Uniform Luminous Perovskite Nanofibers with Color‐Tunability and Improved Stability Prepared by One‐Step Core/Shell Electrospinning

A one‐step core/shell electrospinning technique is exploited to fabricate uniform luminous perovskite‐based nanofibers, wherein the perovskite and the polymer are respectively employed in the core and the outer shell. Such a coaxial electrospinning technique enables the in situ formation of perovskite nanocrystals, exempting the needs of presynthesis of perovskite quantum dots or post‐treatments. It is demonstrated that not only the luminous electrospun nanofibers can possess color‐tunability by simply tuning the perovskite composition, but also the grain size of the formed perovskite nanocrystals is largely affected by the perovskite precursor stoichiometry and the polymer solution concentration. Consequently, the optimized perovskite electrospun nanofiber yields a high photoluminescence quantum yield of 30.9%, significantly surpassing the value of its thin‐film counterpart. Moreover, owing to the hydrophobic characteristic of shell polymer, the prepared perovskite nanofiber is endowed with a high resistance to air and water. Its photoluminescence intensity remains constant while stored under ambient environment with a relative humidity of 85% over a month and retains intensity higher than 50% of its initial intensity while immersed in water for 48 h. More intriguingly, a white light‐emitting perovskite‐based nanofiber is successfully fabricated by pairing the orange light‐emitting compositional perovskite with a blue light‐emitting conjugated polymer.     

Light Generation in Lead Halide Perovskite Nanocrystals: LEDs,Color Converters,Lasers, and Other Applications

Facile solution processing lead halide perovskite nanocrystals (LHP‐NCs) exhibit superior properties in light generation, including a wide color gamut, a high flexibility for tuning emissive wavelengths, a great defect tolerance and resulting high quantum yield; and intriguing electric feature of ambipolar transport with moderate and comparable mobility. As a result, LHP‐NCs have accomplished great achievements in various light generation applications, including color converters for lighting and display, light‐emitting diodes, low threshold lasing, X‐ray scintillators, and single photon emitters. Herein, the considerable progress that has been made thus far is reviewed along with the current challenges and future prospects in the light generation applications of LHP‐NCs.     

Molecule‐Induced p‐Doping in Perovskite Nanocrystals Enables Efficient Color‐Saturated Red Light‐Emitting Diodes

Color‐saturated red light‐emitting diodes (LEDs) with emission wavelengths at around 620–640 nm are an essential part of high‐definition displays. Metal halide perovskites with very narrow emission linewidth are promising emitters, and rapid progress has been made in perovskite‐based LEDs (PeLEDs); however, the efficiency of the current color—pure red PeLEDs—still far lags behind those of other‐colored ones. Here, a simple but efficient strategy is reported to gradually down‐shift the Fermi level of perovskite nanocrystals (NCs) by controlling the interaction between NCs and their surface molecular electron acceptor—benzyl iodide with aromatic rings—and realize p‐doping in the color‐saturated 625 nm emitting NCs, which significantly reduces the hole injection barrier in devices. Besides, both the luminescence efficiency and electric conductivity of perovskite NCs are enhanced as additional advantages as the result of surface defects passivation. As a result, the external quantum efficiency for the resulting LED is increased from 4.5% to 12.9% after benzyl iodide treatment, making this device the best‐performing color‐saturated red PeLED so far. It is further found that the hole injection plays a more critical role than the photoluminescence efficiency of perovskite emitter in determining the LED performance, which implies design principles for efficient thin‐film planar LEDs.     

White light-emitting diode coated with ZnSe:Mn/ZnSe nanocrystal films enveloped by SiO2

Mn-doped nanocrystals (NCs) have attracted much attention for their excellent properties. In our work, colloidal Mn-doped NCs with high quantum yield are synthesized and enveloped with silica hydrosol. The blend of NCs and silica hydrosol is coated on a blue light-emitting diode (LED), and the appropriate thickness of the NC film is found. White light is gained through the mix of the blue emission of the LED and the orange emission from Mn-doped NC films. The chromaticity coordinates and the image of the white LED indicate that Mn-doped NCs can be a good substitute for YAG:Ce phosphor, and the reliability of the white LED can be improved by enveloping NCs with SiO(2).     

