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Epitaxial growth of complex oxides on large-area wafers, such as sapphire and silicon, represents a key step toward scalable oxide device production. Solid phase epitaxy allows the synthesis of γ-Al2O3 on α-Al2O3 and provides a template with a matched lattice constant and appropriate cubic symmetry for subsequent heteroepitaxial growth of perovskite complex oxides. Nb-doped SrTiO3 thin films were deposited epitaxially on (111)-oriented γ-Al2O3 intermediate layers on (0001) c-axis-oriented sapphire α-Al2O3 crystals using pulsed laser deposition. The Nb:SrTiO3 thin films with a thickness of 53 nm, grown at 700 °C on γ-Al2O3, reached fully relaxed lattice parameters and were epitaxially oriented with respect to the substrate. Nb:SrTiO3 layers deposited using identical deposition conditions directly on α-Al2O3, without the γ-Al2O3 intermediate layer, were polycrystalline. The sheet conductivity of Nb:SrTiO3 grown on γ-Al2O3/α-Al2O3 is more than ten times higher than that of Nb:SrTiO3 grown directly on α-Al2O3 without the γ-Al2O3 layer. The results point to new directions for the integration of (111)-oriented pseudocubic perovskite complex oxides and the integration of epitaxial complex oxides over larger areas using α-Al2O3 single-crystal substrates. 

Recent advances in ferroic materials have identified topological defects as promising candidates for enabling additional functionalities in future electronic systems. The generation of stable and customizable polar topologies is needed to achieve multistates that enable beyond-binary device architectures. In this study, we show how to autonomously pattern on-demand highly tunable striped closure domains in pristine rhombohedral-phase BiFeO3 thin films through precise scanning of a biased atomic force microscopy tip along carefully designed paths. By employing this strategy, we generate and manipulate closed-loop structures with high spatial resolution in an automated manner, allowing the creation of highly tunable and intricate topological domain structures that exhibit distinct polarization configurations without the need for electrode deposition or complex heterostructure growth. As a proof-of-concept for ferroelectric beyond-binary memory devices, we use such topological domains as multistates, engineering an alphabet and automating the symbolic writing/reading process using autonomous microscopy. The resulting information density is compared with that of current commercially available memory devices, demonstrating the potential of ferroelectric topological domains for multistate information storage applications. 

Hierarchical assemblies of ferroelectric nanodomains, so-called super-domains, can exhibit exotic morphologies that lead to distinct behaviours. Controlling these super-domains reliably is critical for realizing states with desired functional properties. Here we reveal the super-switching mechanism by using a biased atomic force microscopy tip, that is, the switching of the in-plane super-domains, of a model ferroelectric Pb0.6Sr0.4TiO3. We demonstrate that the writing process is dominated by a super-domain nucleation and stabilization process. A complex scanning-probe trajectory enables on-demand formation of intricate centre-divergent, centre-convergent and flux-closure polar structures. Correlative piezoresponse force microscopy and optical spectroscopy confirm the topological nature and tunability of the emergent structures. The precise and versatile nanolithography in a ferroic material and the stability of the generated structures, also validated by phase-field modelling, suggests potential for reliable multi-state nanodevice architectures and, thereby, an alternative route for the creation of tunable topological structures for applications in neuromorphic circuits. 

Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu_1−xMn_1+ySiTe₃(0.04 ≤x≤ 0.26; 0.03 ≤y≤ 0.15), which crystallizes in a polar monoclinic structure (Pmspace group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides. 

Abstract Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second‐order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain‐tunable photonics. Though very different phenomena at distinct frequencies, both second‐order optical nonlinearity and piezoelectricity are third‐rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm⁻²was reported in Zn_1‐xMg_xO films. Here, ferroelectric Zn_1‐xMg_xO is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi‐phase‐matched optical harmonic generation as well as domain‐engineered piezoelectric devices. 

Abstract The presence of the top electrode on hafnium oxide‐based thin films during processing has been shown to drive an increase in the amount of metastable ferroelectric orthorhombic phase and polarization performance. This “Clamping Effect,” also referred to as the Capping or Confinement Effect, is attributed to the mechanical stress and confinement from the top electrode layer. However, other contributions to orthorhombic phase stabilization have been experimentally reported, which may also be affected by the presence of a top electrode. In this study, it is shown that the presence of the top electrode during thermal processing results in larger tensile biaxial stress magnitudes and concomitant increases in ferroelectric phase fraction and polarization response, whereas film chemistry, microstructure, and crystallization temperature are not affected. Through etching experiments and measurement of stress evolution for each processing step, it is shown that the top electrode locally inhibits out‐of‐plane expansion in the HZO during crystallization, which prevents equilibrium monoclinic phase formation and stabilizes the orthorhombic phase. This study provides a mechanistic understanding of the clamping effect and orthorhombic phase formation in ferroelectric hafnium oxide‐based thin films, which informs the future design of these materials to maximize ferroelectric phase purity and corresponding polarization behavior.