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CoxFe3-xO4(CFO)/Pt bilayers prepared by molecular beam epitaxy were investigated for the anomalous Hall effect and X-ray magnetic circular dichroism (XMCD). We found that the anomalous Hall effect originates from a magnetic proximity effect at the CFO/Pt interface. The XMCD signal in the Pt L-edge was obtained only for the sample deposited at 600 °C, indicating that the magnetic proximity effect is sensitive to the interface structure. Transmission electron microscopy images of the CFO/Pt interface and XMCD measurements of Co and Fe L-edges do not provide direct evidence for interfacial atomic diffusion or alloying. In summary, these results suggest that the magnetic proximity effect is robust for transport properties, such as the anomalous Hall effect, while the induced magnetic moment depends on slight differences in the interfacial structure, such as the presence or absence of interfacial oxygen ions.
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We report the pyrolysis of copper-containing metal-organic frameworks under high pressure and the effect of the applied pressure on the morphology and electrocatalytic performance toward the oxygen-related reactions of the products. The high-pressure and high-temperature (HPHT) syntheses were performed under 5, 2.5, 1, and 0.5 GPa, and the Cu@C products were obtained except for the 2.5 GPa experiment. Copper formed a shell-like nanostructure on the carbon matrices during the 0.5 GPa experiment, whereas copper formed sub-nanometer sized particles in the carbon matrices with the increasing pressure. It is considered that the transportation of copper atoms by outgassing during the pyrolysis affects the morphology. Electrochemical measurements revealed that all samples exhibited activity for the oxygen reduction reaction (ORR). The 0.5 GPa-treated product also exhibited the oxygen evolution reaction (OER). The overall ORR/OER performance of this product was excellent among Cu-based bifunctional materials even though it did not contain cocatalysts such as nitrogen-doped carbon or other metal elements. The Cu(iii) species in the nano-thick copper shell structure provided the active sites for the OER.
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Poly(ether ether ketone) (PEEK) is an important engineering plastic and evaluation of its local crystallinity in composites is critical for producing strong and reliable mechanical parts. Low wavenumber Raman spectroscopy and X-ray diffraction are promising techniques for the analysis of crystal ordering but a detailed understanding of the spectra has not been established. Here, we use molecular dynamics combined with a newly developed approximation to simulate local vibrational features to understand the effect of intermolecular ordering in the Raman spectra. We found that intermolecular ordering does affect the low wavenumber Raman spectra and the X-ray diffraction as observed in the experiment. Raman spectroscopy of intermolecular vibration modes is a promising technique to evaluate the local crystallinity of PEEK and other engineering plastics, and the present technique offers an estimation without requiring heavy computational resources.
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MoO2 nanowires (NWs), MoO2/MoS2 core-shell NWs, and MoS2 nanotubes (NTs) were synthesized by the turbulent flow chemical vapor deposition of MoO2 using MoO3, followed by sulfurization in the sulfur gas flow. The involvement of MoO x suboxide is suggested by density functional theory (DFT) calculations of the surface energies of MoO2. The thickness of the MoS2 layers can be controlled by precise tuning of sulfur vapor flow and temperatures. MoS2 had an armchair-type winding topology due to the epitaxial relation with the MoO2 NW surface. A single â¼ few-layer MoO2/MoS2 core-shell structure showed photoluminescence after the treatment with a superacid. The resistivities of an individual MoO2 NW and a MoS2 NT were measured, and they showed metallic and semiconducting resistivity-temperature relationships, respectively.
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We report the crystal growth of pentacene from a solution of naphthalene. The solubility of pentacene in naphthalene was evaluated by optical absorption at elevated temperature. The crystal growth was performed in an H-shaped sealed glass tube or metal vessels sealed with ultrahigh-vacuum compatible flanges placed in heated two-zone aluminum blocks. The obtained crystals had a single-crystal-like appearance and flat surface. They were made of aligned microtwins of the "bulk type" (interlayer spacing 14.5 Å) polymorph.
