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Abstract Multiferroic materials have generated great interest due to their potential as functional device materials. Nanocomposites have been increasingly used to design and generate new functionalities by pairing dissimilar ferroic materials, though the combination often introduces new complexity and challenges unforeseeable in single-phase counterparts. The recently developed approaches to fabricate 3D super-nanocomposites (3D‐sNC) open new avenues to control and enhance functional properties. In this work, we develop a new 3D‐sNC with CoFe₂O₄(CFO) short nanopillar arrays embedded in BaTiO₃(BTO) film matrix via microstructure engineering by alternatively depositing BTO:CFO vertically-aligned nanocomposite layers and single-phase BTO layers. This microstructure engineering method allows encapsulating the relative conducting CFO phase by the insulating BTO phase, which suppress the leakage current and enhance the polarization. Our results demonstrate that microstructure engineering in 3D‐sNC offers a new bottom–up method of fabricating advanced nanostructures with a wide range of possible configurations for applications where the functional properties need to be systematically modified. 

Abstract Mixtures of Ce‐doped rare‐earth aluminum perovskites are drawing a significant amount of attention as potential scintillating devices. However, the synthesis of complex perovskite systems leads to many challenges. Designing the A‐site cations with an equiatomic ratio allows for the stabilization of a single‐crystal phase driven by an entropic regime. This work describes the synthesis of a highly epitaxial thin film of configurationally disordered rare‐earth aluminum perovskite oxide (La_0.2Lu_0.2Y_0.2Gd_0.2Ce_0.2)AlO₃and characterizes the structural and optical properties. The thin films exhibit three equivalent epitaxial domains having an orthorhombic structure resulting from monoclinic distortion of the perovskite cubic cell. An excitation of 286.5 nm from Gd³⁺and energy transfer to Ce³⁺with 405 nm emission are observed, which represents the potential for high‐energy conversion. These experimental results also offer the pathway to tunable optical properties of high‐entropy rare‐earth epitaxial perovskite films for a range of applications. 

Abstract Interface‐type (IT) resistive switching (RS) memories are promising for next generation memory and computing technologies owing to the filament‐free switching, high on/off ratio, low power consumption, and low spatial variability. Although the switching mechanisms of memristors have been widely studied in filament‐type devices, they are largely unknown in IT memristors. In this work, using the simple Au/Nb:SrTiO₃(Nb:STO) as a model Schottky system, it is identified that protons from moisture are key element in determining the RS characteristics in IT memristors. The Au/Nb:STO devices show typical Schottky interface controlled current–voltage (I–V) curves with a large on/off ratio under ambient conditions. Surprisingly, in a controlled environment without protons/moisture, the largeI–Vhysteresis collapses with the disappearance of a high resistance state (HRS) and the Schottky barrier. Once the devices are re‐exposed to a humid environment, the typical largeI–Vhysteresis can be recovered within hours as the HRS and Schottky interface are restored. The RS mechanism in Au/Nb:STO is attributed to the Schottky barrier modulation by a proton assisted electron trapping and detrapping process. This work highlights the important role of protons/moisture in the RS properties of IT memristors and provides fundamental insight for switching mechanisms in metal oxides‐based memory devices. 

Abstract A variety of mechanisms are reported to play critical roles in contributing to the high carrier/electron mobility in oxide/SrTiO₃(STO) heterostructures. By using La_0.95Sr_0.05TiO₃(LSTO) epitaxially grown on different single crystal substrates (such as STO, GdScO₃, LaAlO₃, (LaAlO₃)_0.3(Sr₂AlTaO₆)_0.7, and CeO₂buffered STO) as the model systems, the formation of a conducting substrate surface layer (CSSL) on STO substrate is shown at relatively low growth temperature and high oxygen pressure (725 °C, 5 × 10^–4 Torr), which contributes to the enhanced conductivity of the LSTO/STO heterostructures. Different from the conventional oxygen vacancy model, this work reveals that the formation of the CSSL occurs when growing an oxide layer (LSTO in this case) on STO, while neither annealing nor the growth of an Au layer alone at the exact same growth condition generates the CSSL in STO. It demonstrates that the oxide layer actively pulls oxygen from STO substrate at given growth conditions, leading to the formation of the CSSL. The observations emphasize the oxygen transfer across film/substrate interface during the synthesis of oxide heterostructures playing a critical role in functional properties. 

Abstract To investigate the role of interlayers on the growth, microstructure, and physical properties of 3D nanocomposite frameworks, a set of novel 3D vertically aligned nanocomposite (VAN) frameworks are assembled by a relatively thin interlayer (M) sandwiched by two consecutively grown La_0.7Sr_0.3MnO₃(LSMO)‐ZnO VANs layers. ZnO nanopillars from the two VAN layers and the interlayer (M) create a heterogeneous 3D frame embedded in the LSMO matrix. The interlayer (M) includes yttria‐stabilized zirconia (YSZ), CeO₂, SrTiO₃, BaTiO₃, and MgO with in‐plane matching distances increasing from ≈3.63 to ≈4.21 Å, and expected in‐plane strains ranging from tensile (≈8.81% on YSZ interlayer) to compressive (≈–6.23% on MgO interlayer). The metal‐insulator transition temperature increases from ≈133 K (M = YSZ) to ≈252 K (M = MgO), and the low‐field magnetoresistance peak value is tuned from ≈36.7% to ≈20.8%. The 3D heterogeneous frames empower excellent tunable magnetotransport properties and promising potentials for microstructure‐enabled applications. 

