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CsPbI3 perovskite quantum dots (QDs) could achieve pure-red emission by reducing their size, but the increased exciton binding energy (EB) and surface defects for the small-sized QDs (SQDs) cause severe Auger and trap recombinations, thus worsening their electroluminescence (EL) performance. Herein, we utilize the dangling bonds of the SQDs as a driving force to accelerate KI dissolution to solve its low solubility in nonpolar solvents, thereby allowing K+ and I- to bond to the surface of SQDs. The EB of the SQDs was decreased from 305 to 51 meV because of the attraction of K+ to electrons, meanwhile surface vacancies were passivated by K+ and I-. The Auger and trap recombinations were simultaneously suppressed by this difunctional ligand. The SQD-based light-emitting diode showed a stable pure-red EL peak of 639 nm, an external quantum efficiency of 25.1% with low roll-off, and a brightness of 5934 cd m-2.
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ZnTe colloidal semiconductor nanocrystals (NCs) have shown promise for light-emitting diodes (LEDs) and displays, because they are free from toxic heavy metals (Cd). However, so far, their low photoluminescence (PL) efficiency (â¼30%) has hindered their applications. Herein, we devised a novel structure of ZnTe NCs with the configuration of ZnSe (core)/ZnTe (spherical quantum well, SQW)/ZnSe (shell). The inner layer ZnTe was grown at the surface of ZnSe core with avoiding using highly active and high-risk Zn sources. Due to the formation of coherently strained heterostructure which reduced the lattice mismatch, and the thermodynamic growth of ZnTe, the surface or interface defects were suppressed. A high PL efficiency of >60% was obtained for the green light-emitting ZnSe/ZnTe/ZnSe SQWs after ZnS outer layer passivation, which is the highest value for colloidal ZnTe-based NCs. This work paves the way for the development of novel semiconductor NCs for luminescent and display applications.
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Colloidal quantum well (CQW) based light emitting diodes (LEDs) possess extra-high theoretical efficiency, but their performance still lags far behind conventional LEDs due to severe exciton quenching and unbalanced charge injection. Herein, we devised a gradient composition CdxZn1-xS shell to address these issues. The epitaxial shell with gradient composition was achieved through controlling competition between Cd2+ and Zn2+ cations to preferentially bind to the anions S2-. Thus, exciton quenching was suppressed greatly by passivating defects and reducing nonradiative recombination, thereby achieving near-unity photoluminescence quantum yield (PLQY). The gradient energy level of the shell reduced the hole injection barriers and increased the hole injection efficiency to balance the charge injection of LEDs. As a result, the LEDs achieved a high external quantum efficiency (EQE) of 22.83%, luminance of 111,319 cd/m2 and a long operational lifetime (T95@100 cd/m2) over 6,500 h, demonstrating the state-of-the-art performance for the CQW based LEDs.
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Environmentally friendly InP-based quantum dots (QDs) are promising for light-emitting diodes (LEDs) and display applications. So far, the synthesis of highly emitting InP-based QDs via safe and economically viable amine-phosphine remains a challenge. Herein, we report the synthesis of amine-phosphine based InP/ZnSe/ZnS QDs by introducing an alloyed oxidation-free In-ZnSe transition layer (TL) at the core-shell interface. The TL not only has the essential function of preventing oxidation of the core and relieving interfacial strain but also results in oriented epitaxial growth of shell. The alloyed TL significantly mitigates the nonradiative recombination at core-shell interfacial trap states, thereby boosting the photoluminescence (PL) efficiency of the QDs up to 98%. Also, the Auger recombination is suppressed, extending the biexciton lifetime from 60 to 100 ps. The electroluminescence device based on the InP-based QDs shows a high external quantum efficiency over 10%, further demonstrating high quality QDs synthesized by this process.
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Spectrally stable pure-red perovskite quantum dots (QDs) with low lead content are essential for high-definition displays but are difficult to synthesize due to QD self-purification. Here, we make use of entropy-driven quantum-confined pure-red perovskite QDs to fabricate light-emitting diodes (LEDs) that have low toxicity and are efficient and spectrum-stable. Based on experimental data and first-principles calculations, multiple element alloying results in a 60% reduction in lead content while improving QD entropy to promote crystal stability. Entropy-driven QDs exhibit photoluminescence with 100% quantum yields and single-exponential decay lifetimes without alteration of their morphology or crystal structure. The pure-red LEDs utilizing entropy-driven QDs have spectrally stable electroluminescence, achieving a brightness of 4932 cd/m2, a maximum external quantum efficiency of over 20%, and a 15-fold longer operational lifetime than the CsPbI3 QD-based LEDs. These achievements demonstrate that entropy-driven QDs can mitigate local compositional heterogeneity and ion migration.
