Addressable and Color‐Tunable Piezophotonic Light‐Emitting Stripes

Piezophotonic light‐emitting devices have great potential for future microelectromechanical systems (MEMS) and nanoelectromechanical systems (NEMS) due to the added functionality provided by the electromechanical transduction coupled with the ability of light emission. Piezophotonic light‐emitting source based on Pb(Mg_1/3Nb_2/3)O₃–PbTiO₃ (PMN–PT) bulk is severely restricted by many challenges, such as high voltage burden, low integration density, and micromanufacturing complexity. Developing chip‐integrated devices or incorporating such photonic components onto a Si platform is highly sought after in this field. In this work, the authors overcome the abovementioned problems by introducing single‐crystal PMN–PT thin films on Si as central active elements. Taking advantage of mature microfabrication techniques, arrays of PMN–PT actuators with small footprints and low operation voltages have been implemented. Each actuator can be individually addressed, generating local deformation to trigger piezophotonic luminescence from ZnS:Mn thin films. Moreover, the authors have realized continuous and reversible color manipulation of piezophotonic luminescence on a bilayer film of ZnS:Cu,Al/ZnS:Mn. The color tunability promises an extra degree of freedom and distinctly suggests its great potential in developing a more compact and colorful piezophotonic light sources and displays related applications together with the “single pixel” addressability.     

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.     

Wavelength‐Tunable Electroluminescent Light Sources from Individual Ga‐Doped ZnO Microwires

Electrically driven wavelength‐tunable light emission from biased individual Ga‐doped ZnO microwires (ZnO:Ga MWs) is demonstrated. Single crystalline ZnO:Ga MWs with different Ga‐doping concentrations have been synthesized using a one‐step chemical vapor deposition method. Strong electrically driven light emission from individual ZnO:Ga MW based devices is realized with tunable colors, and the emission region is localized toward the center of the wires. Increasing Ga‐doping concentration in the MWs can lead to the redshift of electroluminescent emissions in the visible range. Interestingly, owing to the lack of rectification characteristics, relevant electrical measurement results show that the alternating current‐driven light emission functions excellently on the ZnO:Ga MWs. Consequently, individual ZnO:Ga MWs, which can be analogous to incandescent sources, offer unique possibilities for future electroluminescence light sources. This typical multicolor emitter can be used to rival and complement other conventional semiconductor devices in displays and lighting.     

Designable Luminescence with Quantum Dot–Silver Plasmon Coupler

We explore a strongly interacting QDs/Ag plasmonic coupling structure that enables multiple approaches to manipulate light emission from QDs. Group II–VI semiconductor QDs with unique surface states (SSs) impressively modify the plasmonic character of the contiguous Ag nanostructures whereby the localized plasmons (LPs) in the Ag nanostructures can effectively extract the non‐radiative SSs of the QDs to radiatively emit via SS–LP resonance. The SS–LP coupling is demonstrated to be readily tunable through surface‐state engineering both during QD synthesis and in the post‐synthesis stage. The combination of surface‐state engineering and band‐tailoring engineering allows us to precisely control the luminescence color of the QDs and enables the realization of white‐light emission with single‐size QDs. Being a versatile metal, the Ag in our optical device functions in multiple ways: as a support for the LPs, for optical reflection, and for electrical conduction. Two application examples of the QDs/Ag plasmon coupler for optical devices are given, an Ag microcavity + plasmon‐coupling structure and a new QD light‐emitting diode. The new QDs/Ag plasmon coupler opens exciting possibilities in developing novel light sources and biomarker detectors.     

