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Inorganic CsPbX3 perovskite quantum dots (PeQDs) show great potential in white light-emitting diodes (WLEDs) due to excellent optoelectronic properties, but their practical application is hampered by low photoluminescence quantum yield (PLQY) and especially poor stability. Herein, we developed an in-situ and general multidentate ligand passivation strategy that allows for CsPbX3 PeQDs not only near-unit PLQY, but significantly improved stability against storage, heat, and polar solvent. The enhanced optical property arises from high effectiveness of the multidentate ligand, diethylenetriaminepentaacetic acid (DTPA) with five carboxyl groups, in passivating uncoordinated Pb2+ defects and suppressing nonradiative recombination. First-principles calculations reveal that the excellent stability is attributed to tridentate binding mode of DTPA that remarkably boosts the adsorption capacity to PeQD core. Finally, combining the green and red PeQDs with blue chip, we demonstrated highly luminous WLEDs with distinctly enhanced operation stability, a wide color gamut of 121.3% of national television system committee, standard white light of (0.33,0.33) in CIE 1931, and tunable color temperatures from warm to cold white light readily by emitters' ratio. This study provides an operando yet general approach to achieve efficient and stable PeQDs for WLEDs and accelerates their progress to commercialization.
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Warm red-emitting praseodymium-doped LiSrVO4 phosphors were synthesized via solid-state reaction. The phase formation was verified using an X-ray diffraction study and the morphology was investigated using a scanning electron microscope study. The LiSrVO4 :Pr3+ phosphors emitted red light when exposed to ultraviolet light, indicating their possibility for use in warm white light-emitting diodes (WLEDs). Furthermore, the effect of charge compensators on the luminescence characteristics was addressed. The decay time was investigated using time-resolved photoluminescence. Furthermore, thermal quenching was analyzed through temperature-dependent photoluminescence spectra. Their sensitivity was calculated using temperature-dependent decay time analysis. The colour purity of the emitted light could be measured by photometric analysis. This comprehensive investigation provides a thorough understanding of the luminescence properties of phosphors for WLED applications.
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Luminescência , Luz Vermelha , Difração de Raios X , Raios Ultravioleta , TemperaturaRESUMO
Nitrides and oxynitrides isostructural to α-Si3N4 (M-α-SiAlON, M = Sr, Ca, Li) possess superb thermally stable photoluminescence (PL) properties, making them reliable phosphors for high-power solid-state lighting. However, the synthesis of phase-pure Sr-α-SiAlON still remains a great challenge and has only been reported for Sr below 1.35 at.% as the large size of Sr2+ ions tends to destabilize the α-SiAlON structure. Here, we succeeded to synthesize the single-phase powders of a unique 'Sr-rich' polytypoid α-SiAlON (Sr3Si24Al6N40:Eu2+) phosphor with three distinctive Sr/Eu luminescence sites using a solid-state remixing-reannealing process. The Sr content of this polytypoid structure exceeds those of a few previously reported structures by over 200%. The phase purity, composition, structure, and PL properties of this phosphor were investigated. A single phase can be obtained by firing the stoichiometric mixtures of all-nitride precursors at 2050°C under a 0.92 MPa N2 atmosphere. The Sr3Si24Al6N40:Eu2+ shows an intense orange-yellow emission, with the emission maximum of 590 nm and internal/external quantum efficiency of 66%/52% under 400 nm excitation. It also has a quite small thermal quenching, maintaining 93% emission intensity at 150°C. In comparison to Ca-α-SiAlON:Eu2+, this Sr counterpart shows superior quantum efficiency and thermal stability, enabling it to be an interesting orange-yellow down-conversion luminescent material for white LEDs. The experimental confirmation of the existence of such 'Sr-rich' SiAlON systems, in a single-phase powder form, paves the way for the design and synthesis of novel 'Sr-rich' SiAlON-based phosphor powders with unparalleled properties.
A distinctive orange-yellow-emitting 'Sr-rich' α-SiAlON-based phosphor with quite small thermal quenching (93% PL intensity at 150°C) that can surprisingly be synthesized in a single-phase powder form for white LEDs.