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Double perovskite films have been extensively studied for ferroelectric order, ferromagnetic order, and photovoltaic effects. The customized ion combinations and ordered ionic arrangements provide unique opportunities for bandgap engineering. Here, a synergistic strategy to induce chemical strain and charge compensation through inequivalent element substitution is proposed. A-site substitution of the barium ion is used to modify the chemical valence and defect density of the two B-site elements in Bi2FeMnO6 double perovskite epitaxial thin films. We dramatically increased the ferroelectric photovoltaic effect to â¼135.67 µA/cm2 from 30.62 µA/cm2, which is the highest in ferroelectric thin films with a thickness of less than 100 nm under white-light LED irradiation. More importantly, the ferroelectric polarization can effectively improve the photovoltaic efficiency of more than 5 times. High-resolution HAADF-STEM, synchrotron-based X-ray diffraction and absorption spectroscopy, and DFT calculations collectively demonstrate that inequivalent ion plays a dual role of chemical strain (+1.92 and -1.04 GPa) and charge balance, thereby introducing lattice distortion effects. The reduction of the oxygen vacancy density and the competing Jahn-Teller distortion of the oxygen octahedron are the main phenomena of the change in electron-orbital hybridization, which also leads to enhanced ferroelectric polarization values and optical absorption. The inequivalent strategy can be extended to other double perovskite systems and applied to other functional materials, such as photocatalysis for efficient defect control.
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Potassium (K+) is one of the most abundant cations in the human body. Under normal conditions, the vast majority of K+ is found within cells, and the extracellular [K+] is tightly regulated to within 3.0 to 5.0 mM. However, it has recently been shown that high levels of localized necrosis can increase the extracellular concentration of K+ to above 50 mM. This raises the possibility that elevated extracellular K+ might influence a variety of biological processes that occur within regions of necrotic tissue. For example, K+ has been shown to play a central role in the replication cycles of numerous viral families, and in cases of lytic infection, localized regions containing large numbers of necrotic cells can be formed. Here, we show that the replication of the model poxvirus myxoma virus (MYXV) is delayed by elevated levels of extracellular K+. These increased K+ concentrations alter the cellular endocytic pathway, leading to increased phagocytosis but a loss of endosomal/lysosomal segregation. This slows the release of myxoma virus particles from the endosomes, resulting in delays in genome synthesis and infectious particle formation as well as reduced viral spread. Additionally, mathematical modeling predicts that the extracellular K+ concentrations required to impact myxoma virus replication can be reached in viral lesions under a variety of conditions. Taken together, these data suggest that the extracellular [K+] plays a role in determining the outcomes of myxoma infection and that this effect could be physiologically relevant during pathogenic infection. IMPORTANCE Intracellular K+ homeostasis has been shown to play a major role in the replication of numerous viral families. However, the potential impact of altered extracellular K+ concentrations is less well understood. Our work demonstrates that increased concentrations of extracellular K+ can delay the replication cycle of the model poxvirus MYXV by inhibiting virion release from the endosomes. Additionally, mathematical modeling predicts that the levels of extracellular K+ required to impact MYXV replication can likely be reached during pathogenic infection. These results suggest that localized viral infection can alter K+ homeostasis and that these alterations might directly affect viral pathogenesis.
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Myxoma virus , Humanos , Myxoma virus/genética , Potássio , Endossomos , Replicação Viral , VírionRESUMO
Here, we develop an in situ photoluminescence (PL) system to monitor the nucleation and growth of perovskite nanocrystals and control the monomer supply rate to achieve strongly confined and monodispersed quantum dots (QDs) with average size of 3.4 nm. Pure-blue (460 nm wavelength) CsPbBr3 QDs with near unity PL quantum yield and narrow size distribution (small size dispersion of 9.6%) were thus produced. Light-emitting diodes (LEDs) based on these QDs were prepared by using an all-solution processing route, which showed narrow electroluminescence with full width at half-maximum of 20 nm and a high color purity of 97.3%. The device also had a high external quantum efficiency of 10.1%, maximum luminance of 11â¯610 cd m-2, and continuous operation lifetime of 21 h at the initial luminance of 102 cd m-2, corresponding to the state-of-art for pure-blue perovskite LEDs.