Postsynthetic Doping of MnCl2 Molecules into Preformed CsPbBr3 Perovskite Nanocrystals via a Halide Exchange‐Driven Cation Exchange

Unlike widely used postsynthetic halide exchange for CsPbX₃ (X is halide) perovskite nanocrystals (NCs), cation exchange of Pb is of a great challenge due to the rigid nature of the Pb cationic sublattice. Actually, cation exchange has more potential for rendering NCs with peculiar properties. Herein, a novel halide exchange‐driven cation exchange (HEDCE) strategy is developed to prepare dually emitting Mn‐doped CsPb(Cl/Br)₃ NCs via postsynthetic replacement of partial Pb in preformed perovskite NCs. The basic idea for HEDCE is that the partial cation exchange of Pb by Mn has a large probability to occur as a concomitant result for opening the rigid halide octahedron structure around Pb during halide exchange. Compared to traditional ionic exchange, HEDCE is featured by proceeding of halide exchange and cation exchange at the same time and lattice site. The time and space requirements make only MnCl₂ molecules (rather than mixture of Mn and Cl ions) capable of doping into perovskite NCs. This special molecular doping nature results in a series of unusual phenomenon, including long reaction time, core–shell structured mid states with triple emission bands, and dopant molecules composition‐dependent doping process. As‐prepared dual‐emitting Mn‐doped CsPb(Cl/Br)₃ NCs are available for ratiometric temperature sensing.     

High Performance Quasi‐2D Perovskite Sky‐Blue Light‐Emitting Diodes Using a Dual‐Ligand Strategy

For quasi‐2D perovskite light‐emitting diodes, the introduction of insulating bulky cation reduces the charge transport property, leading to lowered brightness and increased turn‐on voltage. Herein, a dual‐ligand strategy is adopted to prepare perovskite films by using an appropriate ratio of i‐butylammonium (iBA) and phenylethylammonium (PEA) as capping ligands. The introduction of iBA enhances the binding energy of the ligands on the surface of the quasi‐2D perovskite, and effectively controls the proportion of 2D perovskite to allow more efficient energy transfer, resulting in the great enhancement of the electric and luminescent properties of the perovskite. The photoluminescence (PL) mapping of the perovskite films exhibits that enhanced photoluminescence performance with better uniformity and stronger intensity can be achieved with this dual‐ligand strategy. By adjusting the proportion of the two ligands, sky‐blue perovskite light‐emitting diodes (PeLEDs) with electroluminescence (EL) peak located 485 nm are achieved with a maximum luminance up to 1130 cd m^?2 and a maximum external quantum efficiency (EQE) up to 7.84%. In addition, the color stability and device stability are significantly enhanced by using a dual‐ligand strategy. This simple and feasible method paves the way for improving the performance of quasi‐2D PeLEDs.     

Ligands in Lead Halide Perovskite Nanocrystals: From Synthesis to Optoelectronic Applications

Ligands are indispensable for perovskite nanocrystals (NCs) throughout the whole lifetime, as they not only play key roles in the controllable synthesis of NCs with different sizes and shapes, but also act as capping shell that affects optical properties and electrical coupling of NCs. Establishing a systematic understanding of the relationship between ligands and perovskite NCs is significant to enable many potential applications of NCs. This review mainly focuses on the influence of ligands on perovskite NCs. First of all, the ligands-dominated size and shape control of NCs is discussed. Whereafter, the surface defects of NCs and the bonding between ligands and perovskite NCs are classified, and corresponding post-treatment of surface defects via ligands is also summarized. Furthermore, advances in engineering the ligands towards the high performance of optoelectronic devices based on perovskite NCs, including photodetector, solar cell, light emitting diode (LED), and laser, and finally to potential challenges are also discussed.     

One‐Step Synthesis of Silica‐Coated Carbon Dots with Controllable Solid‐State Fluorescence for White Light‐Emitting Diodes

Carbon dots (CDots)‐based solid‐state luminescent materials have important applications in light‐emitting devices owing to their outstanding optical properties. However, it still remains a challenge to develop multiple‐color‐emissive solid‐state CDots, due to the serious self‐quenching of the CDots in the aggregation or solid state. Herein, a one‐step synthesis of multiple‐color‐emissive solid‐state silica‐coated CDots (silica/CDots) composites by controlling CDots loading fraction and composite morphology to realize the adjustment of emitting color is reported. The emission of resultant silica/CDots composites shifts from blue to orange with the photoluminescence quantum yields of 57.9%, 34.3%, and 32.7% for blue, yellow, and orange emitting, respectively. Furthermore, the yellow emitting silica/CDots composites exhibit an excellent fluorescence thermal stability, and further have been applied to fabricate white‐light‐emitting devices with a high color rendering index of above 80.     

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.     