Strategies to Improve Luminescence Efficiency of Metal‐Halide Perovskites and Light‐Emitting Diodes

Metal‐halide perovskites (MHPs) are well suited to be vivid natural color emitters due to their superior optical and electrical properties, such as narrow emission linewidths, easily and widely tunable emission wavelengths, low material cost, and high charge carrier mobility. Since the first development of MHP light‐emitting diodes (PeLEDs) in 2014, many researchers have tried to understand the properties of MHP emitters and the limitations to luminescence efficiency (LE) of PeLEDs, and have devoted efforts to increase the LE of MHP emitters and PeLEDs. Within three and half years, PeLEDs have shown rapidly increased LE from external quantum efficiency ≈0.1% to ≈14.36%. Herein, the factors that limit the LE of PeLEDs are reviewed; the factors are characterized into the following groups: i) photophysical properties of MHP crystals, ii) morphological factors of MHP layers, and iii) problems caused by device architectures. Then, the strategies to overcome those luminescence‐limiting factors in MHP emitters and PeLEDs are critically evaluated. Finally, research directions to further increase the LE of MHP emitters and the potential of MHPs as a core component in next‐generation displays and solid‐state lightings are suggested.     

A ZnS/CaZnOS Heterojunction for Efficient Mechanical-to-Optical Energy Conversion by Conduction Band Offset

Actively collecting the mechanical energy by efficient conversion to other forms of energy such as light opens a new possibility of energy-saving, which is of pivotal significance for supplying potential solutions for the present energy crisis. Such energy conversion has shown promising applications in modern sensors, actuators, and energy harvesting. However, the implementation of such technologies is being hindered because most luminescent materials show weak and non-recoverable emissions under mechanical excitation. Herein, a new class of heterojunctioned ZnS/CaZnOS piezophotonic systems is presented, which displays highly reproducible mechanoluminescence (ML) with an unprecedented intensity of over two times higher than that of the widely used commercial ZnS (the state-of-the-art ML material). Density functional theory calculations reveal that the high-performance ML originates from efficient charge transfer and recombination through offset of the valence and conduction bands in the heterojunction interface region. By controlling the ZnS-to-CaZnOS ratio in conjunction with manganese (Mn²⁺) and lanthanide (Ln³⁺) doping, tunable ML across the full spectrum is activated by a small mechanical stimulus of 1 N (10 kPa). The findings demonstrate a novel strategy for constructing efficient ML materials by leveraging interface effects and ultimately promoting practical applications for ML.     

Inside Front Cover: Redox‐Tunable Defects in Colloidal Photonic Crystals (Adv. Mater. 20/2005)

The inside front cover illustrates reversible tuning of an intragap transmitting state induced by redox cycling, accomplished using a redox‐active polyferrocenylsilane polyelectrolyte multilayer planar defect embedded in a colloidal photonic crystal (CPC) synthesized by a bottom–up method combining colloidal self‐assembly and microcontact printing. In work reported on p. 2455 by Manners, Ozin, and co‐workers, the wavelength position of the defect state can be changed by changing the oxidation state of the ferrocene moieties in the polymer backbone. This could find applications in electrochemically tunable microcavities, and—if light emitters are incorporated—electrochemically tunable CPC‐based laser sources. Cover design by Ludovic Cademartiri.     

Spontaneous Self‐Assembly of Perovskite Nanocrystals into Electronically Coupled Supercrystals: Toward Filling the Green Gap

Self‐assembly of nanoscale building blocks into ordered nanoarchitectures has emerged as a simple and powerful approach for tailoring the nanoscale properties and the opportunities of using these properties for the development of novel optoelectronic nanodevices. Here, the one‐pot synthesis of CsPbBr₃ perovskite supercrystals (SCs) in a colloidal dispersion by ultrasonication is reported. The growth of the SCs occurs through the spontaneous self‐assembly of individual nanocrystals (NCs), which form in highly concentrated solutions of precursor powders. The SCs retain the high photoluminescence (PL) efficiency of their NC subunits, however also exhibit a redshifted emission wavelength compared to that of the individual nanocubes due to interparticle electronic coupling. This redshift makes the SCs pure green emitters with PL maxima at ≈530–535 nm, while the individual nanocubes emit a cyan‐green color (≈512 nm). The SCs can be used as an emissive layer in the fabrication of pure green light‐emitting devices on rigid or flexible substrates. Moreover, the PL emission color is tunable across the visible range by employing a well‐established halide ion exchange reaction on the obtained CsPbBr₃ SCs. These results highlight the promise of perovskite SCs for light emitting applications, while providing insight into their collective optical properties.     