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Because of their exceptional physical and thermal properties, cellulose nanocrystals (CNCs) are a highly promising bio-based material for reinforcing fillers. Studies have revealed that some functional groups from CNCs can be used as a capping ligand to coordinate with metal nanoparticles or semiconductor quantum dots during the fabrication of novel complex materials. Therefore, through CNCs ligand encapsulation and electrospinning, perovskite-NC-embedded nanofibers with exceptional optical and thermal stability are demonstrated. The results indicate that, after continuous irradiation or heat cycling, the relative photoluminescence (PL) emission intensity of the CNCs-capped perovskite-NC-embedded nanofibers is maintained at ≈90%. However, the relative PL emission intensity of both ligand-free and long-alkyl-ligand-doped perovskite-NC-embedded nanofibers decrease to almost 0%. These results are attributable to the formation of specific clusters of perovskite NCs along with the CNCs structure and thermal property improvement of polymers. CNCs-doped luminous complex materials offer a promising avenue for stability-demanding optoelectronic devices and other novel optical applications.
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Lanthanide-doped upconversion luminescent materials (LUCMs) have attracted much attention in diverse practical applications because of their superior features. However, the relatively weak luminescence intensity and low efficiency of LUCMs are the bottleneck problems that seriously limit their development. Unfortunately, most of the current major strategies of luminescence enhancement have some inherent shortcomings in their implementation. Here, a new and simple strategy of molten salt-assisted synthesis is proposed to enhance lanthanide upconversion luminescence for the first time. As a proof-of-concept, a series of rare earth oxides with obvious luminescence enhancement are prepared by a one-step method, utilizing molten NaCl as the high-temperature reaction media and rare earth chlorides as the precursors. The enhancement factors at different reaction temperatures are systematically investigated by taking Yb3+ /Er3+ co-doped Y2 O3 as an example, which can be enhanced up to more than six times. In addition, the molten salts are extended to all alkali chlorides, indicating that it is a universal strategy. Finally, the potential application of obtained UCL materials is demonstrated in near-infrared excited upconversion white light-emitting diodes (WLEDs) and other monochromatic LEDs.
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In this study, pre-crystallization-controlled, solid-state preparation of red carbon dots (C-dots) from o-phenylenediamine on a hectogram scale with a 94% yield is reported. Highly efficient red phosphor (C-dots@MCC) is obtained by dispersing the C-dots in microcrystalline cellulose, which matched extremely well with the commercial Y3 Al5 O12 :Ce3+ (YAG) phosphor. White light-emitting diodes (WLEDs) fabricated from the two phosphors emitted warm white light with a correlated color temperature of 3845 K, CIE color coordinates of (0.38, 0.37), and an extremely high color rendering index (CRI) of 95, outperforming all the reported YAG-derived WLEDs. Furthermore, the CRI value of the WLED can be further increased to 97 after fine-tuning, which is the highest CRI for WLEDs of any C-dots derived devices reported so far. The superior performance of the WLED is attributed to a delicate energy transfer between YAG and C-dots@MCC. Most importantly, the WLED maintained excellent stabilities under varied currents, working durations, moistures, and temperatures.
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In order to achieve a high color-rendering index (CRI) and low correlated color temperature (CCT) indoor lighting, single-component phosphors with broad-band dual emission are in high demand for white-light-emitting diodes (WLEDs). However, phosphors with such fluorescent properties are rare at present. Herein, we report a facile solid-state chemical method for the synthesis of single-component phosphor with broad-band emission and a large Stokes shift that can meet the requirements of future white-light sources. These new tetrabutylammonium copper halides phosphors have excellent warm white emission characteristics, and their luminescence peaks are located at 494 and 654â nm. The optimized photoluminescence (PL) quantum yield can reach 93.7 %. The typical CIE coordinate of the as-fabricated WLED is at (0.3620, 0.3731) with a CRI of 89 and low CCT of 4516â K.
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The application of multiple quantum dots (QDs) in the field of white light emitting diodes (WLEDs) is still an important challenge due to their low luminous efficiency and quenching phenomenon. In this paper, we prepared AgInS2 QDs/zeolitic imidazolate framework-70 (AIS/ZIF-70) composite by a microwave hydrothermal method. Owing to the high porosity and stability of ZIF-70, it could effectively prevent quenching issues due to the aggregation of QDs. Since the ZIF-70 and QDs were chemically bonded, the formation of the ZnS layer could effectively passivate the surface defect and thus the quantum yield reached 21.49 % in aqueous solution. The luminous efficiency (LE) of the assembled AIS/ZIF-based WLED was reinforced by 6.8â times with a molar ratio of AgIn/Zn=18, i. e. at 5.26 % molar fraction of ZIF-70. Moreover, the color rendering index (CRI) and correlated color temperature (CCT) of AIS/ZIF-based WLED were 84.3 and 3631â K, respectively, indicating its potential application in solid-state lighting.
