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Dielectric capacitors are highly desired for electronic systems owing to their high-power density and ultrafast charge/discharge capability. However, the current dielectric capacitors suffer severely from the thermal instabilities, with sharp deterioration of energy storage performance at elevated temperatures. Here, guided by phase-field simulations, we conceived and fabricated the self-assembled metadielectric nanostructure with HfO2 as second-phase in BaHf0.17Ti0.83O3 relaxor ferroelectric matrix. The metadielectric structure can not only effectively increase breakdown strength, but also broaden the working temperature to 400 oC due to the enhanced relaxation behavior and substantially reduced conduction loss. The energy storage density of the metadielectric film capacitors can achieve to 85 joules per cubic centimeter with energy efficiency exceeding 81% in the temperature range from 25 °C to 400 °C. This work shows the fabrication of capacitors with potential applications in high-temperature electric power systems and provides a strategy for designing advanced electrostatic capacitors through a metadielectric strategy.
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RNA acetylation is a universal post-transcriptional modification that occurs in various RNAs. Transfer RNA (tRNA) acetylation is found at position 34 (ac4C34) in bacterial tRNAMet and position 12 (ac4C12) in eukaryotic tRNASer and tRNALeu. The biochemical mechanism, structural basis and functional significance of ac4C34 are well understood; however, despite being discovered in the 1960s and identification of Kre33/NAT10 and Tan1/THUMPD1 as modifying apparatuses, ac4C12 modification activity has never been reconstituted for nearly six decades. Here, we successfully reconstituted the ac4C12 modification activity of yeast Kre33 and Tan1. Biogenesis of ac4C12 is primarily dependent on a minimal set of elements, including a canonical acceptor stem, the presence of the 11CCG13 motif and correct D-arm orientation, indicating a molecular ruler mechanism. A single A13G mutation conferred ac4C12 modification to multiple non-substrate tRNAs. Moreover, we were able to introduce ac4C modifications into small RNAs. ac4C12 modification contributed little to tRNA melting temperature and aminoacylation in vitro and in vivo. Collectively, our results realize in vitro activity reconstitution, delineate tRNA substrate selection mechanism for ac4C12 biogenesis and develop a valuable system for preparing acetylated tRNAs as well as non-tRNA RNA species, which will advance the functional interpretation of the acetylation in RNA structures and functions.
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RNA de Transferência , Proteínas de Ligação a RNA , Proteínas de Saccharomyces cerevisiae , Acetilação , Mutação , Conformação de Ácido Nucleico , Processamento Pós-Transcricional do RNA , RNA de Transferência/metabolismo , RNA de Transferência/genética , RNA de Transferência/química , Saccharomyces cerevisiae/genética , Saccharomyces cerevisiae/metabolismo , Proteínas de Saccharomyces cerevisiae/metabolismo , Proteínas de Saccharomyces cerevisiae/genética , Proteínas de Saccharomyces cerevisiae/química , Proteínas de Ligação a RNA/metabolismoRESUMO
Due to dielectric capacitors' already-obtained fast charge-discharge speed, research has been focused on improving their Wrec. Increasing the polarization and enhancing the voltage endurance are efficient ways to reach higher Wrec, however simultaneous modification still seems a paradox. For example, in the ferroelectric-to-relaxor ferroelectric (FE-to-RFE) phase transition strategy, which has been widely used in the latest decade, electric breakdown strength (Eb) and energy storage efficiency (η) always increase, while at the same time, the maximum polarization (Pmax) inevitably decreases. The solution to this problem can be obtained from another degree of freedom, like defect engineering. By incorporating Bi(Zn2/3Ta1/3)O3 (BZT) into the Ba0.15Ca0.85Zr0.1Ti0.9O3 (BCZT) lattice to form (1 - x)Ba0.15Ca0.85Zr0.1Ti0.9O3-xBi(Zn2/3Ta1/3)O3 (BCZT-xBZT) solid-solution ceramics, in this work, ultrahigh ferroelectric polarization was achieved in BCZT-0.15BZT, which is caused by the polarization double-enhancement, comprising the contribution of interfacial and dipole polarization. In addition, due to the electron compensation, a Schottky contact formed at the interface between the electrode and the ceramic, which in the meantime, enhanced its Eb. A Wrec of 8.03 J cm-3, which is the highest among the BCZT-based ceramics reported so far, with an extremely low energy consumption, was finally achieved. BCZT-0.15BZT also has relatively good polarization fatigue after long-term use, good energy storage frequency stability and thermal stability, as well as excellent discharge properties.
