Single‐Mode Lasing from Colloidal Water‐Soluble CdSe/CdS Quantum Dot‐in‐Rods

Core–shell CdSe/CdS nanocrystals are a very promising material for light emitting applications. Their solution‐phase synthesis is based on surface‐stabilizing ligands that make them soluble in organic solvents, like toluene or chloroform. However, solubility of these materials in water provides many advantages, such as additional process routes and easier handling. So far, solubilization of CdSe/CdS nanocrystals in water that avoids detrimental effects on the luminescent properties poses a major challenge. This work demonstrates how core–shell CdSe/CdS quantum dot‐in‐rods can be transferred into water using a ligand exchange method employing mercaptopropionic acid (MPA). Key to maintaining the light‐emitting properties is an enlarged CdS rod diameter, which prevents potential surface defects formed during the ligand exchange from affecting the photophysics of the dot‐in‐rods. Films made from water‐soluble dot‐in‐rods show amplified spontaneous emission (ASE) with a similar threshold (130 μJ/cm²) as the pristine material (115 μJ/cm²). To demonstrate feasibility for lasing applications, self‐assembled microlasers are fabricated via the “coffee‐ring effect” that display single‐mode operation and a very low threshold of ～10 μJ/cm². The performance of these microlasers is enhanced by the small size of MPA ligands, enabling a high packing density of the dot‐in‐rods.     

Chiral Octahydro‐Binaphthol Compound‐Based Thermally Activated Delayed Fluorescence Materials for Circularly Polarized Electroluminescence with Superior EQE of 32.6% and Extremely Low Efficiency Roll‐Off

Circularly polarized organic light‐emitting diodes (CP‐OLEDs) are particularly favorable for the direct generation of CP light, and they demonstrate a promising application in 3D display. However, up to now, such CP devices have suffered from low brightness, insufficient efficiency, and serious efficiency roll‐off. In this study, a pair of octahydro‐binaphthol ( OBN )‐based chiral emitting enantiomers, (R/S)‐OBN‐Cz , are developed by ingeniously merging a chiral source and a luminophore skeleton. These chirality–acceptor–donor (C–A–D)‐type and rod‐like compounds concurrently generate thermally activated delayed fluorescence with a small ΔE_ST of 0.037 eV, as well as a high photoluminescence quantum yield of 92% and intense circularly polarized photoluminescence with dissymmetry factors (|g_PL|) of ≈2.0 × 10^?3 in thin films. The CP‐OLEDs based on (R/S)‐OBN‐Cz enantiomers not only display obvious circularly polarized electroluminescence signals with a |g_EL| of ≈2.0 × 10^?3, but also exhibit superior efficiencies with maximum external quantum efficiency (EQE_max) up to 32.6% and extremely low efficiency roll‐off with an EQE of 30.6% at 5000 cd m^?2, which are the best performances among the reported CP devices to date.     

A Singlet Oxygen Generating Agent by Chirality‐dependent Plasmonic Shell‐Satellite Nanoassembly

Photodynamic therapy (PDT) agent, which generates singlet oxygen (¹O₂) under light, has attracted significant attention for its broad biological and medical applications. Here, DNA‐driven shell–satellite (SS) gold assemblies as chiral photosensitizers are first fabricated. The chiral plasmonic nanostructure, coupling with cysteine enantiomers on its surface, exhibits intense chiroplasmonic activities (?40.2 ± 2.6 mdeg) in the visible region. These chiral SS nanoassemblies have high reactive oxygen species generating efficiency under circular polarized light illumination, resulting in a ¹O₂ quantum yield of 1.09. Meanwhile, it is found that SS could be utilized as PDT agent with remarkable efficiency under right circular polarized light irradiation in vitro and in vivo, allowing X‐ray computed tomography (CT) and photoacoustics (PA) imaging for tumors simultaneously. The achievements reveal that the enantiomer‐dependent and structure‐induced nanoassemblies play an important role in PDT effects. The present researches open up a new avenue for cancer diagnose and therapy using chiral nanostructures as multifunctional platform.     

Stretchable Organometal‐Halide‐Perovskite Quantum‐Dot Light‐Emitting Diodes

Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A^?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.     

