDs) have attracted great attention in recent years; however, the halogen vacancy defects in perovskite notably hamper the development of high-efficiency devices. Previously, large-sized passivation agents have been usually used, while the effect of defect passivation is limited due to the weak bonding or the large space steric hindrance. Here, we predict that the ultrasmall-sized formate (Fa) and acetate (Ac) have more efficient passivation ability because of the stronger binding with the perovskite, as demonstrated by density functional theory calculation. We introduce ultrasmall-sized cesium salts (CsFa/CsAc) into buried interface, which can also diffuse into the bulk, resulting in both buried interface and bulk passivation. In addition, the improved perovskite growth has been found due to the enhanced hydrophily after introducing CsFa/CsAc as additive. According to these advantages, a pure-red PeLED with 24.2% efficiency at 639 nm has been achieved.

Roadmap on Perovskite light-emitting diodes

Abstract In recent years, the field of metal-halide perovskite emitters has rapidly emerged as a new community in solid-state lighting. Their exceptional optoelectronic properties have contributed to the rapid rise in external quantum efficiencies (EQEs) in perovskite light-emitting diodes (PeLEDs) from <1% (in 2014) to approaching 30% (in 2023) across a wide range of wavelengths. However, several challenges still hinder their commercialization, including the relatively low EQEs of blue/white devices, limited EQEs in large-area devices, poor device stability, as well as the toxicity of the easily accessible lead components and the solvents used in the synthesis and processing of PeLEDs. This roadmap addresses the current and future challenges in PeLEDs across fundamental and applied research areas, by sharing the community's perspectives. This work will provide the field with practical guidelines to advance PeLED development and facilitate more rapid commercialization.

Charge Injection and Auger Recombination Modulation for Efficient and Stable Quasi-2D Perovskite Light-Emitting Diodes.

The inefficient charge transport and large exciton binding energy of quasi-2D perovskites pose challenges to the emission efficiency and roll-off issues for perovskite light-emitting diodes (PeLEDs) despite excellent stability compared to 3D counterparts. Herein, alkyldiammonium cations with different molecular sizes, namely 1,4-butanediamine (BDA), 1,6-hexanediamine (HDA) and 1,8-octanediamine (ODA), are employed into quasi-2D perovskites, to simultaneously modulate the injection efficiency and recombination dynamics. The size increase of the bulky cation leads to increased excitonic recombination and also larger Auger recombination rate. Besides, the larger size assists the formation of randomly distributed 2D perovskite nanoplates, which results in less efficient injection and deteriorates the electroluminescent performance. Moderate exciton binding energy, suppressed 2D phases and balanced carrier injection of HDA-based PeLEDs contribute to a peak external quantum efficiency of 21.9%, among the highest in quasi-2D perovskite based near-infrared devices. Besides, the HDA-PeLED shows an ultralong operational half-lifetime T50 up to 479h at 20mA cm‒2, and sustains the initial performance after a record-level 30000 cycles of ON-OFF switching, attributed to the suppressed migration of iodide anions into adjacent layers and the electrochemical reaction in HDA-PeLEDs. This work provides a potential direction of cation design for efficient and stable quasi-2D-PeLEDs.

Thermally Induced Phase Separation of the PEDOT:PSS Layer for Highly Efficient Laminated Polymer Light-Emitting Diodes.

Among various conductive polymers, the poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) film has been studied as a promising material for use as a transparent electrode and a hole-injecting layer in organic optoelectronic devices. Due to the increasing demand for the low-cost fabrication of organic light-emitting diodes (OLEDs), PEDOT:PSS has been employed as the top electrode by using the coating or lamination method. Herein, a facile method is reported for the fabrication of highly efficient polymer light-emitting diodes (PLEDs) based on a laminated transparent electrode (LTE) consisting of successive PEDOT:PSS and silver-nanowire (AgNW) layers. In particular, thermally induced phase separation (TIPS) of the PEDOT:PSS film is found to depend on the annealing temperature (Tanneal) during preparation of the LTE. At Tanneal close to the glass transition temperature of the PSS chains, a PSS-rich phase with a large number of PSS- molecules enhances the work function of the PEDOT:PSS on the glass-side surface relative to the air side. By using the optimized LTEs, bidirectional laminated PLEDs are obtained with a total external quantum efficiency of 2.9% and a turn-on voltage of 2.6 V, giving a comparable performance to that of the reference bottom-emitting PLED based on a costly evaporated metal electrode. In addition, an analysis of the angular characteristics, including the variation in the electroluminescence spectra and the change in luminance according to the emission angle, indicates that the laminated PLED with the LTE provides a more uniform angular distribution regardless of the direction of emission. Detailed optical and electrical analyses are also performed to evaluate the suitability of LTEs for the low-cost fabrication of efficient PLEDs.