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Perovskite oxide-based memristors have been extensively investigated for the application of non-volatile memories, and the oxygen vacancies associated with Schottky barrier changing are considered as the origin of the memristive behaviors. However, due to the difference of device fabrication progress, various resistive switching (RS) behaviors have been observed even in one device, deteriorating the stability and reproducibility of devices. Precisely controlling the oxygen vacancies distribution and shedding light on the behind physic mechanism of these RS behaviors, are highly desired to help improve the performance and stability of such Schottky junction-based memristors. In this work, the epitaxial LaNiO3(LNO)/Nb:SrTiO3(NSTO) is adopted to explore the influence of oxygen vacancy profiles on these abundant RS phenomena. It demonstrates that the migration of oxygen vacancy in LNO films plays a key role in memristive behaviors. When the effect of oxygen vacancies at the LNO/NSTO interface is negligible, improving the oxygen vacancies concentration in LNO film could facilitate resistance on/off ratio of HRS and LRS, and the corresponding conducting mechanisms attributes to the thermionic emission and tunneling-assisted thermionic emission, respectively. Moreover, it is found that reasonably increasing the oxygen vacancies at LNO/NSTO interface makes trap-assisted tunneling possible, also providing an effective way to improve the performance of the device. The results in this work have clearly elucidated the relationship between oxygen vacancy profile and RS behaviors, and give physical insights into the strategies for improving the device performance of Schottky junction-based memristors.
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Nióbio , Oxigênio , Reprodutibilidade dos TestesRESUMO
In this work, we explored the potential of the ferroelectric gate of (Pb0.92La0.08)(Zr0.30Ti0.70)O3 (PLZT(8/30/70)) for flexible graphene field effect transistor (GFET) devices. Based on the deep understanding of the VDirac of PLZT(8/30/70) gate GFET, which determines the application of the flexible GFET devices, the polarization mechanisms of PLZT(8/30/70) under bending deformation were analyzed. It was found that both flexoelectric polarization and piezoelectric polarization exist under bending deformation, and their polarization direction is opposite under the same bending deformation. Thus, a relatively stable of VDirac is obtained due to the combination of these two effects. In contrast to the relatively good linear movement of VDirac under bending deformation of relaxor ferroelectric (Pb0.92La0.08)(Zr0.52Ti0.48)O3 (PLZT(8/52/48)) gated GFET, these stable properties of the PLZT(8/30/70) gate GFETs make them have great potential for applications in flexible devices.
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The leakage behavior of ferroelectric film has an important effect on energy storage characteristics. Understanding and controlling the leakage mechanism of ferroelectric film at different temperatures can effectively improve its wide-temperature storage performance. Here, the structures of a 1 mol% SiO2-doped BaZr0.35Ti0.65O3 (BZTS) layer sandwiched between two undoped BaZr0.35Ti0.65O3 (BZT35) layers was demonstrated, and the leakage mechanism was analyzed compared with BZT35 and BZTS single-layer film. It was found that interface-limited conduction of Schottky (S) emission and the Fowler-Nordheim (F-N) tunneling existing in BZT35 and BZTS films under high temperature and a high electric field are the main source of the increase of leakage current and the decrease of energy storage efficiency at high temperature. Only an ohmic conductive mechanism exists in the whole temperature range of BZT35/BZTS/BZT35(1:1:1) sandwich structure films, indicating that sandwich multilayer films can effectively simulate the occurrence of interface-limited conductive mechanisms and mention the energy storage characteristics under high temperature.
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Magnetoresistance based information devices have attracted much attention due to the ability to utilize spins as information carriers. To promote the magnetoresistance-based devices, ultrahigh magnetoresistance ratios are highly desirable for magnetic sensing, memory, and artificial intelligent devices, etc. However, today the magnetoresistance devices are facing the challenge of limited magnetoresistance ratio, low work temperature, or high magnetic field, which calls for proper theories and mechanisms. To address it, we first introduce the flexible bending-controlled magnetoresistance device based on the La0.67Ba0.33MnO3 film. Due to the anisotropic resistance of the La0.67Ba0.33MnO3 film and the nonlinear amplification effect of the Zener diode, the device has exhibited strong magnetoresistive performance (â¼8725% at 1 T, 300 K). Combining the assist from mechanical bending and diode, high magnetic field sensitivity with large magnetoresistance ratio (â¼1.7 × 104% at 1 T, 300 K) and low work current (â¼0.15 mA) is simultaneously achieved at room temperature, which is over 104 times larger than that of the planar La0.67Ba0.33MnO3 film. Based on the above results, we propose one but not the only possible application as tunable multistage switch. Our findings may pave a strategy to develop flexible diode-enhanced magnetoresistance device with ultrahigh magnetoresistance ratios and bending tunable performances.