Nanofiber‐Directed Anisotropic Self‐Assembly of CdSe–CdS Quantum Rods for Linearly Polarized Light Emission Evidenced by Quantum Rod Orientation Microscopy

Hybrid soft materials composed of CdSe–CdS nanorods or “quantum rods” (QRs) and the fluorescent 2,3‐didecyloxyanthracene (DDOA) low molecular weight organogelator are obtained through self‐assembly. Spectroscopy, microscopy, and rheology studies show that the QRs and DDOA coassemble, thereby stabilizing the organogels. Depending on the QR load and excitation wavelength, single nanofibers (NFs) of the hybrid gel display either sharp polarized red luminescence (under green excitation), or dual perpendicularly polarized blue and red emissions (under UV excitation). Transmission electron microscopy, microspectroscopy, and quantum rod orientation microscopy (QROM) reveal that QRs align along the organogel NFs with order parameters reaching 76% and 87%. This paves the way for obtaining surfaces of QR/NF assemblies yielding sharp red linearly polarized emission. In addition, this work demonstrates that QRs can be used more generally to probe nanostructured soft materials, even nonemissive ones. QROM allows to establish maps of the orientation of single QRs dispersed onto or within a gel network by measuring the polarization of the emission of the individual QRs. As occurs within this work in which QRs and NFs interact, the orientation of each QR reveals information on the underlying nanostructure (such as surface striation, bundle formation, and helicity).     

All‐Solution‐Processed Pure Formamidinium‐Based Perovskite Light‐Emitting Diodes

All‐solution‐processed pure formamidinium‐based perovskite light‐emitting diodes (PeLEDs) with record performance are successfully realized. It is found that the FAPbBr₃ device is hole dominant. To achieve charge carrier balance, on the anode side, PEDOT:PSS 8000 is employed as the hole injection layer, replacing PEDOT:PSS 4083 to suppress the hole current. On the cathode side, the solution‐processed ZnO nanoparticle (NP) is used as the electron injection layer in regular PeLEDs to improve the electron current. With the smallest ZnO NPs (2.9 nm) as electron injection layer (EIL), the solution‐processed PeLED exhibits a highest forward viewing power efficiency of 22.3 lm W^?1, a peak current efficiency of 21.3 cd A^?1, and an external quantum efficiency of 4.66%. The maximum brightness reaches a record 1.09 × 10⁵ cd m^?2. A record lifetime T₅₀ of 436 s is achieved at the initial brightness of 10 000 cd m^?2. Not only do PEDOT:PSS 8000 HIL and ZnO NPs EIL modulate the injected charge carriers to reach charge balance, but also they prevent the exciton quenching at the interface between the charge injection layer and the light emission layer. The subbandgap turn‐on voltage is attributed to Auger‐assisted energy up‐conversion process.     

High‐Efficiency Perovskite Light‐Emitting Diodes with Synergetic Outcoupling Enhancement

Perovskite light‐emitting diodes (PeLEDs) show great application potential in high‐quality flat‐panel displays and solid‐state lighting due to their steadily improved efficiency, tunable colors, narrow emission peak, and easy solution‐processing capability. However, because of high optical confinement and nonradiative charge recombination during electron–photon conversion, the highest reported efficiency of PeLEDs remains far behind that of their conventional counterparts, such as inorganic LEDs, organic LEDs, and quantum‐dot LEDs. Here a facile route is demonstrated by adopting bioinspired moth‐eye nanostructures at the front electrode/perovskite interface to enhance the outcoupling efficiency of waveguided light in PeLEDs. As a result, the maximum external quantum efficiency and current efficiency of the modified cesium lead bromide (CsPbBr₃) green‐emitting PeLEDs are improved to 20.3% and 61.9 cd A^?1, while retaining spectral and angular independence. Further reducing light loss in the substrate mode using a half‐ball lens, efficiencies of 28.2% and 88.7 cd A^?1 are achieved, which represent the highest values reported to date for PeLEDs. These results represent a substantial step toward achieving practical applications of PeLEDs.     

