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This work reports the growth of crystalline SrHfxTi1−xO3 (SHTO) films on Ge (001) substrates by atomic layer deposition. Samples were prepared with different Hf content x to explore if strain, from tensile (x = 0) to compressive (x = 1), affected film crystallization temperature and how composition affected properties. Amorphous films grew at 225 °C and crystallized into epitaxial layers at annealing temperatures that varied monotonically with composition from ~530 °C (x = 0) to ~660 °C (x = 1). Transmission electron microscopy revealed abrupt interfaces. Electrical measurements revealed 0.1 A/cm2 leakage current at 1 MV/cm for x = 0.55.
Epitaxial heterostructures composed of complex oxides have fascinated researchers for over a decade as they offer multiple degrees of freedom to unveil emergent many-body phenomena often unattainable in bulk. Recently, apart from stabilizing such artificial structures along the conventional [001]-direction, tuning the growth direction along unconventional crystallographic axes has been highlighted as a promising route to realize novel quantum many-body phases. Here we illustrate this rapidly developing field of geometrical lattice engineering with the emphasis on a few prototypical examples of the recent experimental efforts to design complex oxide heterostructures along the (111) orientation for quantum phase discovery and potential applications.
Solid oxide fuel cells (SOFCs) efficiently generate electricity, but high operating temperatures (Top > 800 °C) limit their utility. Reducing Top requires mixed ion–electron conducting (MIEC) cathode materials. Density functional theory is used here to investigate the role of potassium substitutions in the MIEC material Sr1−xKxFeO3 (SKFO). We predict that such substitutions are endothermic. SrFeO3 and SKFO have nearly identical metallic electronic structures. Oxygen vacancy formation energies decrease by ~0.2 eV when xK increases from 0 to 0.0625. SKFO is a promising SOFC MIEC cathode material; however, further experimental investigations must assess its long-term stability at the desired operating temperatures.
Multifunctional, complex oxides capable of exhibiting highly-coupled electrical, mechanical, thermal, and magnetic susceptibilities have been pursued to address a range of salient technological challenges. Today, efforts are focused on addressing the pressing needs of a range of applications and identifying, understanding, and controlling materials with the potential for enhanced or novel responses. In this prospective, we highlight important developments in theoretical and computational techniques, materials synthesis, and characterization techniques. We explore how these new approaches could revolutionize our ability to discover, probe, and engineer these materials and provide a context for new arenas where these materials might make an impact.
Mesocrystal—a new class of crystals compared with conventional single crystals and randomly distributed nanocrystal systems—has captured significant attention in recent decades. Current studies have been focused on the advanced synthesis as well as the intriguing properties of mesocrystal. In order to create new opportunities upon functional mesocrystals, they can be regarded as a new functional entirety when integrated with unique matrix environments. The elegant combination of mesocrystals and matrices has enabled researchers to realize enthralling tunabilities and to derive new functionalities that cannot be found in individual components. Therefore, mesocrystal-embedded system forms a new playground towards multifunctionalities. This review article delivers a general roadmap that portrays the enhancement of intrinsic properties and new functionalities driven by novel mesocrystal-embedded oxide systems. An in-depth understanding and breakthroughs achieved in mesocrystal-embedded oxide systems are highlighted. This article concludes with a brief discussion on potential directions and perspectives along this research field.
We use first-principles calculations based on density functional theory to investigate the interplay between oxygen vacancies, A-site cation size/tolerance factor, epitaxial strain, ferroelectricity, and magnetism in the perovskite manganite series, AMnO3 (A = Ca2+, Sr2+, Ba2+). We find that, as expected, increasing the volume through either chemical pressure or tensile strain generally lowers the formation energy of neutral oxygen vacancies consistent with their established tendency to expand the lattice. Increased volume also favors polar distortions, both because competing rotations of the oxygen octahedra are suppressed and because Coulomb repulsion associated with cation off-centering is reduced. Interestingly, the presence of ferroelectric polarization favors ferromagnetic (FM) over antiferromagnetic (AFM) ordering due to suppressed AFM superexchange as the polar distortion bends the Mn–O–Mn bond angles away from the optimal 180°. Intriguingly, we find that polar distortions compete with the formation of oxygen vacancies, which have a higher formation energy in the polar phases; conversely the presence of oxygen vacancies suppresses the onset of polarization. In contrast, oxygen vacancy formation energies are lower for FM than AFM orderings of the same structure type. Our findings suggest a rich and complex phase diagram, in which defect chemistry, polarization, structure, and magnetism can be modified using chemical potential, stress or pressure, and electric or magnetic fields.