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With the development of miniaturization, lightweight and integration of electronic devices, the demand for high-temperature dielectric capacitors is becoming urgent. Nevertheless, the breakdown strength and polarization are deteriorated at high temperatures due to the thermal energy assisting the electron transport and impeding the dipole alignment. Here, a structure of capacitor with double gradients of dielectric constant gradient and strain gradient is designed to achieve high breakdown strength, high working temperature, and high energy storage density simultaneously. It is found that the designed structure of BaHf0.17 Ti0.83 O3 /1mol% SiO2 doped BaZr0.35 Ti0.65 O3 /0.85BaTiO3 -0.15Bi(Mg0.5 Zr0.5 )O3 exhibits excellent energy storage performance. The energy storage density of 127.3 J cm-3 with an energy storage efficiency of 79.6% is realized in the up-sequence multilayer with period N = 2 at room temperature. Moreover, when the working temperature varies from -100 to 200 °C, the energy storage density of the N = 4 capacitor keeps stably at 84.62 J cm-3 with an energy storage efficiency 78.42% at 6.86 MV cm-1 . All these properties promise great potential applications of the designed multilayer capacitors with the double gradients in harsh environments, and the design principle can be applicable to other systems to boost working temperature.
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Although complex Lü systems have been considered in many studies, application of the self-time-delay synchronization (STDS) of complex Lü systems in secure speech communications does not appear to have been covered in much of the literature. Therefore, it is meaningful to study the STDS of complex Lü systems and its application in secure speech communication. First, a complex Lü system with double time-delay is introduced and its chaotic characteristics are analyzed. Second, a synchronization controller is designed to achieve STDS. Third, the improved STDS controller is used to design a speech communication scheme based on a complex Lü system. Finally, the effectiveness of the controller and communication scheme are verified by simulation.
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Industry has been seeking a thin-film capacitor that can work at high temperature in a harsh environment, where cooling systems are not desired. Up to now, the working temperature of the thin-film capacitor is still limited up to 200 °C. Herein, we design a multilayer structure with layers of paraferroelectric (Ba0.3Sr0.7TiO3, BST) and relaxor ferroelectric (0.85BaTiO3-0.15Bi(Mg0.5Zr0.5)O3, BT-BMZ) to realize optimum properties with a flat platform of dielectric constant and high breakdown strength for excellent energy storage performance at high temperature. Through optimizing the multilayer structure, a highly stable relaxor ferroelectric state is obtained for the BST/BT-BMZ multilayer thin-film capacitor with a total thickness of 230 nm, a period number N = 8, and a layer thickness ratio of BST/BT-BMZ = 3/7. The optimized multilayer film shows significantly improved energy storage density (up to 30.64 J/cm3) and energy storage efficiency (over 70.93%) in an ultrawide temperature range from room temperature to 250 °C. Moreover, the multilayer system also exhibits excellent thermal stability in such an ultrawide temperature range with a change of 5.15 and 12.75% for the recoverable energy density and energy storage efficiency, respectively. Our results demonstrate that the designed thin-film capacitor is promising for the application in a harsh environment and open a way to tailor a thin-film capacitor toward higher working temperature with enhanced energy storage performance.
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Chitooligosaccharide (COS) has been recognized to exhibit efficient anti-oxidant activity. Enzymatic hydrolysis using chitosanases can retain all the amino and hydroxyl groups of chitosan, which are necessary for its activity. In this study, a new chitosanase encoding gene, csnQ, was cloned from the marine Bacillus sp. Q1098 and expressed in Escherichia coli. The recombinant chitosanase, CsnQ, showed maximal activity at pH 5.31 and 60 °C. Determination of CsnQ pH-stability showed that CsnQ could retain more than 50% of its activity over a wide pH, from 3.60 to 9.80. CsnQ is an endo-type chitosanase, yielding chitodisaccharide as the main product. Additionally, in vitro and in vivo analyses indicated that chitodisaccharide possesses much more effective anti-oxidant activity than glucosamine and low molecular weight chitosan (LMW-CS) (~5 kDa). Notably, to our knowledge, this is the first evidence that chitodisaccharide is the minimal COS fragment required for free radical scavenging.