Room‐Temperature Triple‐Ligand Surface Engineering Synergistically Boosts Ink Stability,Recombination Dynamics,and Charge Injection toward EQE‐11.6% Perovskite QLEDs

Developing low‐cost and high‐quality quantum dots (QDs) or nanocrystals (NCs) and their corresponding efficient light‐emitting diodes (LEDs) is crucial for the next‐generation ultra‐high‐definition flexible displays. Here, there is a report on a room‐temperature triple‐ligand surface engineering strategy to play the synergistic role of short ligands of tetraoctylammonium bromide (TOAB), didodecyldimethylammonium bromide (DDAB), and octanoic acid (OTAc) toward “ideal” perovskite QDs with a high photoluminescence quantum yield (PLQY) of >90%, unity radiative decay in its intrinsic channel, stable ink characteristics, and effective charge injection and transportation in QD films, resulting in the highly efficient QD‐based LEDs (QLEDs). Furthermore, the QD films with less nonradiative recombination centers exhibit improved PL properties with a PLQY of 61% through dopant engineering in A‐site. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on CsPbBr₃ QDs with the peak external quantum efficiency (EQE) of 11.6%, and the corresponding peak internal quantum efficiency (IQE) and power efficiency are 52.2% and 44.65 lm W^?1, respectively, which are the most‐efficient perovskite QLEDs with colloidal CsPbBr₃ QDs as emitters up to now. These results demonstrate that the as‐obtained QD inks have a wide range application in future high‐definition QD displays and high‐quality lightings.     

Rare‐Earth‐Element‐Ytterbium‐Substituted Lead‐Free Inorganic Perovskite Nanocrystals for Optoelectronic Applications

Lead‐(Pb‐) halide perovskite nanocrystals (NCs) are interesting nanomaterials due to their excellent optical properties, such as narrow‐band emission, high photoluminescence (PL) efficiency, and wide color gamut. However, these NCs have several critical problems, such as the high toxicity of Pb, its tendency to accumulate in the human body, and phase instability. Although Pb‐free metal (Bi, Sn, etc.) halide perovskite NCs have recently been reported as possible alternatives, they exhibit poor optical and electrical properties as well as abundant intrinsic defect sites. For the first time, the synthesis and optical characterization of cesium ytterbium triiodide (CsYbI₃) cubic perovskite NCs with highly uniform size distribution and high crystallinity using a simple hot‐injection method are reported. Strong excitation‐independent emission and high quantum yields for the prepared NCs are verified using photoluminescence measurements. Furthermore, these CsYbI₃ NCs exhibit potential for use in organic–inorganic hybrid photodetectors as a photoactive layer. The as‐prepared samples exhibit clear on–off switching behavior as well as high photoresponsivity (2.4 × 10³ A W^?1) and external quantum efficiency (EQE, 5.8 × 10⁵%) due to effective exciton dissociation and charge transport. These results suggest that CsYbI₃ NCs offer tremendous opportunities in electronic and optoelectronic applications, such as chemical sensors, light emitting diodes (LEDs), and energy conversion and storage devices.     

Air‐Stable and High‐Performance Solution‐Processed Organic Light‐Emitting Devices Based on Hydrophobic Polymeric Ionic Liquid Carrier‐Injection Layers

A lot of research, mostly using electron‐injection layers (EILs) composed of alkali‐metal compounds has been reported with a view to increase the efficiency of solution‐processed organic light‐emitting devices (OLEDs). However, these materials have intractable properties, such as a strong affinity for moisture, which cause the degradation of OLEDs. Consequently, optimal EIL materials should exhibit high electron‐injection efficiency as well as be stable in air. In this study, polymer light‐emitting devices (PLEDs) based on the commonly used yellow‐fluorescence‐emitting polymer F8BT, which utilize poly(diallyldimethylammonium)‐based polymeric ionic liquids, are experimentally and analytically investigated. As a result, the optimized PLED employing an EIL comprising poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (poly(DDA)TFSI), which is expected to display good moisture resistance because of water repellency of fluorocarbon groups, exhibits excellent storage stability in air and electroluminescence performance with a low turn‐on voltage of 2.01 V, maximum external quantum efficiency of 9.00%, current efficiency of 30.1 cd A^?1, and power efficiency of 32.4 lm W^?1. The devices with poly(DDA)TFSI show one of the highest efficiencies as compared to the reported standard PLEDs. Moreover, poly(DDA)TFSI is applied as a hole‐injection layer (HIL). The optimized PLED using poly(DDA)TFSI as the HIL exhibits performances comparable to those of a device that uses a conventional poly(3,4‐ethylenedioxy‐thiophene):poly(4‐styrenesulfonate) HIL.     