Nanomaterials have been intensively studied over the past decades with many advantages over traditional bulk materials in many applications. Nanomaterials' properties are largely governed by their chemical compositions, sizes, shapes, dimensions, morphologies and structures, which are primarily controlled with the chemical and/or physical fabrication methods and processes. This prospective will highlight recent progress on the modifications of oxide nanomaterials' properties by hydrogenation, namely heat treatment under hydrogen or hydrogen plasma environment, for various applications.
Engineering of a novel heterostructured oxide interface was used to enhance the oxygen surface exchange kinetics of La0.6Sr0.4Co0.2Fe0.8O3−δ (LSCF113) thin films. A single-layer decoration of mixed (LaSr)2CoO4±δ (LSC214) and La1−xSrxCoO3−δ (LSC113) and a double-layer decoration of stacked LSC214 and LSC113 grown on the LSCF113 markedly enhanced the surface exchange coefficients of the LSCF113 by up to ~1.5 orders of magnitude relative to the undecorated LSCF113. It is hypothesized that two different types of surface decorations can enable Sr segregation at the interface and surfaces of LSC113 and LSC214, leading to enhancement of the oxygen surface exchange kinetics of decorated LSCF113.
Direct electrical measurement of single grain boundaries is performed for ZnO-based multilayer ceramic varistors with fine grains of 2 µm, using a nano-prober. The effect of ZnO grains on non-linearity is shown to be significant. The microstructure is comprised at least two non-linear types as good- and bad-junctions. The numerical ratio of good to bad is estimated to be about one (non-linearity exponent αmax ≥ 10) to two (<10), which is independent of microstructural development as grain growth. The grain control of twinning as well as crystal orientation and donor concentration is considered effective in the further improvement.
Photocatalytic reduction of carbon dioxide (CO2) into renewable hydrocarbon fuels using solar energy has gained much attention in the effort to conserve energy and enhance carbon cycling. This paper begins with a brief description of the basic concepts of the photocatalytic reduction of CO2, introduces some experimental challenges in the gas photoreaction system and provides a review of perovskite oxide semiconductor catalysts, including tantalates, niobates, titanates, zirconates and cerates, for use in the gas phase photoreduction of CO2. The prospects for the future research of CO2 photoreduction are also presented.
Tin oxide (SnO2) hollow spheres modified with titanium dioxide (TiO2) nanowires (NWs) synthesized by sequential hydrothermal reactions were investigated as photoanodes for dye-sensitized solar cells. Not only does the hydrothermal treatment form numerous short TiO2 NWs on the surface of SnO2 spheres, but also passivates the surface of SnO2. Consequently, the specific surface area of the photoanode and dye loading are almost doubled, at the same time the surface defects and charge recombination are both appreciably reduced. As a result, the short-circuit photocurrent density and open-circuit photovoltage both greatly increased. The power conversion efficiency of the solar cells increases from 0.4% to 2.9%.
Heterostructures consisting of two ferromagnetic oxides La0.7Ca0.3MnO3 (LCMO) and SrRuO3 (SRO) were epitaxially grown by pulsed laser deposition onto a silicon (Si) substrate buffered by SrTiO3 (STO)/MgO/TiN. The x-ray scans and electron-diffraction patterns reveal the epitaxial nature of all five layers. From transmission electron microscopy, the thicknesses of the LCMO and SRO layers were estimated to be ~100 and ~200 nm, respectively. The magnetic properties of individual SRO and LCMO layers are in good agreement with the previous studies reported for those individual layers deposited on lattice-matched substrates, such as STO. The LCMO/SRO heterostructures showed enhanced switching field (from 6008 to 7600 Oe), which may originate from the bulk part of the heterostructure. The ability to grow these multifunctional structures on Si provides a route for wafer scale integration with Si, in contrast to oxide substrates that are not suitable for CMOS integration for microelectronics and spintronics applications.
Nickel–molybdenum (Ni–Mo) materials are widely used functional oxide catalysts for the hydrogen evolution reaction. In this work, we investigate the high activity of Ni–Mo by depositing size-controlled Ni nanocrystals (NCs) onto Mo substrates. We observe a synergistic increase in catalytic activity that does not scale with the Ni–Mo interface length. This evidence points to a bulk electronic interaction of the two metals that is separate from the mechanism of enhancement seen in conventionally co-deposited Ni–Mo electrocatalysts. In addition to elucidating the catalytic behavior of the Ni–Mo system, this work offers a general NC-based paradigm for investigating fundamental interactions and synergistic effects in electrocatalytic materials.