Aggregation‐Induced Dual‐Phosphorescence from Organic Molecules for Nondoped Light‐Emitting Diodes

Aggregation‐induced emission (AIE) is a beneficial strategy for generating highly effective solid‐state molecular luminescence without suffering losses in quantum yield. However, the majority of reported AIE‐active molecules exhibit only strong fluorescence, which is not ideal for electrical excitation in organic light‐emitting diodes (OLEDs). By introducing various substituent groups onto the biscarbazole compound, a series of molecular materials with aggregation‐induced phosphorescence (AIP) is designed, which exhibits two distinctly different phosphorescence bands and an absolute solid‐state room‐temperature phosphorescence quantum yield up to 64%. Taking advantage of the AIE feature, the AIP molecules are fabricated into OLEDs as a homogeneous light‐emitting layer, which allows for relatively small efficiency roll‐off and shows an external electroluminescence quantum yield of up to 5.8%, more than the theoretical limit for purely fluorescent OLED devices. The design showcases a promising strategy for the production of cost‐effective and highly efficient OLED technology.     

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.     

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.     

Tunable Resonator‐Upconverted Emission (TRUE) Color Printing and Applications in Optical Security

Lanthanide‐doped nanophosphors are promising in anti‐counterfeiting and security printing applications. These nanophosphors can be incorporated as transparent inks that fluoresce by upconverting near‐infrared illumination into visible light to allow easy verification of documents. However, these inks typically exhibit a single luminescent color, low emission efficiency, and low print resolutions. Tunable resonator‐upconverted emission (TRUE) is achieved by placing upconversion nanoparticles (UCNPs) within plasmonic nanoresonators. A range of TRUE colors are obtained from a single‐UCNP species self‐assembled within size‐tuned gap‐plasmon resonances in Al nanodisk arrays. The luminescence intensities are enhanced by two orders of magnitude through emission and absorption enhancements. The enhanced emissive and plasmonic colors are simultaneously employed to generate TRUE color prints that exhibit one appearance under ambient white light, and a multicolored luminescence appearance that is revealed under near‐infrared excitation. The printed color and luminescent images are of ultrahigh resolutions (≈50 000 dpi), and enable multiple colors from a single excitation source for increased level of security.     

Layered Rare‐Earth Hydroxide/Polyacrylamide Nanocomposite Hydrogels with Highly Tunable Photoluminescence

Polymer nanocomposite (NC) hydrogels, with 3D networks composed of delaminated inorganic nanoparticles and a polymer matrix, usually display super mechanical toughness. However, the few types of inorganic materials and relatively scarce research for NC hydrogel functions seriously limit their applications. For the first time layered rare‐earth hydroxide (LRH)/polyacrylamide NC hydrogels with highly tunable photoluminescence (PL) function are reported, prepared via a convenient and green in situ polymerization process. Interestingly, the NC hydrogels reveal exciting multicolored PL phenomenon (green, yellow, orange, reddish‐orange to bluish violet), long luminescence lifetime, and relatively high quantum efficiency. Furthermore, the fascinating PL function is highly tunable by adjusting LRH constituent or its concentration, and excitation wavelength. The results highlight the fabrication and applications of functional polymer NC hydrogels with highly tunable PL function.     

Highly Deformable and See‐Through Polymer Light‐Emitting Diodes with All‐Conducting‐Polymer Electrodes

Despite the high expectation of deformable and see‐through displays for future ubiquitous society, current light‐emitting diodes (LEDs) fail to meet the desired mechanical and optical properties, mainly because of the fragile transparent conducting oxides and opaque metal electrodes. Here, by introducing a highly conductive nanofibrillated conducting polymer (CP) as both deformable transparent anode and cathode, ultraflexible and see‐through polymer LEDs (PLEDs) are demonstrated. The CP‐based PLEDs exhibit outstanding dual‐side light‐outcoupling performance with a high optical transmittance of 75% at a wavelength of 550 nm and with an excellent mechanical durability of 9% bending strain. Moreover, the CP‐based PLEDs fabricated on 4 µm thick plastic foils with all‐solution processing have extremely deformable and foldable light‐emitting functionality. This approach is expected to open a new avenue for developing wearable and attachable transparent displays.     