Photoaligned Nanorod Enhancement Films with Polarized Emission for Liquid‐Crystal‐Display Applications

Semiconductor nanorods (NR) emit polarized light, which is expected to bring manifold benefits, in terms of brightness and color enhancement, for modern liquid‐crystal displays (LCD). In this regard, photoaligned nanorod enhancement films (NREF) for color and polarization conversion for LCD backlights are introduced here. The photoinduced anchoring forces, by the photoalignment layer, stimulate well‐ordered self‐assembly of NR in the thin polymer films. Green and red emitting NR with a quantum yield of ≈80% are aligned unidirectionally and in‐plane, showing a polarization ratio of >7:1 and a degree of polarization of >0.81. The photoalignment technique facilitates the fabrication of mixed and multiple stacked NREF for LCDs, which improves the color gamut and polarization efficiency, and is thus expected to increase the optical efficiency of conventional LCDs by ≈60%.     

Versatile Indolocarbazole‐Isomer Derivatives as Highly Emissive Emitters and Ideal Hosts for Thermally Activated Delayed Fluorescent OLEDs with Alleviated Efficiency Roll‐Off

Maintaining high efficiency at high brightness levels is an exigent challenge for real‐world applications of thermally activated delayed fluorescent organic light‐emitting diodes (TADF‐OLEDs). Here, versatile indolocarbazole‐isomer derivatives are developed as highly emissive emitters and ideal hosts for TADF‐OLEDs to alleviate efficiency roll‐off. It is observed that photophysical and electronic properties of these compounds can be well modulated by varying the indolocarbazole isomers. A photoluminescence quantum yield (η_PL) approaching unity and a maximum external quantum efficiency (EQE_max) of 25.1% are obtained for the emitter with indolo[3,2‐a]carbazolyl subunit. Remarkably, record‐high EQE/power efficiency of 26.2%/69.7 lm W^?1 at the brightness level of 5000 cd m^?2 with a voltage of only 3.74 V are also obtained using the same isomer as the host in a green TADF‐OLED. It is evident that TADF hosts with high η_PL values, fast reverse intersystem crossing processes, and balanced charge transport properties may open the path toward roll‐off‐free TADF‐OLEDs.     

Mixed Lead–Tin Halide Perovskites for Efficient and Wavelength‐Tunable Near‐Infrared Light‐Emitting Diodes

Near‐infrared (NIR) light‐emitting diodes (LEDs), with emission wavelengths between 800 and 950 nm, are useful for various applications, e.g., night‐vision devices, optical communication, and medical treatments. Yet, devices using thin film materials like organic semiconductors and lead based colloidal quantum dots face certain fundamental challenges that limit the improvement of external quantum efficiency (EQE), making the search of alternative NIR emitters important for the community. In this work, efficient NIR LEDs with tunable emission from 850 to 950 nm, using lead–tin (Pb‐Sn) halide perovskite as emitters are demonstrated. The best performing device exhibits an EQE of 5.0% with a peak emission wavelength of 917 nm, a turn‐on voltage of 1.65 V, and a radiance of 2.7 W Sr^?1 m^?2 when driven at 4.5 V. The emission spectra of mixed Pb‐Sn perovskites are tuned either by changing the Pb:Sn ratio or by incorporating bromide, and notably exhibit no phase separation during device operation. The work demonstrates that mixed Pb‐Sn perovskites are promising next generation NIR emitters.     

