Approaching the Ideal Linearity in Epitaxial Crystalline-Type Memristor by Controlling Filament Growth.

Brain-inspired neuromorphic computing has attracted widespread attention owing to its ability to perform parallel and energy-efficient computation. However, the synaptic weight of amorphous/polycrystalline oxide based memristor usually exhibits large nonlinear behavior with high asymmetry, which aggravates the complexity of peripheral circuit system. Controllable growth of conductive filaments is highly demanded for achieving the highly linear conductance modulation. However, the stochastic behavior of the filament growth in commonly used amorphous/polycrystalline oxide memristor makes it very challenging. Here, the epitaxially grown Hf0.5Zr0.5O2-based memristor with the linearity and symmetry approaching ideal case is reported. A layer of Cu nanoparticles is inserted into epitaxially grown Hf0.5Zr0.5O2 film to form the grain boundaries due to the breaking of the epitaxial growth. By combining with the local electric field enhancement, the growth of filament is confined in the grain boundaries due to the fact that the diffusion of oxygen vacancy in crystalline lattice is more difficult than that in the grain boundaries. Furthermore, the decimal operation and high-accuracy neural network are demonstrated by utilizing the highly linear and multi-level conductance modulation capacity. This method opens an avenue to control the filament growth for the application of resistance random access memory (RRAM) and neuromorphic computing.

Effective electrical manipulation of a topological antiferromagnet by orbital torques.

The electrical control of the non-trivial topology in Weyl antiferromagnets is of great interest for the development of next-generation spintronic devices. Recent studies suggest that the spin Hall effect can switch the topological antiferromagnetic order. However, the switching efficiency remains relatively low. Here, we demonstrate the effective manipulation of antiferromagnetic order in the Weyl semimetal Mn3Sn using orbital torques originating from either metal Mn or oxide CuOx. Although Mn3Sn can convert orbital current to spin current on its own, we find that inserting a heavy metal layer, such as Pt, of appropriate thickness can effectively reduce the critical switching current density by one order of magnitude. In addition, we show that the memristor-like switching behaviour of Mn3Sn can mimic the potentiation and depression processes of a synapse with high linearity-which may be beneficial for constructing accurate artificial neural networks. Our work paves a way for manipulating the topological antiferromagnetic order and may inspire more high-performance antiferromagnetic functional devices.

Strain-Induced Uphill Hydrogen Distribution in Perovskite Oxide Films.

Incorporating hydrogen into transition-metal oxides (TMOs) provides a facile and powerful way to manipulate the performances of TMOs, and thus numerous efforts have been invested in developing hydrogenation methods and exploring the property modulation via hydrogen doping. However, the distribution of hydrogen ions, which is a key factor in determining the physicochemical properties on a microscopic scale, has not been clearly illustrated. Here, focusing on prototypical perovskite oxide (NdNiO3 and La0.67Sr0.33MnO3) epitaxial films, we find that hydrogen distribution exhibits an anomalous "uphill" feature (against the concentration gradient) under tensile strain, namely, the proton concentration enhances upon getting farther from the hydrogen source. Distinctly, under a compressive strain state, hydrogen shows a normal distribution without uphill features. The epitaxial strain significantly influences the chemical lattice coupling and the energy profile as a function of the hydrogen doping position, thus dominating the hydrogen distribution. Furthermore, the strain-(H+) distribution relationship is maintained in different hydrogenation methods (metal-alkali treatment) which is first applied to perovskite oxides. The discovery of strain-dependent hydrogen distribution in oxides provides insights into tailoring the magnetoelectric and energy-conversion functionalities of TMOs via strain engineering.

Highly Energy-Efficient Spin Current Generation in SrIrO3 by Manipulating the Octahedral Rotation.