Endowing Perovskite Nanocrystals with Circularly Polarized Luminescence

Perovskite nanocrystals are attracting great interest due to their excellent photonic properties. Here, through a supramolecular self‐assembly approach, the perovskite nanocrystals (NCs) with a novel circularly polarized luminescence (CPL) are successfully endowed. It is found that the achiral perovskite NCs can coassemble with chiral gelator in nonpolar solvents, in which the gelator molecules modify the surface of the perovskite NCs. Through such cogelation, the molecular chirality can transfer to the NCs resulting in CPL signals with a dissymmetric factor (g_lum) up to 10^?3. Furthermore, depending on the molecular chirality of the gelator, the CPL sense can be selected and the mirror‐imaged CPL is obtained. Such gels can be further embedded into the polymer film to facilitate flexible CPL devices. It is envisaged that this approach will afford a new insight into the designing of the functional chiroptical materials.     

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.     

Introduction of Red‐Green‐Blue Fluorescent Dyes into a Metal–Organic Framework for Tunable White Light Emission

The unique features of the metal–organic frameworks (MOFs), including ultrahigh porosities and surface areas, tunable pores, endow the MOFs with special utilizations as host matrices. In this work, various neutral and ionic guest dye molecules, such as fluorescent brighteners, coumarin derivatives, 4‐(dicyanomethylene)‐2‐methyl‐6‐(p‐dimethylaminostyryl)‐4H‐pyran (DCM), and 4‐(p‐dimethylaminostyryl)‐1‐methylpyridinium (DSM), are encapsulated in a neutral MOF, yielding novel blue‐, green‐, and red‐phosphors, respectively. Furthermore, this study introduces the red‐, green‐, and blue‐emitting dyes into a MOF together for the first time, producing white‐light materials with nearly ideal Commission International ed'Eclairage (CIE) coordinates, high color‐rendering index values (up to 92%) and quantum yields (up to 26%), and moderate correlated color temperature values. The white light is tunable by changing the content or type of the three dye guests, or the excitation wavelength. Significantly, the introduction of blue‐emitting guests in the methodology makes the available MOF host more extensive, and the final white‐light output more tunable and high‐quality. Such strategy can be widely adopted to design and prepare white‐light‐emitting materials.     

Oxalic Acid Enabled Emission Enhancement and Continuous Extraction of Chloride from Cesium Lead Chloride/Bromide Perovskite Nanocrystals

All‐inorganic cesium lead halide perovskite nanocrystals (NCs) have demonstrated excellent optical properties and an encouraging potential for optoelectronic applications; however, mixed‐halide perovskites, especially CsPb(Cl/Br)₃ NCs, still show lower photoluminescence quantum yields (PL QY) than the corresponding single‐halide materials. Herein, anhydrous oxalic acid is used to post‐treat CsPb(Cl/Br)₃ NCs in order to initially remove surface defects and halide vacancies, and thus, to improve their PL QY from 11% to 89% for the emission of 451 nm. Furthermore, due to the continuous chelating reaction with the oxalate ion, chloride anions from the mixed‐halide CsPb(Cl/Br)₃ perovskite NCs could be extracted, and green emitting CsPbBr₃ NCs with PL QY of 85% at 511 nm emission are obtained. Besides being useful to improve the emission of CsPb(Cl/Br)₃ NCs, the oxalic acid treatment strategy introduced here provides a further tool to adjust the distribution of halide anions in mixed‐halide perovskites without using any halide additives.     

Perovskite‐Initiated Photopolymerization for Singly Dispersed Luminescent Nanocomposites

Metal halide perovskites have demonstrated rich photophysics and remarkable potential in photovoltaic and electroluminescent devices. However, the photoactivity of perovskite semiconductors in chemical processes remains relatively unexplored. Here, a general approach toward the synthesis of luminescent perovskite–polymer nanocomposites is reported, whereby perovskite nanocrystals are used as photoinitiators in the polymerization of vinyl monomers. The white‐light illumination of a perovskite–monomer mixture triggers a free‐radical chain‐growth polymerization process, giving rise to high molecular weight polymers of ≈200 kDa. The in situ growth of polymer chains from the perovskite crystal surface allows the formation of individually dispersed nanocrystal cores within an encapsulating polymer matrix, and leads to a significant threefold enhancement in photoluminescence quantum yield. This photoluminescence enhancement is attributed to the spatial separation of the perovskite nanocrystals and hence the deactivation of energy transfer to dark crystals. The resulting perovskite–polymer nanocomposites exhibit excellent stability against moisture and are shown to be useful as functional downconversion phosphor films for luminescent displays and lighting.     