Efficient Red Perovskite Light‐Emitting Diodes Based on Solution‐Processed Multiple Quantum Wells

This paper reports a facile and scalable process to achieve high performance red perovskite light‐emitting diodes (LEDs) by introducing inorganic Cs into multiple quantum well (MQW) perovskites. The MQW structure facilitates the formation of cubic CsPbI₃ perovskites at low temperature, enabling the Cs‐based QWs to provide pure and stable red electroluminescence. The versatile synthesis of MQW perovskites provides freedom to control the crystallinity and morphology of the emission layer. It is demonstrated that the inclusion of chloride can further improve the crystallization and consequently the optical properties of the Cs‐based MQW perovskites, inducing a low turn‐on voltage of 2.0 V, a maximum external quantum efficiency of 3.7%, a luminance of ≈440 cd m^?2 at 4.0 V. These results suggest that the Cs‐based MQW LED is among the best performing red perovskite LEDs. Moreover, the LED device demonstrates a record lifetime of over 5 h under a constant current density of 10 mA cm^?2. This work suggests that the MQW perovskites is a promising platform for achieving high performance visible‐range electroluminescence emission through high‐throughput processing methods, which is attractive for low‐cost lighting and display applications.     

Spontaneous Formation of Noble‐ and Heavy‐Metal‐Free Alloyed Semiconductor Quantum Rods for Efficient Photocatalysis

Quasi‐1D cadmium chalcogenide quantum rods (QRs) are benchmark semiconductor materials that are combined with noble metals to constitute QR heterostructures for efficient photocatalysis. However, the high toxicity of cadmium and cost of noble metals are the main obstacles to their widespread use. Herein, a facile colloidal synthetic approach is reported that leads to the spontaneous formation of cadmium‐free alloyed ZnS_xSe_1?x QRs from polydisperse ZnSe nanowires by alkylthiol etching. The obtained non‐noble‐metal ZnS_xSe_1?x QRs can not only be directly adopted as efficient photocatalysts for water oxidation, showing a striking oxygen evolution capability of 3000 µmol g^?1 h^?1, but also be utilized to prepare QR‐sensitized TiO₂ photoanodes which present enhanced photo‐electrochemical (PEC) activity. Density functional theory (DFT) simulations reveal that alloyed ZnS_xSe_1?x QRs have highly active Zn sites on the (100) surface and reduced energy barrier for oxygen evolution, which in turn, are beneficial to their outstanding photocatalytic and PEC activities.     

Understanding and Manipulating the Interplay of Wide‐Energy‐Gap Host and TADF Sensitizer in High‐Performance Fluorescence OLEDs

Comprising an emitting layer (EML) constituting a wide‐energy‐gap host, a thermally activated delayed fluorescence (TADF) sensitizer and a conventional fluorescent dopant, TADF‐sensitizing‐fluorescence organic light‐emitting diodes (TSF‐OLEDs) highly depend on component interplay to maximize their performance, which, however, is still under‐researched. Taking the host type (TADF or non‐TADF) and the recombination position (on the host or on the TADF sensitizer) into consideration, the interplay of host and TADF sensitizer is comprehensively studied and manipulated. A wide‐energy‐gap host with TADF and recombination of charges on it are both required to maximize device performances by triggering multiple sensitizing processes to eliminate exciton losses. Based on those findings, a maximum external quantum efficiency (EQE)/power efficiency (PE) of 23.2%/76.9 lm W^?1 is realized with a newly developed TADF host, significantly outperforming the reference devices. Further device optimization leads to unprecedently high EQE/PE of 24.2%/89.5 lm W^?1 and a half‐lifetime of over 400 h at an initial luminance of 2000 cd m^?2, with the peak PE being the highest value among the reported TSF‐OLEDs. This work reveals the importance of manipulating the component interplay in EMLs, opening a new avenue toward highly efficient TSF‐OLEDs.     