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We found that oxidized Cu nanoparticles can catalyze the growth of boron nitride nanotubes from borazine via plasma-assisted chemical vapor deposition. The Raman spectra suggest that the formation of thin-walled nanotubes show a radial breathing mode vibration. The presence of oxygen in the plasma environment was necessary for the growth of the nanotubes, and a part of the nanotubes had a core shell structure with a cupper species inside it. In atomic resolution transmission electron microscope (TEM) images, Cu2O was found at the interface between the Cu-core and turbostratic BN-shell. The growth mechanism seemed different from that of carbon nanotube core-shell structures. Therefore, we pointed out the important role of the dynamic morphological change in the Cu2O-Cu system.
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A metal-organic framework (MOF) consisting of Cu-benzenetricarboxylic acid was processed under ultrahigh pressure (5 GPa) and at temperature of up to 500 °C. The products were characterized with TEM, FTIR, and XAFS. The decomposition of the MOF started at 200 °C at 5 GPa. This temperature was much lower than that in the vacuum. Single-nanometer Cu nanoparticles were obtained in carbon matrix, which was significantly smaller than the Cu particles prepared at ambient pressure. The catalytic activity for Huisgen cycloaddition was examined, and the sample processed at 5 GPa showed a much improved performance compared with that of the MOF-derived Cu nanoparticles prepared without high pressure.
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Two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanoplates (CNNP) have become a hot research topic in photocatalysis due to their small thickness and large specific surface area that favors charge transport and catalytic surface reactions. However, the wide application of 2D g-C3N4 nanoplates prepared by ordinary methods suffers from increased band gaps with a poor solar harvesting capability caused by the strong quantum confinement effect and reduced conjugation distance. In this paper, a facile approach of exfoliation and the following fast thermal treatment of the bulk g-C3N4 is proposed to obtain a porous few-layered g-C3N4 with nitrogen defects. Due to the preferable crystal, textural, optical and electronic structures, the as-obtained porous CNNP demonstrated a significantly improved photocatalytic activity towards water splitting than the bulk g-C3N4 and even the 3 nm-thick CNNP obtained by sugar-assisted exfoliation of the bulk g-C3N4. The difference in the enhancement factors between the H2O splitting and organic decomposition has revealed the effect of N defects. This study offers insightful outlooks on the scalable fabrication of a porous few-layered structure with a promoted photocatalytic performance.
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One of the most important achievements in the field of spintronics is the development of magnetic tunnel junctions (MTJs). MTJs exhibit a large tunneling magnetoresistance (TMR). However, TMR is strongly dependent on biasing voltage, generally, decreasing with applying bias. The rapid decay of TMR was a major deficiency of MTJs. Here we report a new phenomenon at room temperature, in which the tunneling magnetocapacitance (TMC) increases with biasing voltage in an MTJ system based on Co40Fe40B20/MgO/Co40Fe40B20. We have observed a maximum TMC value of 102% under appropriate biasing, which is the largest voltage-induced TMC effect ever reported for MTJs. We have found excellent agreement between theory and experiment for the bipolar biasing regions using Debye-Fröhlich model combined with quartic barrier approximation and spin-dependent drift-diffusion model. Based on our calculation, we predict that the voltage-induced TMC ratio could reach 1100% in MTJs with a corresponding TMR value of 604%. Our work has provided a new understanding on the voltage-induced AC spin-dependent transport in MTJs. The results reported here may open a novel pathway for spintronics applications, e.g., non-volatile memories and spin logic circuits.