Materials with strong spin-orbit coupling (SOC) have been continuously attracting intensive attention due to their promising application in energy-efficient, high-density, and nonvolatile spintronic devices. Particularly, transition-metal perovskite oxides with strong SOC have been demonstrated to exhibit efficient charge-spin interconversion. In this study, we systematically investigated the impact of epitaxial strain on the spin-orbit torque (SOT) efficiency in the SrIrO3(SIO)/Ni81Fe19(Py) bilayer. The results reveal that the SOT efficiency is strongly related to the octahedral rotation around the in-plane axes of the single-crystal SIO. By modulating the epitaxial strain using different substrates, the SOT efficiency can be remarkably improved from 0.15 to 1.45. This 10-fold enhancement of SOT efficiency suggests that modulating the epitaxial strain is an efficient approach to control the SOT efficiency in complex oxide-based heterostructures. Our work may have the potential to advance the application of complex oxides in energy-efficient spintronic devices.

Coexistence of Magnon-Induced and Rashba-Induced Unidirectional Magnetoresistance in Antiferromagnets.

Unidirectional magnetoresistance (UMR) has been intensively studied in ferromagnetic systems, which is mainly induced by spin-dependent and spin-flip electron scattering. Yet, UMR in antiferromagnetic (AFM) systems has not been fully understood to date. In this work, we reported UMR in a YFeO3/Pt heterostructure where YFeO3 is a typical AFM insulator. Magnetic-field dependence and temperature dependence of transport measurements indicate that magnon dynamics and interfacial Rashba splitting are two individual origins for AFM UMR, which is consistent with the UMR theory in ferromagnetic systems. We further established a comprehensive theoretical model that incorporates micromagnetic simulation, density functional theory calculation, and the tight-binding model, which explain the observed AFM UMR phenomenon well. Our work sheds light on the intrinsic transport property of the AFM system and may facilitate the development of AFM spintronic devices.

Realizing Metastable Cobaltite Perovskite via Proton-Induced Filling of Oxygen Vacancy Channels.

The interaction between transition-metal oxides (TMOs) and protons has become a key issue in magneto-ionics and proton-conducting fuel cells. Until now, most investigations on oxide-proton reactions rely on electrochemical tools, while the direct interplay between protons and oxides remains basically at simple dissolution of metal oxides by an acidic solution. In this work, we find classical TMO brownmillerite SrCoO2.5 (B-SCO) films with ordered oxygen vacancy channels experiencing an interesting transition to a metastable perovskite phase (M-SCO) in a weak acidic solution. M-SCO exhibits a strong ferromagnetism (1.01 µB/Co, Tc > 200 K) and a greatly elevated electrical conductivity (∼104 of pristine SrCoO2.5), which is similar to the prototypical perovskite SrCoO3. Besides, such M-SCO tends to transform back to B-SCO in a vacuum environment or heating at a relatively low temperature. Two possible mechanisms (H2O addition/active oxygen filling) have been proposed to explain the phenomenon, and the control experiments demonstrate that the latter mechanism is the dominant process. Our work finds a new way to realize cobaltite perovskite with enhanced magnetoelectric properties and may deepen the understanding of oxide-proton interaction in an aqueous solution.

Oxide Spintronics as a Knot of Physics and Chemistry: Recent Progress and Opportunities.

Transition-metal oxides (TMOs) constitute a key material family in spintronics because of mutually coupled degrees of freedom and tunable magneto-ionic properties. In this Perspective, we consider oxide spintronics as a knot of physics and chemistry and mainly discuss two current hot topics: spin-charge interconversion and magneto-ionics. First, spin-charge interconversion is focused on oxide films and heterostructures including 4d/5d heavy metal oxides (e.g., SrIrO3) and two-dimensional electron gases. Based on spin-charge interconversion, charge currents can be transformed to spin currents and generate spin-orbit torque in oxide/metal and all-oxide heterostructures. Additionally, the voltage control of magnetism in TMOs by the magneto-ionic pathway has rapidly accelerated during the past few years due to the versatile advantages of effective control, nonvolatile nature, low power cost, etc. Typical magneto-ionic oxide systems and corresponding physicochemical mechanisms will be discussed. Finally, further developments of oxide spintronics are envisioned, including material discovery, physics exploration, device design, and manipulation methods.

Facilitating room-temperature oxygen ion migration via Co-O bond activation in cobaltite films.