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Antioxidantes/farmacologia , Bacillus/enzimologia , Proteínas de Bactérias/metabolismo , Glicosídeo Hidrolases/metabolismo , Sequência de Aminoácidos , Antioxidantes/química , Proteínas de Bactérias/química , Proteínas de Bactérias/genética , Regulação Bacteriana da Expressão Gênica , Regulação Enzimológica da Expressão Gênica , Glicosídeo Hidrolases/química , Glicosídeo Hidrolases/genética , Hidrólise , FilogeniaRESUMO
High-quality flexible magnetic oxide thin films have promoted a wide range of potential applications in spintronic devices due to their unique physical properties. To obtain the optimized microwave magnetism for future all-oxide-based spintronic applications, high-quality oxide materials with excellent epitaxial quality as well as specific bending properties related to ferromagnetic resonance are high in demand. Here, (001)-oriented La0.67Sr0.33MnO3 epitaxial thin films with different thicknesses have been grown and subsequently transferred onto flexible poly(dimethylsiloxane) substrates. The microwave magnetisms of these film samples have been investigated under various bending states. Under bending, the ferromagnetic resonance lineshape of the film gradually transits from a single mode to a superposition of multimodes, possibly because of the uneven distribution of magnetization in the bending film at X-band. This phenomenon is more apparent when the direction of the applied magnetic field goes close to the out-of-plane of the film. Hence, an integration of invariable and continuous tuning of ferromagnetic resonance field under various mechanical bending can be achieved in one same sample by just tuning the direction of the applied magnetic field, which reveals that the flexible La0.67Sr0.33MnO3 thin films have huge potential in the applications in future flexible multifunctional devices.
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As passive components in flexible electronics, the dielectric capacitors for energy storage are facing the challenges of flexibility and capability for integration and miniaturization. In this work, the all-inorganic flexible dielectric film capacitors have been obtained. The flexible capacitors show a desirable recoverable energy density ( Wrec) of 40.6 J/cm3 and a good energy efficiency (η) of 68.9%. Moreover, they have no obvious deterioration on both the Wrec and η after 104 times of mechanical bending cycles or under the bending state with a curvature radius of 4 mm. Besides, the outstanding stability of the capacitors against cycle fatigue over fast 106 charge-discharge cycles is demonstrated. Most importantly, they work properly at a wide temperature range from -120 to 150 °C with Wrec > 15 J/cm3 and η > 70%. These fascinating performances endow the flexible capacitors with huge potential application in the future "microenergy storage" system in flexible electronics.
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With the development of flexible electronics, the mechanical flexibility of functional materials is becoming one of the most important factors that needs to be considered in materials selection. Recently, flexible epitaxial nanoscale magnetic materials have attracted increasing attention for flexible spintronics. However, the knowledge of the bending coupled dynamic magnetic properties is poor when integrating the materials in flexible devices, which calls for further quantitative analysis. Herein, a series of epitaxial LiFe5O8 (LFO) nanostructures are produced as research models, whose dynamic magnetic properties are characterized by ferromagnetic resonance (FMR) measurements. LFO films with different crystalline orientations are discussed to determine the influence from magnetocrystalline anisotropy. Moreover, LFO nanopillar arrays are grown on flexible substrates to reveal the contribution from the nanoscale morphology. It reveals that the bending tunability of the FMR spectra highly depends on the demagnetization field energy of the sample, which is decided by the magnetism and the shape factor in the nanostructure. Following this result, LFO film with high bending tunability of microwave magnetic properties, and LFO nanopillar arrays with stable properties under bending are obtained. This work shows guiding significances for the design of future flexible tunable/stable microwave magnetic devices.
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Recent development in magnetic nanostructures has promoted flexible electronics into the application of integrated devices. However, the magnetic properties of flexible devices strongly depend on the bending states. In order to realize the design of new flexible devices driven by an external field, the first step is to make the magnetic properties insensitive to the bending. Herein, a series of LiFe5O8 nanopillar arrays were fabricated, whose microwave magnetic properties can be modulated by tuning the nanostructure. This work demonstrates that nanostructure engineering is useful to control the bending sensitivity of microwave magnetism and further design stable flexible devices.