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Nitrogen-doped carbon dots (NCDs), exhibiting strong yellow emission in aqueous solution and solid matrices, have been utilized for fabricating heterostructure white electroluminescence devices. These devices consist of nitrogen-doped carbon dots as an emissive layer sandwiched between an organic hole transport layer (PEDOT:PSS) and an array of rutile TiO2nanorods, acting as an electron transport layer. Under an applied forward bias of 5 V, the device exhibits broadband electroluminescence covering the wavelength range of 390-900 nm, resulting in pure white light emission characteristics at room temperature. The result demonstrates the successful fabrication of all solution-processed, low-cost, eco-friendly NCDs-based LEDs with CIE (Commission Internationale d'Éclairage) coordinate of (0.31, 0.34) and color rendering index (CRI) > 90, which are close to ideal white light emission characteristics. The device functionalities are achieved based on defect-related NIR emission from TiO2nanorods array and visible emission from nitrogen-doped carbon dots. This result paves a new opportunity to develop low-cost, solution-processed nitrogen-doped carbon dots based on warm White light emitting diodes with high CRI for large-area display and lighting applications.
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Lead-halide perovskites have come to dominate the emerging photovoltaics research scene over the past decade. But whilst perovskite photovoltaics exhibit exceptional efficiencies, their limited stability, as well as the toxicity of their lead component remain challenges. This focus collection captures a snapshot of the efforts in the community to address these challenges, from modifications to the synthesis and device structure of perovskite photovoltaics to improve their stability, through to efforts to understand, develop, and improve lead-free perovskite-inspired materials (PIMs). PIMs range from direct perovskite-derivatives (e.g. CsSnI3or halide elpasolites) through to electronic analogs (e.g. BiOI). The collection discusses the application of these materials not only for solar cells, but also more broadly for photodetection, light emission, and anti-counterfeiting devices. This collection emphasizes the diversity of strategies and directions in this field, as well as its highly interdisciplinary nature.
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This study synthesized BaMoO4:Eu3+ red phosphors using the microwave method. In addition, the phase composition, morphology, and luminescence properties of the red phosphors were characterized using X-ray diffraction, field-scanning electron microscopy, and photoluminescence spectroscopy. The results revealed that doping red phosphors with different concentrations of Eu3+ does not change the crystal structure of the matrix material. The BaMoO4 :Eu3+ phosphors exhibited micron-scale irregular polyhedra, which could be excited by ultraviolet light with a wavelength of 395 nm to induce red-light emission. The optimal dosage of Eu3+ was 0.08, and the chromaticity coordinates of BaMoO4 :0.08Eu3+ phosphors were (0.5869, 0.3099). White light-emitting diode (w-LED) devices manufactured by using a combination of BaMoO4 :0.08Eu3+ phosphor and commercially available phosphors exhibited good white-light emission under the excitation of an ultraviolet chip. The BaMoO4 :0.08Eu3+ red phosphors that rapidly synthesized under the microwave field are expected to be used in w-LED devices.
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Európio , Micro-Ondas , Európio/química , Luz , Luminescência , Raios UltravioletaRESUMO
The rapid development of solid-state lighting technology has attracted much attention for searching efficient and stable luminescent materials, especially the single-component white-light emitter. Here, we adopt a facile ion-doping technology to synthesize vacancy-ordered double perovskite Cs2ZrCl6:Sb. The introduction of Sb3+ ions with a 5s2 active lone pair into Cs2ZrCl6 host stimulates the singlet (blue) and triplet (orange) states emission of Sb3+ ions, and their relative emission intensity can be tuned through the energy transfer from singlet to triplet states. Benefiting from the dual-band emission as a pair of perfect complementary colors, the optimum Cs2ZrCl6:1.5%Sb exhibits a high-quality white emission with a color-rendering index of 96. By employing Cs2ZrCl6:1.5%Sb as the down-conversion phosphor, stable single-component white light-emitting diodes with a record half-lifetime of 2003 h were further fabricated. This study puts forward an effective ion-doping strategy to design single-component white-light emitter, making practical applications of them in lighting technologies a real possibility.