A Fluorescence–Phosphorescence–Phosphorescence Triple‐Channel Emission Strategy for Full‐Color Luminescence

Organic luminogens constitute promising prototypes for various optoelectronic applications. Since gaining distinct color emissions normally requires the alternation of the conjugated backbone, big issues remain in material synthetic cost and skeleton compatibility while pursuing full‐color luminescence. Upon a facile one‐step coupling, three simple but smart perchalcogenated (O, S, and Se) arenes are synthesized. They exhibit strong luminescent tricolor primaries (i.e., blue, green, and red, respectively) in the solid state with a superior quantum yield up to >40% (5–10 times higher than that in corresponding solutions). The properties originate from a fluorescence–phosphorescence–phosphorescence triple‐channel emission effect, which is regulated by S and Se heavy atoms–dependent intersystem crossing upon molecular packing, as well as Se–Se atom interaction–caused energy splittings. Consequently, full‐color luminescence, including a typical white‐light luminescence with a Commission Internationale de I'Eclairage coordinate of (0.30, 0.35), is realized by complementarily incorporating these tricolor luminescent materials in the film. Moreover, mechanochromic luminescent color conversions are also observed to achieve the fine‐tuning of the luminescent tints. This strategy can be smart to address full‐color luminescence on the same molecular skeleton, showing better material compatibility as an alternative to the traditional multiple‐luminophore engineering.     

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.     

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.     

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

As emerging efficient emitters, metal‐halide perovskites offer the intriguing potential to the low‐cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron–hole pairs). Here, Sn‐triggered extrinsic self‐trapping of excitons in bulk 2D perovskite crystal, PEA₂PbI₄ (PEA = phenylethylammonium), is reported, where exciton self‐trapping never occurs in its pure state. By creating local potential wells, isoelectronic Sn dopants initiate the localization of excitons, which would further induce the large lattice deformation around the impurities to accommodate the self‐trapped excitons. With such self‐trapped states, the Sn‐doped perovskites generate broadband red‐to‐near‐infrared (NIR) emission at room temperature due to strong exciton–phonon coupling, with a remarkable quantum yield increase from 0.7% to 6.0% (8.6 folds), reaching 42.3% under a 100 mW cm^?2 excitation by extrapolation. The quantum yield enhancement stems from substantial higher thermal quench activation energy of self‐trapped excitons than that of free excitons (120 vs 35 meV). It is further revealed that the fast exciton diffusion involves in the initial energy transfer step by transient absorption spectroscopy. This dopant‐induced extrinsic exciton self‐trapping approach paves the way for extending the spectral range of perovskite emitters, and may find emerging application in efficient supercontinuum sources.     

Light‐Emitting Diodes with Cu‐Doped Colloidal Quantum Wells: From Ultrapure Green,Tunable Dual‐Emission to White Light

Copper‐doped colloidal quantum wells (Cu‐CQWs) are considered a new class of optoelectronic materials. To date, the electroluminescence (EL) property of Cu‐CQWs has not been revealed. Additionally, it is desirable to achieve ultrapure green, tunable dual‐emission and white light to satisfy the various requirement of display and lighting applications. Herein, light‐emitting diodes (LEDs) based on colloidal Cu‐CQWs are demonstrated. For the 0% Cu‐doped concentration, the LED exhibits Commission Internationale de L'Eclairage 1931 coordinates of (0.103, 0.797) with a narrow EL full‐wavelength at half‐maximum of 12 nm. For the 0.5% Cu‐doped concentration, a dual‐emission LED is realized. Remarkably, the dual emission can be tuned by manipulating the device engineering. Furthermore, at a high doping concentration of 2.4%, a white LED based on CQWs is developed. With the management of doping concentrations, the color tuning (green, dual‐emission to white) is shown. The findings not only show that LEDs with CQWs can exhibit polychromatic emission but also unlock a new direction to develop LEDs by exploiting 2D impurity‐doped CQWs that can be further extended to the application of other impurities (e.g., Mn, Ag).