Oxygen ion migration in strongly correlated oxides can cause dramatic changes in the crystal structure, chemical and magnetoelectric properties, which holds promising for a wide variety of applications in catalysis, energy conversion, and electronics. However, the high strength and stability of metal-oxygen (M-O) bonds cause a large thermodynamic barrier for oxygen migration. Here, we designed Co-O bond activation in cobaltite (SrCoOx) films by Au-nanodot-decoration. Charge transfer from Au to SrCoOx effectively weakens the Co-O bond, meanwhile Co-O-Au synergistic bonding remarkably decreases the migration barrier of oxygen ions. Fast oxygen evolution occurs at the perimeter of the Au/SrCoOx interface, and the chemical potential gradient of O2- drives inner ion diffusion to the surface. Consequently, bias-free topotactic phase reduction from perovskite SrCoO3-δ to brownmillerite SrCoO2.5 has been achieved at room temperature. Our finding explores a new dimension to accelerate oxygen ion kinetics in transition-metal oxides from the aspect of interfacial bond activation, which is significant for developing oxide/noble-metal interfaces for high-efficiency ion migration and redox catalysis at low temperature.

Atomic insight into spin, charge and lattice modulations at SrFeO3-x/SrTiO3 interfaces.

Novel phenomena and functionalities at interfaces of oxide heterostructures are currently of great interest in a wide range of applications. At such interfaces, charge, spin, orbital and lattice ordering coexist and correlate closely, contributing to rich functional responses. By using atomically resolved imaging and spectroscopy techniques, we investigated magnetic behaviors and structural modulation at the SrFeO3-x/SrTiO3 interface. Fe/Ti element intermixing and oxygen vacancies occurred across a few unit cells at the interface. Furthermore, antiferromagnetic spin ordering of Fe with different valence states in the interface of SrFeO3-x/SrTiO3 induced uncompensated magnetic moments. Compared to the SrFeO3-x/La0.3Sr0.7Al0.65Ta0.35O3 heterojunction, the variations of charge and lattice order parameters at the SrFeO3-x/SrTiO3 interfaces were also determined by advanced electron microscopy, which provided a good understanding of the physical origin of disparate macroscopic magnetic properties, further investigated by magnetometer measurements and X-ray magnetic circular dichroism (XMCD) spectra. These studies provide comprehensive insight into the interfacial modulation of ferrite oxide, which may be useful for designing future devices in oxide electronics.

Lateral 2D WSe2 p-n Homojunction Formed by Efficient Charge-Carrier-Type Modulation for High-Performance Optoelectronics.

As unique building blocks for next-generation optoelectronics, high-quality 2D p-n junctions based on semiconducting transition metal dichalcogenides (TMDs) have attracted wide interest, which are urgent to be exploited. Herein, a novel and facile electron doping of WSe2 by cetyltrimethyl ammonium bromide (CTAB) is achieved for the first time to form a high-quality intramolecular p-n junction with superior optoelectronic properties. Efficient manipulation of charge carrier type and density in TMDs via electron transfer between Br- in CTAB and TMDs is proposed theoretically by density functional theory (DFT) calculations. Compared with the intrinsic WSe2 photodetector, the switching light ratio (Ilight /Idark ) of the p-n junction device can be enhanced by 103 , and the temporal response is also dramatically improved. The device possesses a responsivity of 30 A W-1 , with a specific detectivity of over 1011 Jones. In addition, the mechanism of charge transfer in CTAB-doped 2D WSe2 and WS2 are investigated by designing high-performance field effect transistors. Besides the scientific insight into the effective manipulation of 2D materials by chemical doping, this work presents a promising applicable approach toward next-generation photoelectronic devices with high efficiency.

Interfacial Control of Ferromagnetism in Ultrathin SrRuO3 Films Sandwiched between Ferroelectric BaTiO3 Layers.