Efficient green light-emitting diodes based on alloy quantum dots with an organic/inorganic hybrid surface passivation

As we know, the ligands on the surface of core/shell structured quantum dots (QDs) play an important role. They not only bind with metal ions to passivate surface defects but also have a great influence on colloidal stability. All-organic or all-inorganic ligands afford QDs with some disadvantages such as low conductivity, poor dispersibility and undesirable stability. By combining with the advantages of organic and inorganic ligands, herein, we achieve an organic/inorganic hybrid surface passivation through exchanging partial oleic acid ligands with chlorine ions (Cl−), affording QD with a core/shell structure of CdZnSe/ZnSe/ZnS/OACl. It exhibits an excellent nanostructure with a mean size of around 11.6 nm. According to X-ray photoelectron spectroscopy (XPS) spectra, around 30% oleid acid ligands are removed by Cl−, resulting in the hybrid surface passivation. The CdZnSe/ZnSe/ZnS/OACl QD exhibit an efficient green emission at the wavelength of around 535 nm with a quantum yield of over 90%. The QD light-emitting diode (QLED) based on CdZnSe/ZnSe/ZnS/OACl exhibits a peak EQE of 15.6% and a brightness of over 1.1 × 105 cd m−2 at 6 V, corresponding to an efficient green emitting device. Therefore, we believe that the hybrid surface passivation could provid a reliable avenue to efficient QD materials.

Vertically Concentrated Quantum Wells Enabling Highly Efficient Deep-Blue Perovskite Light-Emitting Diodes.

Deep-blue perovskite light-emitting diodes (PeLEDs) based on quasi-two-dimensional (quasi-2D) systems exist heightened sensitivity to the domain distribution. The top-down crystallization mode will lead to a vertical gradient distribution of quantum well (QW) structure, which is unfavorable for deep-blue emission. Herein, a thermal gradient annealing treatment is proposed to address the polydispersity issue of vertical QWs in quasi-2D perovskites. The formation of large-n domains at the upper interface of the perovskite film can be effectively inhibited by introducing a low-temperature source in the annealing process. Combined with the utilization of NaBr to inhibit the undesirable n=1 domain, a vertically concentrated QW structure is ultimately attained. As a result, the fabricated device delivers a narrow and stable deep-blue emission at 458 nm with an impressive external quantum efficiency (EQE) of 5.82 %. Green and sky-blue PeLEDs with remarkable EQE of 21.83 % and 17.51 % are also successfully achieved, respectively, by using the same strategy. The findings provide a universal strategy across the entire quasi-2D perovskites, paving the way for future practical application of PeLEDs.

Nanosurface-reconstructed perovskite for highly efficient and stable active-matrix light-emitting diode display.

Perovskite quantum dots (QDs) are promising for various photonic applications due to their high colour purity, tunable optoelectronic properties and excellent solution processability. Surface features impact their optoelectronic properties, and surface defects remain a major obstacle to progress. Here we develop a strategy utilizing diisooctylphosphinic acid-mediated synthesis combined with hydriodic acid-etching-driven nanosurface reconstruction to stabilize CsPbI3 QDs. Diisooctylphosphinic acid strongly adsorbs to the QDs and increases the formation energy of halide vacancies, enabling nanosurface reconstruction. The QD film with nanosurface reconstruction shows enhanced phase stability, improved photoluminescence endurance under thermal stress and electric field conditions, and a higher activation energy for ion migration. Consequently, we demonstrate perovskite light-emitting diodes (LEDs) that feature an electroluminescence peak at 644 nm. These LEDs achieve an external quantum efficiency of 28.5% and an operational half-lifetime surpassing 30 h at an initial luminance of 100 cd m-2, marking a tenfold improvement over previously published studies. The integration of these high-performance LEDs with specifically designed thin-film transistor circuits enables the demonstration of solution-processed active-matrix perovskite displays that show a peak external quantum efficiency of 23.6% at a display brightness of 300 cd m-2. This work showcases nanosurface reconstruction as a pivotal pathway towards high-performance QD-based optoelectronic devices.

Ca2+ induced highly fluorescent CsPb(Br/Cl)3 perovskite quantum dots via fast Anion-Exchange & Cation-Doping Inter-Promotion strategy for efficient deep-blue light-emitting diodes

Despite the impressive development of perovskite light-emitting diodes (PeLEDs), it is still challenging to achieve high-efficiency deep-blue PeLEDs using colloid perovskite quantum dots (PQDs). The efficiency of PQDs with a wavelength below 460 nm, which meets the requirements for deep-blue emission in the Telecommunication Union UHD television standard (ITU REC. 2020), lags far behind those of their sky-blue counterparts. To address this issue, a novel strategy of fast anion-exchange & cation-doping inter-promotion (FAECDIP) is proposed to achieve highly efficient deep-blue PQDs by introducing CaBr2 into the CsPbCl3 PQDs. Owing to the presence of Ca2+, the speed of ion exchange is increased, driven by the smaller cation, Ca2+, improving the preparation efficiency. Additionally, Ca2+ was doped on the surface of PQDs. Based on studies of fast anion-exchange and theoretical calculations, Ca2+ improves the optical performance by decreasing the number of traps and increasing the crystallinity of target PQDs, facilitating the stability of treated films and PeLEDs by enhancing the formation energy of halogen vacancies. Here, a high PLQY of 80.3 % CaBr2-induced CsPb(Cl/Br)3 deep-blue PQDs (∼446 nm) was achieved. The correspondent PeLEDs (∼447 nm) achieved a superior EQE of 5.88 %, which is the state-of-the-art among the reported deep-blue PeLEDs. Our strategy provides a potential route to achieve deep-blue PeLEDs, which differs from the previous tedious-complex methods.