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The additive engineering strategy promotes the efficiency of solution-processed perovskite solar cells (PSCs) over 25%. However, compositional heterogeneity and structural disorders occur in perovskite films with the addition of specific additives, making it imperative to understand the detrimental impact of additives on film quality and device performance. In this work, the double-edged sword effects of the methylammonium chloride (MACl) additive on the properties of methylammonium lead mixed-halide perovskite (MAPbI3-x Clx ) films and PSCs are demonstrated. MAPbI3-x Clx films suffer from undesirable morphology transition during annealing, and its impacts on the film quality including morphology, optical properties, structure, and defect evolution are systematically investigated, as well as the power conversion efficiency (PCE) evolution for related PSCs. The FAX (FA = formamidinium, X = I, Br, and Ac) post-treatment strategy is developed to inhibit the morphology transition and suppress defects by compensating for the loss of the organic components, a champion PCE of 21.49% with an impressive open-circuit voltage of 1.17 V is obtained, and remains over 95% of the initial efficiency after storing over 1200 hours. This study elucidates that understanding the additive-induced detrimental effects in halide perovskites is critical to achieve the efficient and stable PSCs.
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Starting from a deterministic model, we propose and study a stochastic model for human papillomavirus infection and cervical cancer progression. Our analysis shows that the chronic infection state as random variables which have the ergodic invariant probability measure is necessary for progression from infected cell population to cervical cancer cells. It is shown that small progression rate from infected cells to precancerous cells and small microenvironmental noises associated with the progression rate and viral infection help to establish such chronic infection states. It implicates that large environmental noises associated with viral infection and the progression rate in vivo can reduce chronic infection. We further show that there will be a cervical cancer if the noise associated with precancerous cell growth is large enough. In addition, comparable numerical studies for the deterministic model and stochastic model, together with Hopf bifurcations in both deterministic and stochastic systems, highlight our analytical results.
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Lesões Pré-Cancerosas , Neoplasias do Colo do Útero , Viroses , Humanos , Feminino , Papillomavirus Humano , Processos Estocásticos , Infecção PersistenteRESUMO
It is still challenging to achieve high-efficiency pure-red (620-650 nm wavelength) perovskite light-emitting diodes (PeLEDs). Herein, we report pure-red PeLEDs with Commission Internationale de l'Eclairage coordinates (0.703, 0.297) meeting the Rec. 2020, an external quantum efficiency of 20.8%, and a luminance of 3775 cd/m2. This design is based on the strong quantum confinement CsPbI3 quantum dots (QDs) capped by composite ligands of 3-phenyl-1-propylamine and tetrabutylammonium iodide. This strategy stabilized the structure of the strong-confined QDs and reduced the influence of the electric field-induced Stark effect on the PeLEDs. Furthermore, the exciton binding energy of the QDs was decreased by the composited ligands to suppress Auger recombination within the devices. Additionally, the valence-band maximum of the QDs was lifted to match the hole-transport layer, thus balancing charge injection in the PeLEDs. Our device also demonstrated a stable electroluminescence spectrum and a lifetime of 5.6 times longer than the control device.
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Perovskite colloidal quantum wells (QWs) are promising to realize narrow deep-blue emission, but the poor optical performance and stability suppress their practical application. Here, we creatively propose a water-driven synthesis strategy to obtain size-homogenized and strongly confined deep-blue CsPbBr3 QWs, corresponding to three monolayers, which emit at the deep-blue wavelength of 456â nm. The water controls the orientation and distribution of the ligands on the surface of the nanocrystals, thus inducing orientated growth through the Ostwald ripening process by phagocytizing unstable nanocrystals to form well-crystallized QWs. These QWs present remarkable stability and high photoluminescence quantum yield of 94 %. Furthermore, we have prepared light-emitting diodes based on the QWs via the all-solution fabrication strategy, achieving an external quantum efficiency of 1 % and luminance of 2946â cd m-2 , demonstrating state-of-the-art brightness for perovskite QW-based LEDs.