High Efficiency Light‐Emitting Transistor with Vertical Metal–Oxide Heterostructure

The monolithic integration of light‐emission with a standard logic transistor is a much‐desired multifunctionality. Here, a high‐efficiency light‐emitting transistor (LET) employing an inorganic quantum dots (QDs) emitter and a laser‐annealed vertical metal–oxide heterostructure is reported. The experimental results show that the peak efficiency and luminance of this QDs LET (QLET) are 11% and 8000 cdm^?2, respectively at a monochromatic emitting light wavelength of 585 nm. As far as it is known, these are among the highest values ever achieved for LETs. More importantly, the QLET exhibits an ultrahigh electron mobility of up to 25 cm² V^?1 S^?1, a lower efficiency roll‐off (7% at high 3000 cdm^?2), and excellent stability with long‐duration gate stress switching cycles. Additionally, this approach is compatible with those used in conventional large‐area silicon electronic manufacturing and can enable a scalable and cost‐effective procedure for future integrated versatile displays and lighting applications.     

A Phosphanthrene Oxide Host with Close Sphere Packing for Ultralow‐Voltage‐Driven Efficient Blue Thermally Activated Delayed Fluorescence Diodes

A phosphanthrene oxide host, 5,10‐diphenyl‐phosphanthrene 5,10‐dioxide ( DPDPO₂A ), with intra‐ and intermolecular hydrogen bonds achieves spheroidal cis ‐configuration and close sphere packing. DPDPO₂A realizes effective exciton suppression and excellent and balanced carrier transporting ability, both at the same time, demonstrating favorable photoluminescence quantum yield of 84% from its blue thermally activated delayed fluorescence (TADF) dye, namely bis[4‐(9,9‐dimethyl‐9,10‐dihydroacridine) phenyl]sulfone, doped films and high electron and hole mobility at the level of 10^?4 and 10^?5 cm² V^?1 s^?1, respectively. DPDPO₂A endows its blue TADF devices with record‐low driving voltages, e.g., turn‐on voltage of 2.5 V, and the state‐of‐the‐art efficiencies with maxima of 22.5% for external quantum efficiency and 52.9 lm W^?1 for power efficiency, which is the best comprehensive performance to date of ultralow‐voltage‐driven blue TADF diodes.     

Lead Halide Post‐Perovskite‐Type Chains for High‐Efficiency White‐Light Emission

Hybrid metal halides containing perovskite layers have recently shown great potential for applications in solar cells and light‐emitting diodes. Such compounds exhibit quantum confinement effects leading to tunable optical and electronic properties. Thus, broadband white‐light emission has been observed from diverse metal halides and, owing to high color rendering index, high thermal stability, and low‐temperature solution processability, these materials have attracted interest for application in solid‐state lighting. However, the reported quantum yields for white photoluminescence (PLQY) remain low (i.e., in the range 0.5–9%) and no approach has shown to successfully increase the intensity of this emission. Here, it is demonstrated that the quantum efficiencies of hybrid metal halides can be greatly enhanced if they contain a polymorph of the [PbX₄]^2? perovskite‐type layers: the [PbX₄]^2? post‐perovskite‐type chains showing a PLQY of 45%. Different piperazines lead to a hybrid lead halide with either perovskite layers or post‐perovskite chains influencing strongly the presence of self‐trapped states for excitons. It is anticipated that this family of hybrid lead halide materials could enhance all the properties requiring the stabilization of trapped excitons.     

High‐Performance Fluorescent Organic Light‐Emitting Diodes Utilizing an Asymmetric Anthracene Derivative as an Electron‐Transporting Material

Fluorescent organic light‐emitting diodes with thermally activated delayed fluorescent sensitizers (TSF‐OLEDs) have aroused wide attention, the power efficiencies of which, however, are limited by the mutual exclusion of high electron‐transport mobility and large triplet energy of electron‐transporting materials (ETMs). Here, an asymmetric anthracene derivative with electronic properties manipulated by different side groups is developed as an ETM to promote TSF‐OLED performances. Multiple intermolecular interactions are observed, leading to a kind of “cable‐like packing” in the crystal and favoring the simultaneous realization of high electron‐transporting mobility and good exciton‐confinement ability, albeit the low triplet energy of the ETM. The optimized TSF‐OLEDs exhibit a record‐high maximum external quantum efficiency/power efficiency of 24.6%/76.0 lm W^?1, which remain 23.8%/69.0 lm W^?1 at a high luminance of even 5000 cd m^?2 with an extremely low operation voltage of 3.14 V. This work opens a new paradigm for designing ETMs and also paves the way toward practical application of TSF‐OLEDs.