Abstract Memristors with excellent scalability have the potential to revolutionize not only the field of information storage but also neuromorphic computing. Conventional metal oxides are widely used as resistive switching materials in memristors. Interface‐type memristors based on ferroelectric materials are emerging as alternatives in the development of high‐performance memory devices. A clear understanding of the switching mechanisms in this type of memristors, however, is still in its early stages. By comparing the bipolar switching in different systems, it is found that the switchable diode effect in ferroelectric memristors is controlled by polarization modulated Schottky barrier height and polarization coupled interfacial deep states trapping/detrapping. Using semiconductor theories with consideration of polarization effects, a phenomenological theory is developed to explain the current–voltage behavior at the metal/ferroelectric interface. These findings reveal the critical role of the interaction among polarization charges, interfacial defects, and Schottky interface in controlling ferroelectric resistive switching and offer the guidance to design ferroelectric memristors with enhanced performance. 

Combinatorial growth is capable of creating a compositional gradient for thin film materials and thus has been adopted to explore composition variation mostly for metallic alloy thin films and some dopant concentrations for ceramic thin films. This study uses a combinatorial pulsed laser deposition method to successfully fabricate two‐phase oxide–oxide vertically aligned nanocomposite (VAN) thin films of La_0.7Sr_0.3MnO₃(LSMO)‐NiO with variable composition across the film area. The LSMO‐NiO compositional gradient across the film alters the two‐phase morphology of the VAN through varying nanopillar size and density. Additionally, the magnetic anisotropy and magnetoresistance properties of the nanocomposite thin films increase with increasing NiO composition. This demonstration of a combinatorial method for VAN growth can increase the efficiency of nanocomposite thin film research by allowing all possible compositions of thin film materials to be explored in a single deposition. 

Metamaterials present great potential in the applications of solar cells and nanophotonics, such as super lenses and other meta devices, owing to their superior optical properties. In particular, hyperbolic metamaterials (HMMs) with exceptional optical anisotropy offer improved manipulation of light–matter interactions as well as a divergence in the density of states and thus show enhanced performances in related fields. Recently, the emerging field of oxide–metal vertically aligned nanocomposites (VANs) suggests a new approach to realize HMMs with flexible microstructural modulations. In this work, a new oxide–metal metamaterial system, CeO 2 –Au, has been demonstrated with variable Au phase morphologies from nanoparticle-in-matrix (PIM), nanoantenna-in-matrix, to VAN. The effective morphology tuning through deposition background pressure, and the corresponding highly tunable optical performance of three distinctive morphologies, were systematically explored and analyzed. A hyperbolic dispersion at high wavelength has been confirmed in the nano-antenna CeO 2 –Au thin film, proving this system as a promising candidate for HMM applications. More interestingly, a new and abnormal in-plane epitaxy of Au nanopillars following the large mismatched CeO 2 matrix instead of the well-matched SrTiO 3 substrate, was discovered. Additionally, the tilting angle of Au nanopillars, α , has been found to be a quantitative measure of the balance between kinetics and thermodynamics during the depositions of VANs. All these findings provide valuable information in the understanding of the VAN formation mechanisms and related morphology tuning. 

Interface‐type (IT) metal/oxide Schottky memristive devices have attracted considerable attention over filament‐type (FT) devices for neuromorphic computing because of their uniform, filament‐free, and analog resistive switching (RS) characteristics. The most recent IT devices are based on oxygen ions and vacancies movement to alter interfacial Schottky barrier parameters and thereby control RS properties. However, the reliability and stability of these devices have been significantly affected by the undesired diffusion of ionic species. Herein, a reliable interface‐dominated memristive device is demonstrated using a simple Au/Nb‐doped SrTiO₃(Nb:STO) Schottky structure. The Au/Nb:STO Schottky barrier modulation by charge trapping and detrapping is responsible for the analog resistive switching characteristics. Because of its interface‐controlled RS, the proposed device shows low device‐to‐device, cell‐to‐cell, and cycle‐to‐cycle variability while maintaining high repeatability and stability during endurance and retention tests. Furthermore, the Au/Nb:STO IT memristive device exhibits versatile synaptic functions with an excellent uniformity, programmability, and reliability. A simulated artificial neural network with Au/Nb:STO synapses achieves a high recognition accuracy of 94.72% for large digit recognition from MNIST database. These results suggest that IT resistive switching can be potentially used for artificial synapses to build next‐generation neuromorphic computing.