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Electrochemical effects manifest as nonlinear responses to an applied electric field in electrochemical devices, and are linked intimately to the molecular orientation of ions in the electric double layer (EDL). Herein, we probe the origin of the electrochemical effect using a double-gate graphene field effect transistor (GFET) of ionic liquid N,N-diethyl-N-(2-methoxyethyl)-N-methylammonium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) top-gate, paired with a ferroelectric Pb0.92La0.08Zr0.52Ti0.48O3 (PLZT) back-gate of compatible gating efficiency. The orientation of the interfacial molecular ions can be extracted by measuring the GFET Dirac point shift, and their dynamic response to ultraviolet-visible light and a gate electric field was quantified. We have observed that the strong electrochemical effect is due to the TFSI anions self-organizing on a treated GFET surface. Moreover, a reversible order-disorder transition of TFSI anions self-organized on the GFET surface can be triggered by illuminating the interface with ultraviolet-visible light, revealing that it is a useful method to control the surface ion configuration and the overall performance of the device.
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Mechanical flexibility of electronic devices has attracted much attention from research due to the great demand in practical applications and rich commercial value. Integration of functional oxide materials in flexible polymer materials has proven an effective way to achieve flexibility of functional electronic devices. However, the chemical and mechanical incompatibilities at the interfaces of dissimilar materials make it still a big challenge to synthesize high-quality single-crystalline oxide thin film directly on flexible polymer substrates. This study reports an improved method that is employed to successfully transfer a centimeter-scaled single-crystalline LiFe5 O8 thin film on polyimide substrate. Structural characterizations show that the transferred films have essentially no difference in comparison with the as-grown films with respect to the microstructure. In particular, the transferred LiFe5 O8 films exhibit excellent magnetic properties under various mechanical bending statuses and show excellent fatigue properties during the bending cycle tests. These results demonstrate that the improved transfer method provides an effective way to compose single-crystalline functional oxide thin films onto flexible substrates for applications in flexible and wearable electronics.
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Epitaxial thin films of CoFe2O4 (CFO) have successfully been transferred from a SrTiO3 substrate onto a flexible polyimide substrate. By bending the flexible polyimide, different levels of uniaxial strain are continuously introduced into the CFO epitaxial thin films. Unlike traditional epitaxial strain induced by substrates, the strain from bending will not suffer from critical thickness limitation, crystalline quality variation, and substrate clamping, and more importantly, it provides a more intrinsic and reliable way to study strain-controlled behaviors in functional oxide systems. It is found that both the saturation magnetization and coercivity of the transferred films can be changed over the bending status and show a high accord with the movement of the curvature bending radius of the polyimide substrate. This reveals that the mechanical strain plays a critical role in tuning the magnetic properties of CFO thin films parallel and perpendicular to the film plane direction.
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A large energy storage density (ESD) of 30.4 J/cm3 and high energy efficiency of 81.7% under an electrical field of 3 MV/cm was achieved at room temperature by the fabrication of environmentally friendly lead-free BaZr0.2Ti0.8O3 epitaxial thin films on Nb-doped SrTiO3 (001) substrates by using a radio-frequency magnetron sputtering system. Moreover, the BZT film capacitors exhibit great thermal stability of the ESD from 16.8 J/cm3 to 14.0 J/cm3 with efficiency of beyond 67.4% and high fatigue endurance (up to 106 cycles) in a wide temperature range from room temperature to 125 °C. Compared to other BaTiO3-based energy storage capacitor materials and even Pb-based systems, BaZr0.2Ti0.8O3 thin film capacitors show either high ESD or great energy efficiency. All of these excellent results revealed that the BaZr0.2Ti0.8O3 film capacitors have huge potential in the application of modern electronics, such as locomotive and pulse power, in harsh working environments.
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Graphene was inserted into the interface between electric dipole layers from DEME-TFSI ionic liquid (top-gate) and ferroelectric Pb0.92La0.08Zr0.52Ti0.48O3 (PLZT, back-gate) to probe the interface dipole-dipole interaction in response to DC and pulsed gate voltages. A highly complicated behavior of the interface dipole-dipole interaction has been revealed as a combination of electrostatic and electrochemical effects. The interfacial polar molecules in the DEME-TFSI electrical double layer are pinned with assistance from the PLZT back-gate in response to a DC top-gate pump, leading to strong nonlinear electrochemical behavior. In contrast, depinning of these molecules can be facilitated by a faster pulsed top-gate pump, which results in a characteristic linear electrostatic behavior. This result not only sheds light on the dynamic dipole-dipole interactions on the interface between functional materials but also prototypes a unique pump and probe approach using graphene field effect transistors to detect the interface dipole-dipole interaction.