Enhanced efficiency of deep ultraviolet light-emitting diodes utilizing full-coverage Al reflector and highly reflective Ni/Rh p-electrode

Increasing the reflection of p-side is an effective way to improve the optoelectronic performance of flip-chip light-emitting diodes (FCLEDs). Here, we propose a full-coverage Al reflector (FAR) and a highly reflective Ni/Rh p-electrode to enhance the performance of deep ultraviolet (DUV) FCLEDs. The physical mechanism for the impact of the FAR and Ni/Rh electrode on the light extraction efficiency (LEE) is discussed theoretically. Simulations demonstrate that the combination of the FAR and Ni/Rh electrode improves the LEEs of transverse electric- and transverse magnetic-polarized light by 13.62% and 27.08%, respectively. At an injection current of 100 mA, the fabricated DUV FCLEDs with FAR and Ni/Rh electrode exhibits an external quantum efficiency of 4.01% and a wall plugging efficiency of 2.92%, which are 16.85% and 13.18% higher than those of conventional DUV FCLEDs, respectively. These results support the promise of the FAR and Ni/Rh electrode for high-power DUV LED applications.

Regulating Surface-Passivator Binding Priority for Efficient Perovskite Light-Emitting Diodes.

Suppressing trap-assisted nonradiative losses through passivators is a prerequisite for efficient perovskite light-emitting diodes (PeLEDs). However, the complex bonding between passivators and perovskites severely suppresses the passivation process, which still lacks comprehensive understanding. Herein, the number, category, and degree of bonds between different functional groups and the perovskite are quantitatively assessed to study the passivation dynamics. Functional groups with high electrostatic potential and large steric hindrance prioritize strong bonding with organic cations and halides on the perfect surface, leading to suppressed coordination with bulky defects. By modulating the binding priorities and coordination capacity, hindrance from the intense interaction with perfect perovskite is significantly reduced, leading to a more direct passivation process. Consequently, the near-infrared PeLED without external light out-coupling demonstrates a record external quantum efficiency of 24.3% at a current density of 42mA cm-2. In addition, the device exhibits a record-level-cycle ON/OFF switching of 20000 and ultralong half-lifetime of 1126.3h under 5mA cm-2. An in-depth understanding of the passivators can offer new insights into the development of high-performance PeLEDs.

Onion-like multicolor thermally activated delayed fluorescent carbon quantum dots for efficient electroluminescent light-emitting diodes

Carbon quantum dots are emerging as promising nanomaterials for next-generation displays. The elaborate structural design is crucial for achieving thermally activated delayed fluorescence, particularly for improving external quantum efficiency of electroluminescent light-emitting diodes. Here, we report the synthesis of onion-like multicolor thermally activated delayed fluorescence carbon quantum dots with quantum yields of 42.3–61.0%. Structural, spectroscopic characterization and computational studies reveal that onion-like structures assembled from monomer carbon quantum dots of different sizes account for the decreased singlet-triplet energy gap, thereby achieving efficient multicolor thermally activated delayed fluorescence. The devices exhibit maximum luminances of 3785–7550 cd m−2 and maximum external quantum efficiency of 6.0–9.9%. Importantly, owing to the weak van der Waals interactions and adequate solution processability, flexible devices with a maximum luminance of 2554 cd m−2 are realized. These findings facilitate the development of high-performance carbon quantum dots-based electroluminescent light-emitting diodes that are promising for practical applications.

Formation of homogeneous pyridinic emission states in carbon dots via solid-state carbonization of aminoquinoline: Optical design principles and light-emitting diode applications

Developing carbon dots (CDs) for practical applications faces significant hurdles due to non-homogeneity in their chemical structure, leading to broad spectral distribution and the excitation-energy-dependent behavior of their fluorescence (FL) emission properties. To address this challenge, we implemented solid-state carbonization of 6-aminoquinoline (6-AQ) devoid of any additives that could induce chemical non-homogeneity. This process yielded pyridinic-nitrogen-doped CDs (PN-CDs) characterized by homogenous, uniform emission states arising from pyridine-incorporated heteroatomic structures. Notably, these PN-CDs exhibited excitation-energy-independent FL at 520 nm with a full-width-half-maximum of 70 nm. To elucidate the structure-property relationship in PN-CDs, a comprehensive analysis encompassing time-resolved spectroscopy and ab initio calculations was conducted. Furthermore, we performed a comparative study by manipulating synthesis parameters and utilizing six AQ isomers, offering valuable insights to optimize the optical properties of PN-CDs. Finally, we successfully demonstrated high-color-purity and efficient green light-emitting diodes utilizing PN-CDs, highlighting their potential for future display applications. This paves the way for advancement in optical materials with enhanced performance and reduced environmental impact.