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Tin oxide (SnO2 ) nanocrystals-based electron transport layer (ETL) has been widely used in perovskite solar cells due to its high charge mobility and suitable energy band alignment with perovskite, but the high surface trap density of SnO2 nanocrystals harms the electron transfer and collection within device. Here, an effective method to achieve a low trap density and high electron mobility ETL based on SnO2 nanocrystals by devising a difunctional additive of potassium trifluoroacetate (KTFA) is proposed. KTFA is added to the SnO2 nanocrystals solution, in which trifluoroacetate ions could effectively passivate the oxygen vacancies (OV ) in SnO2 nanocrystals through binding of TFA- and Sn4+ , thus reducing the traps of SnO2 nanocrystals to boost the electrons collection in the solar cell. Furthermore, the conduction band of SnO2 nanocrystals is shifted up by surface modification to close to that of perovskite, which facilitates electrons transfer because of the decreased energy barrier between ETL and perovskite layer. Benefiting from the decreased trap density and energy barrier, the perovskite solar cells exhibit a power conversion efficiency of 21.73% with negligible hysteresis.
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Electrocatalytic CO2 reduction reaction (CO2 RR) toward formate production can be operated under mild conditions with high energy conversion efficiency while migrating the greenhouse effect. Herein, an integrated 3D open network of interconnected bismuthene arrays (3D Bi-ene-A/CM) is fabricated via in situ electrochemically topotactic transformation from BiOCOOH nanosheet arrays supported on the copper mesh. The resulted 3D Bi-ene-A/CM consists of 2D atomically thin metallic bismuthene (Bi-ene) in the form of an integrated array superstructure with a 3D interconnected and open network, which harvests the multiple structural advantages of both metallenes and self-supported electrodes for electrocatalysis. Such distinctive superstructure affords the maximized quantity and availability of the active sites with high intrinsic activity and superior charge and mass transfer capability, endowing the catalyst with good CO2 RR performance for stable formate production with high Faradaic efficiency (≈90%) and current density (>300 mA cm-2 ). Theoretical calculation verifies the superior intermediate stabilization of the dominant Bi plane during CO2 RR. Moreover, by further coupling anodic methanol oxidation reaction, an exotic electrolytic system enables highly energy-efficient and value-added pair-electrosynthesis for concurrent formate production at both electrodes, achieving substantially improved electrochemical and economic efficiency and revealing the feasibility for practical implementation.
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Tailoring the thermal expansion coefficient of negative thermal expansion (NTE) materials to achieve near-zero thermal expansion has attracted great attention recently. Here, LiFe diatoms are adopted to substitute Cu in Cu2P2O7 oxide to design Li-O-P and Fe-O-P linkages, with the stronger bond strength of Li-O and Fe-O compared to Cu-O and hence lowering the bond strength of P-O. With increasing the diatomic LiFe in (LiFe)0.5xCu2-xP2O7, new Raman bands corresponding to LiFeP2O7 appear and the NTE coefficient decreases gradually to near-zero thermal expansion at x = 1 (αv = -0.90 × 10-6 °C-1, -100 to 55 °C). Comparing (LiFe)0.5CuP2O7 with Cu2P2O7 and LiFeP2O7, the average bond length of P-O increases while the bond angle of P-O-P decreases, and this is verified by some weakened vibrational energies of terminal PO3 and P-O-P, resulting in the obvious red shift of Raman bands. Ceramic (LiFe)0.5CuP2O7 presents a lower difference in grain size and a higher relative density than Cu2P2O7 and LiFeP2O7.
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The extreme magnetoresistance (XMR) of some compounds, challenging our understanding of magnetoresistance, is an interesting topic in condensed-matter and materials physics and future device applications. Here, we reported magnetotransport and magnetic properties of the as-grown and post-annealed TaCo2Te2 single crystals. The resistivity evolution with temperature in the two TaCo2Te2 single crystals shows a metallic behavior. Below 50 K, the XMR effect for the two crystals is found, and MR values at 3 K under 9 T are about 3.72 × 103% for the as-grown TaCo2Te2 and 5.71 × 102% for the annealed samples, larger than that of the previous report. The studies on the Hall effect of the two TaCo2Te2 single crystals indicate the multiband feature with high carrier mobilities from a two-band model. Electron and hole concentrations and mobilities of as-grown samples are comparable, while for the annealed sample, the hole concentration and mobility are larger than the electron concentration and mobility. The carrier mobilities for the two TaCo2Te2 single crystals have the same order of magnitude, â¼103 cm2 V-1 s-1. The XMR effect may be from high carrier mobilities. Magnetization of the as-grown TaCo2Te2 decreases with increasing temperature, and a weaker magnetic transition at â¼150 K is observed. The annealed TaCo2Te2 shows no magnetic transition and just a paramagnetic behavior with rising temperature. These results indicate that defects/deficiencies may play an important role in magnetotransport and magnetic properties of the two TaCo2Te2 single crystals. These results are helpful in deeply understanding the XMR mechanism and magnetic properties in TaCo2Te2 and offer a way to study the magnetic properties of the XMR Co-Te system.