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Low-color-temperature light-emitting diodes (LEDs) (called 1900 K LEDs for short) have the potential to become a healthy light source due to their blue-free property. Our previous research demonstrated that these LEDs posed no harm to retinal cells and even protected the ocular surface. Treatment targeting the retinal pigment epithelium (RPE) is a promising direction for age-related macular degeneration (AMD). Nevertheless, no study has evaluated the protective effects of these LEDs on RPE. Therefore, we used the ARPE-19 cell line and zebrafish to explore the protective effects of 1900 K LEDs. Our results showed that the 1900 K LEDs could increase the cell vitality of ARPE-19 cells at different irradiances, with the most pronounced effect at 10 W/m2. Moreover, the protective effect increased with time. Pretreatment with 1900 K LEDs could protect the RPE from death after hydrogen peroxide (H2O2) damage by reducing reactive oxygen species (ROS) generation and mitochondrial damage caused by H2O2. In addition, we preliminarily demonstrated that irradiation with 1900 K LEDs in zebrafish did not cause retinal damage. To sum up, we provide evidence for the protective effects of 1900 K LEDs on the RPE, laying the foundation for future light therapy using these LEDs.
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Antioxidantes , Epitélio Pigmentado da Retina , Animais , Epitélio Pigmentado da Retina/metabolismo , Antioxidantes/farmacologia , Estresse Oxidativo/efeitos da radiação , Peixe-Zebra/metabolismo , Peróxido de Hidrogênio/metabolismo , Espécies Reativas de Oxigênio/metabolismo , LuzRESUMO
Double perovskites (DPs) are one of the most promising candidates for developing white light-emitting diodes (WLEDs) owing to their intrinsic broadband emission from self-trapped excitons (STEs). Translation of three-dimensional (3D) DPs to one-dimensional (1D) analogues, which could break the octahedral tolerance factor limit, is so far remaining unexplored. Herein, by employing a fluorinated organic cation, we report a series of highly luminescent 1D DP-inspired materials, (DFPD)2 MI InBr6 (DFPD=4,4-difluoropiperidinium, MI =K+ and Rb+ ). Highly efficient warm-white photoluminescence quantum yield of 92 % is achieved by doping 0.3 % Sb3+ in (DFPD)2 KInBr6 . Furthermore, single-component warm-WLEDs fabricated with (DFPD)2 KInBr6 :Sb yield a luminance of 300 cd/m2 , which is one of the best-performing lead-free metal-halides WLEDs reported so far. Our study expands the scope of In-based metal-halides from 3D to 1D, which exhibit superior optical performances and broad application prospects.
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Luminescent materials are indispensable for applications in lighting, displays and photovoltaics, which can transfer, absorb, store and utilize light energy. Their performance is closely related with their size and morphologies, exact atomic arrangement, and local configuration about photofunctional centers. Advanced electron microscopy-based techniques have enabled the possibility to study nanostructures with atomic resolution. Especially, with the advanced micro-electro-mechanical systems, it is able to characterize the luminescent materials at the atomic scale under various environments, providing a deep understanding of the luminescent mechanism. Accordingly, this review summarizes the recent achievements of microscopic study to directly image the microstructure and local environment of activators in lanthanide and manganese (Ln/Mn2+ )-doped luminescent materials, including: 1) bulk materials, the typical systems are nitride/oxynitride phosphors; and 2) nanomaterials, such as nanocrystals (hexagonal-phase NaLnF4 and perovskite) and 2D nanosheets (Ca2 Ta3 O10 and MoS2 ). Finally, the challenges and limitations are highlighted, and some possible solutions to facilitate the developments of advanced luminescent materials are provided.
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Conventional synthesis of carbon dots (CDs) mostly involves a hydrothermal or solvent-thermal reaction which needs relatively high temperature and pressure. In this work, ionic liquid is used to assist in fast synthesizing CDs with an ultrahigh photoluminescent quantum yield (98.5%) by heating at a low temperature (≤100 °C) and at atmospheric pressure. In addition, through this approach, tunable multicolor emissive CDs can be successfully achieved and used for preparing high-performance white light-emitting diodes. Theoretical computation proves that the activity of synthesis reaction can be significantly enhanced by ionic liquids. Density functional theory calculation reveals that the size and graphite nitrogen ratios of CDs have an effect on bandgap reduction, resulting in a redshift of the emission, which is in good agreement with the experimental results. This simple and promising approach for fast synthesis of tunable emissive CDs using ionic liquid affords the facilitation of CDs-based luminescent materials for fast manufacturing of functional devices.