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The application of magnetic oxides in spintronics has recently attracted much attention. The epitaxial growth of magnetic oxide on Si could be the first step of new functional spintronics devices with semiconductors. However, epitaxial spinel ferrite films are generally grown on oxide substrates, not on semiconductors. To combine oxide spintronics and semiconductor technology, we fabricated Fe3O4 films through epitaxial growth on a Si(111) substrate by inserting a γ-Al2O3 buffer layer. Both of γ-Al2O3 and Fe3O4 layer grew epitaxially on Si and the films exhibited the magnetic and electronic properties as same as bulk. Furthermore, we also found the buffer layer dependence of crystal structure of Fe3O4 by X-ray diffraction and high-resolution transmission electron microscope. The Fe3O4 films on an amorphous-Al2O3 buffer layer grown at room temperature grew uniaxially in the (111) orientation and had a textured structure in the plane. When Fe3O4 was deposited on Si(111) directly, the poly-crystal Fe3O4 films were obtained due to SiOx on Si substrate. The epitaxial Fe3O4 layer on Si substrates enable us the integration of highly functional spintoronic devices with Si technology.
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Magnetocapacitance (MC) effect, observed in a wide range of materials and devices, such as multiferroic materials and spintronic devices, has received considerable attention due to its interesting physical properties and practical applications. A normal MC effect exhibits a higher capacitance when spins in the electrodes are parallel to each other and a lower capacitance when spins are antiparallel. Here we report an inverse tunnel magnetocapacitance (TMC) effect for the first time in Fe/AlOx/Fe3O4 magnetic tunnel junctions (MTJs). The inverse TMC reaches up to 11.4% at room temperature and the robustness of spin polarization is revealed in the bias dependence of the inverse TMC. Excellent agreement between theory and experiment is achieved for the entire applied frequency range and the wide bipolar bias regions using Debye-Fröhlich model (combined with the Zhang formula and parabolic barrier approximation) and spin-dependent drift-diffusion model. Furthermore, our theoretical calculations predict that the inverse TMC effect could potentially reach 150% in MTJs with a positive and negative spin polarization of 65% and -42%, respectively. These theoretical and experimental findings provide a new insight into both static and dynamic spin-dependent transports. They will open up broader opportunities for device applications, such as magnetic logic circuits and multi-valued memory devices.
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The water vapor transmission rate (WVTR) of a gas barrier coating is a critically important parameter for flexible organic device packaging, but its accurate measurement without mechanical stress to ultrathin films has been a significant challenge in instrumental analysis. At the current stage, no reliable results have been reported in the range of 10-6 g m-2 day-1 that is required for organic light emitting diodes (OLEDs). In this article, we describe a solution for this difficult, but important measurement, involving enhanced sensitivity by a cold trap, stabilized temperature system, pumped sealing and calibration by a standard conductance element.
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We report detailed experiments on chemical vapor deposition of an atomic' layer semiconductor MoS2. We developed a new type of CVD system in which MoO3 and S sources are separately supplied to the substrates. It has become possible to precisely control the supply of the materials separately in the order of seconds. Raman and XPS analysis of the films grown under various conditions revealed that the initially obtained films are S-deficient and complete stoichiometry is reached after several minutes under S vapor flow.
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The tunnel magnetoresistance (TMR) effect in magnetic tunnel junctions (MTJs) is the key to developing magnetoresistive random-access-memory (MRAM), magnetic sensors and novel programmable logic devices. Conventional MTJs with an amorphous aluminium oxide tunnel barrier, which have been extensively studied for device applications, exhibit a magnetoresistance ratio up to 70% at room temperature. This low magnetoresistance seriously limits the feasibility of spintronics devices. Here, we report a giant MR ratio up to 180% at room temperature in single-crystal Fe/MgO/Fe MTJs. The origin of this enormous TMR effect is coherent spin-polarized tunnelling, where the symmetry of electron wave functions plays an important role. Moreover, we observed that their tunnel magnetoresistance oscillates as a function of tunnel barrier thickness, indicating that coherency of wave functions is conserved across the tunnel barrier. The coherent TMR effect is a key to making spintronic devices with novel quantum-mechanical functions, and to developing gigabit-scale MRAM.