Recent Developments in Top‐Emitting Organic Light‐Emitting Diodes

Organic light‐emitting diodes (OLEDs) have rapidly progressed in recent years due to their unique characteristics and potential applications in flat panel displays. Significant advancements in top‐emitting OLEDs have driven the development of large‐size screens and microdisplays with high resolution and large aperture ratio. After a brief introduction to the architecture and types of top‐emitting OLEDs, the microcavity theory typically used in top‐emitting OLEDs is described in detail here. Then, methods for producing and understanding monochromatic (red, green, and blue) and white top‐emitting OLEDs are summarized and discussed. Finally, the status of display development based on top‐emitting OLEDs is briefly addressed.     

A Building Brick Principle to Create Transparent Composite Films with Multicolor Emission and Self‐Healing Function

A cellulose paper is used impregnated with light‐emitting CdTe nanocrystals and carbon dots, and filled with a polyurethane to fabricate uniform transparent composite films with bright photoluminescence of red (R), green (G), and blue (B) (RGB) colors. A building brick‐like assembly method is introduced to realize RGB multicolor emission patterns from this composite material. By sectioning out individual pixels from monochrome‐emissive composite sheets, the advantage of the self‐healing properties of polyurethane is taken to arrange and weld them into a RGB patterned fabric by brief exposure to ethanol. This provides an approach to form single layer RGB light‐emitting pixels, such as potentially required in the display applications, without the use of any lithographic or etching processing. The method can utilize a wide range of different solution‐based kinds of light‐emitting materials.     

Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization

Multiple‐color‐emissive carbon dots (CDots) have potential applications in various fields such as bioimaging, light‐emitting devices, and photocatalysis. The majority of the current CDots to date exhibit excitation‐wavelength‐dependent emissions with their maximum emission limited at the blue‐light region. Here, a synthesis of multiple‐color‐emission CDots by controlled graphitization and surface function is reported. The CDots are synthesized through controlled thermal pyrolysis of citric acid and urea. By regulating the thermal‐pyrolysis temperature and ratio of reactants, the maximum emission of the resulting CDots gradually shifts from blue to red light, covering the entire light spectrum. Specifically, the emission position of the CDots can be tuned from 430 to 630 nm through controlling the extent of graphitization and the amount of surface functional groups, ? COOH. The relative photoluminescence quantum yields of the CDots with blue, green, and red emission reach up to 52.6%, 35.1%, and 12.9%, respectively. Furthermore, it is demonstrated that the CDots can be uniformly dispersed into epoxy resins and be fabricated as transparent CDots/epoxy composites for multiple‐color‐ and white‐light‐emitting devices. This research opens a door for developing low‐cost CDots as alternative phosphors for light‐emitting devices.     

Reducing Architecture Limitations for Efficient Blue Perovskite Light‐Emitting Diodes

Light‐emitting diodes utilizing perovskite nanocrystals have generated strong interest in the past several years, with green and red devices showing high efficiencies. Blue devices, however, have lagged significantly behind. Here, it is shown that the device architecture plays a key role in this lag and that NiO_x, a transport layer in one of the highest efficiency devices to date, causes a significant reduction in perovskite luminescence lifetime. An alternate transport layer structure which maintains robust nanocrystal emission is proposed. Devices with this architecture show external quantum efficiencies of 0.50% at 469 nm, seven times higher than state‐of‐the‐art devices at that wavelength. Finally, it is demonstrated that this architecture enables efficient devices across the entire blue‐green portion of the spectrum. The improvements demonstrated here open the door to efficient blue perovskite light‐emitting diodes.     

Highly Emissive Green Perovskite Nanocrystals in a Solid State Crystalline Matrix

Perovskite nanocrystals (NCs) have attracted attention due to their high photoluminescence quantum yield (PLQY) in solution; however, maintaining high emission efficiency in the solid state remains a challenge. This study presents a solution‐phase synthesis of efficient green‐emitting perovskite NCs (CsPbBr₃) embedded in robust and air‐stable rhombic prism hexabromide (Cs₄PbBr₆) microcrystals, reaching a PLQY of 90%. Theoretical modeling and experimental characterization suggest that lattice matching between the NCs and the matrix contribute to improved passivation, while spatial confinement enhances the radiative rate of the NCs. In addition, dispersing the NCs in a matrix prevents agglomeration, which explains their high PLQY.     

Controlled Integration of Nanocrystals in Inverted Hexagonal Nano‐Pits at the Surface of Light‐Emitting Heterostructures (Adv. Mater. 5/2008)

Hexagonal inverted nanopyramids on gallium‐nitride‐based multiple quantum wells are exploited to confine gold nanocrystals (NCs) at the surface of such light‐emitting heterostructures. The number of NCs incorporated in each pit can be controlled by nanoengineering either the NCs' size or the pit size. Capillarity effects can be used to drive the formation of well‐defined assemblies of Au NCs within each pit, as reported by Sérgio Pereira and co‐workers on p. 1038.