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Líquidos Iônicos , Pontos Quânticos , Carbono , Fluorescência , NitrogênioRESUMO
Colloidal all-inorganic perovskites nanocrystals (NCs) have emerged as a promising material for display and lighting due to their excellent optical properties. However, blue emissive NCs usually suffer from low photoluminescence quantum yields (PLQYs) and poor stability, rendering them the bottleneck for full-color all-perovskite optoelectronic applications. Herein, a facile approach is reported to enhance the emission efficiency and stability of blue emissive perovskite nano-structures via surface passivation with potassium bromide. By adding potassium oleate and excess PbBr2 to the perovskite precursor solutions, potassium bromide-passivated (KBr-passivated) blue-emitting (≈450 nm) CsPbBr3 nanoplatelets (NPLs) is successfully synthesized with a respectably high PLQY of 87%. In sharp contrast to most reported perovskite NPLs, no shifting in emission wavelength is observed in these passivated NPLs even after prolonged exposures to intense irradiations and elevated temperature, clearly revealing their excellent photo- and thermal-stabilities. The enhancements are attributed to the formation of K-Br bonding on the surface which suppresses ion migration and formation of Br-vacancies, thus improving both the PL emission and stability of CsPbBr3 NPLs. Furthermore, all-perovskite white light-emitting diodes (WLEDs) are successfully constructed, suggesting that the proposed KBr-passivated strategy can promote the development of the perovskite family for a wider range of optoelectronic applications.
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Carbon dots (CDs) as one of the most promising carbon-based nanomaterials are inspiring extensive research in optoelectronic applications. White-light-emitting diodes (WLEDs) with tunable correlated color temperatures (CCTs) are crucial for applications in white lighting. However, the development of high-performance CDs-based electroluminescent WLEDs, especially those with adjustable CCTs, remains a challenge. Herein, white CDs-LEDs with CCTs from 2863 to 11 240 K are successfully demonstrated by utilizing aggregation-induced emission red-shifting and broadening of CDs. As a result, a series of warm white, pure white, and cold white CDs-LEDs are realized with adjustable emissions in sequence along the blackbody radiation curve. These CDs-LEDs reach maximum brightness and external quantum efficiency up to 1414-4917 cd m-2 and 0.08-0.87%, respectively, which is among the best performances of white CDs-LEDs. To the best of the authors' knowledge, this is the first time that CCT-tunable white electroluminescent CDs-LEDs are demonstrated through controlling the aggregation degrees of CDs.
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Carbon dots (CDs) are widely studied for years due to their unique luminescent properties and potential applications in many fields. However, aggregation-caused quenching, monotonous emission modes, and unsustainable preparation impose restrictions on their performance and practical applications. Here, this work reports the facile synthesis of sustainable silk-derived multimode emitting CDs with dispersed-state fluorescence (DSF), aggregation-induced fluorescence (AIF), and aggregation-induced room temperature phosphorescence (AIRTP) through radiating sericin proteins in a household microwave oven (800 W, 2.5 min). The structure, luminescent properties, and the mechanism are investigated and discussed. The sericin-derived CDs have graphitized cores and heteroatom-cluster-rich surfaces. The DSF corresponds to the graphitized cores and the AIF origins from the aggregation-induced abundant orbital energy levels on the heteroatom-cluster-rich surfaces. The presence of abundant hydrogen bonds and small gap between the lowest singlet and triplet excited states induces AIRTP. Finally, based on the unique multimode emission of the prepared CDs, their applications in high-performance white-light-emitting diode, information encryption, anti-counterfeiting, and visual humidity sensors are demonstrated.
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Carbono , Pontos Quânticos , Fluorescência , Luminescência , SedaRESUMO
Here, we show the fabrication of the carbon dots (CDs) with green and orange emissions from PTCDA (perylene-3,4,9,10-tetracarboxylic dianhydride). Using these CDs as emitters, the orange (or green) CDs LEDs were fabricated, which show electroluminescence (EL) spectra centered at 560â nm (or 498â nm) with an external quantum efficiency (EQE) of 1.98 % (1.76 %) adhering a luminescence of 626â cd m-2 (or 519â cd m-2 ). The machine learning was successfully used to predict PL CCT value. With the model, the white photoluminescence (PL) emission with adjustable correlated color temperature (CCT) from 3093 to 11018â K via combining blue, green, and orange CDs was achieved. Then, we obtained the warm white CDs LEDs with CCT of 3107, 4071 and 4548â K, and cold white CDs LEDs with CCT of 5632 (CIE coordinates of (0.33, 0.33), EQE: 1.18 %, luminescence: 598â cd m-2 ) and 6034â K accurately.