Interfaces between materials provide an intellectually rich arena for fundamental scientific discovery and device design. However, the frustration of magnetization and conductivity of perovskite oxide films under reduced dimensionality is detrimental to their device performance, preventing their active low-dimensional application. Herein, by inserting the ultrathin 4d ferromagnetic SrRuO3 layer between ferroelectric BaTiO3 layers to form a sandwich heterostructure, we observe enhanced physical properties in ultrathin SrRuO3 films, including longitudinal conductivity, Curie temperature, and saturated magnetic moment. Especially, the saturated magnetization can be enhanced to ∼3.12 µB/Ru in ultrathin BaTiO3/SrRuO3/BaTiO3 trilayers, which is beyond the theoretical limit of bulk value (2 µB/Ru). This observation is attributed to the synergistic ferroelectric proximity effect (SFPE) at upper and lower BaTiO3/SrRuO3 heterointerfaces, as revealed by the high-resolution lattice structure analysis. This SFPE in dual-ferroelectric interface cooperatively induces ferroelectric-like lattice distortions in RuO6 oxygen octahedra and subsequent spin-state crossover in SrRuO3, which in turn accounts for the observed enhanced magnetization. Besides the fundamental significance of interface-induced spin-lattice coupling, our findings also provide a viable route to the electrical control of magnetic ordering, taking a step toward low-power applications in all-oxide spintronics.

Oxygen-Valve Formed in Cobaltite-Based Heterostructures by Ionic Liquid and Ferroelectric Dual-Gating.

Manipulation of oxygen vacancies via electric-field-controlled ionic liquid gating has been reported in many model systems within the emergent fields of oxide electronics and iontronics. It is then significant to investigate the oxygen vacancy formation/annihilation and migration across an additional ferroelectric layer with ionic liquid gating. Here, we report that via a combination of ionic liquid and ferroelectric gating, the remote control of oxygen vacancies and magnetic phase transition can be achieved in SrCoO2.5 films capped with an ultrathin ferroelectric BaTiO3 layer at room temperature. The ultrathin BaTiO3 layer acts as an atomic oxygen valve and is semitransparent to oxygen-ion transport due to the competing interaction between vertical electron tunneling and ferroelectric polarization plus surface electrochemical changes in itself, thus resulting in the striking emergence of new mixed-phase SrCoO x. The lateral coexistence of brownmillerite phase SrCoO2.5 and perovskite phase SrCoO3-δ was directly observed by transmission electron microscopy. Besides the fundamental significance of long-range interaction in ionic liquid gating, the ability to control the flow of oxygen ions across the heterointerface by the oxygen valve provides a new approach on the atomic scale for designing multistate memories, sensors, and solid-oxide fuel cells.

Electric Field Control of Phase Transition and Tunable Resistive Switching in SrFeO2.5.

SrFeO x (SFO x) compounds exhibit ionic conduction and oxygen-related phase transformation, having potential applications in solid oxide fuel cells, smart windows, and memristive devices. The phase transformation in SFO x typically requires a thermal annealing process under various pressure conditions, hindering their practical applications. Here, we have achieved a reversible phase transition from brownmillerite (BM) to perovskite (PV) in SrFeO2.5 (SFO2.5) films through ionic liquid (IL) gating. The real-time phase transformation is imaged using in situ high-resolution transmission electron microscopy. The magnetic transition in SFO2.5 is identified by fabricating an assisted La0.7Sr0.3MnO3 (LSMO) bottom layer. The IL-gating-converted PV phase of a SrFeO3-δ (SFO3-δ) layer shows a ferromagnetic-like behavior but applies a huge pinning effect on LSMO magnetic moments, which consequently leads to a prominent exchange bias phenomenon, suggesting an uncompensated helical magnetic structure of SFO3-δ. On the other hand, the suppression of both magnetic and exchange coupling signals for a BM-phased SFO2.5 layer elucidates its fully compensated G-type antiferromagnetic nature. We also demonstrated that the phase transition by IL gating is an effective pathway to tune the resistive switching parameters, such as set, reset, and high/low-resistance ratio in SFO2.5-based resistive random-access memory devices.

Photon-Gated Spin Transistor.

A new type of spin transistor with an optical gate is proposed with partial exposure of the device, where spin scattering is enhanced under light illumination due to the photon-induced minor spins. Consequently a reproducible transient gate operation of reisitance via optical methods is observed, as ascribed to the nature of spin excitation.