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Motivated by our study of infiltrating dynamics of immune cells into tumors, we propose a stochastic model in terms of Ito stochastic differential equations to study how two parameters, the chemoattractant production rate and the chemotactic coefficient, influence immune cell migration and how these parameters distinguish two types of gliomas. We conduct a detailed analysis of the stochastic model and its deterministic counterpart. The deterministic model can differentiate two types of gliomas according to the range of the chemoattractant production rate as two equilibrium solutions, while the stochastic model also can differentiate two types of gliomas according to the ranges of the chemoattractant production rate and chemotactic coefficient with thresholds as one non-zero ergodic invariant measure and one weak persistent state when the noise intensities are small. When the noise intensities are large comparing with the chemotactic coefficient, there is only one type of glioma that corresponds to a non-zero ergodic invariant measure. Using our experimental data, numerical simulations are carried out to demonstrate properties of our models, and we give medical interpretations and implications for our analytical results and numerical simulations. This study also confirms some of our results about IDH gliomas.
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Glioma , Humanos , Processos EstocásticosRESUMO
The coupling strain in nanoscale systems can achieve control of the physical properties in functional materials, such as ferromagnets, ferroelectrics, and superconductors. Here, we directly demonstrate the atomic-scale structure of super-tetragonal PbTiO3 nanocomposite epitaxial thin films, including the extraordinary coupling of strain transition and the existence of the oxygen vacancies. Large strain gradients, both longitudinal and transverse (â¼3 × 107 m-1), have been observed. The original non-magnetic ferroelectric composites notably evoke ferromagnetic properties, derived from the combination of Ti3+ and oxygen vacancies. The saturation ferromagnetic moment can be controlled by the strain of both the interphase and substrate, optimized to a high value of â¼55 emu/cc in 10-nm thick nanocomposite epitaxial thin films on the LaAlO3 substrate. Strain engineering provides a route to explore multiferroic systems in conventional non-magnetic ferroelectric oxides and to create functional data storage devices from both ferroelectrics and ferromagnetics.
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BACKGROUND: Rumen bacteria play a critical role in feed degradation and productivity. This study evaluated the impact of feeding regimen on the rumen microbial populations and fatty acid composition of the meat of sheep. Twenty-four Sunit sheep were raised on a grass pasture from birth to 9 months of age, at which time they were randomly divided into two feeding groups: pasture feeding (PF) and barn feeding (BF). Sheep in the PF group were allowed to graze freely on wild grassland for 3 months. Sheep in the BF group were confined for 3 months to a dry barn, in which they roamed freely with corn straw and corn. RESULTS: Sheep in the PF group had greater rumen bacteria diversity. The relative abundances of the genera Butyrivibrio_2, Saccharofermentans and Succiniclasticum were increased, and that of the genus RC9_gut_group was decreased, in the PF compared to the BF sheep. The n-3 polyunsaturated fatty acid contents were greater in meat from PF sheep than from BF sheep. In addition, the α-linolenic acid (C18:3 n-3, ALA) and conjugated linoleic acid (CLA) contents were positively correlated with the abundance of Butyrivibrio_2. CONCLUSION: Grazing may improve the diversity of rumen bacteria and increase the proportion of ALA and CLA in sheep meat. © 2020 Society of Chemical Industry.
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Bactérias/isolamento & purificação , Ácidos Graxos/química , Microbioma Gastrointestinal , Carne/análise , Rúmen/microbiologia , Ovinos/metabolismo , Ração Animal/análise , Animais , Bactérias/classificação , Bactérias/genética , Bactérias/metabolismo , China , Ácidos Graxos/metabolismo , Feminino , Masculino , Rúmen/metabolismo , Ovinos/microbiologiaRESUMO
The composition, crystallinity, morphology, and trap-state density of halide perovskite thin films critically depend on the nature of the precursor solution. A fundamental understanding of the liquid-to-solid transformation mechanism is thus essential to the fabrication of high-quality thin films of halide perovskite crystals for applications such as high-performance photovoltaics and is the topic of this Review. The roles of additives on the evolution of coordination complex species in the precursor solutions and the resulting effect on perovskite crystallization are presented. The influence of colloid characteristics, DMF/DMSO-free solutions and the degradation of precursor solutions on the formation of perovskite crystals are also discussed. Finally, the general formation mechanism of perovskite thin films from precursor solutions is summarized and some questions for further research are provided.