Julius de Rojas, Alberto Quintana, Aitor Lopeandía, Joaquín Salguero, José L. Costa-Krämer, Llibertat Abad, Maciej O. Liedke, Maik Butterling, Andreas Wagner, L… 展开作者
Julius de Rojas, Alberto Quintana, Aitor Lopeandía, Joaquín Salguero, José L. Costa-Krämer, Llibertat Abad, Maciej O. Liedke, Maik Butterling, Andreas Wagner, Lowie Henderick, Jolien Dendooven, Christophe Detavernier, Jordi Sort, Enric Menéndez
Voltage control of magnetism through electric field-induced oxygen motion (magneto-ionics) could represent a significant breakthrough in the pursuit for new strategies to enhance energy efficiency in a large variety of magnetic devices, such as magnetic micro-electro-mechanical systems (MEMS), magnetic logics, spin electronics, or neuromorphic computing, i.e., envisaging ultra-low power emulation of the biological synapse. Boosting the induced changes in magnetization, magneto-ionic motion and cyclability (endurance) continue to be key challenges to turn magneto-ionic phenomena into real applications. Here, we demonstrate that, without degrading cyclability, room temperature magneto-ionic motion in electrolyte-gated paramagnetic and fairly thick (> 100 nm) Co3O4 films largely depends on the configuration used to apply the electric field. In particular, magneto-ionic effects are significantly increased both in terms of generated magnetization (6 times larger: from 118.5 to 699.2 emu cm-3) and speed (35 times faster: from 33.1 to 1170.8 emu cm-3 h-1) if the electric field is applied across a conducting buffer layer (grown underneath the Co3O4 films), instead of directly contacting Co3O4. This is attributed to a greater uniformity and strength of the applied electric field when using the conducting layer. These results may trigger the use of oxygen magneto-ionics into promising new technologies, such as magnetic MEMS or brain-inspired computing, which require endurance and moderate speeds of operation.
So far, magneto-ionics, understood as voltage-driven ion transport in magnetic materials, has largely relied on controlled migration of oxygen ion/vacancy and, to a lesser extent, lithium and hydrogen. Here, we demonstrate efficient, room-temperature, voltage-driven nitrogen transport (i.e., nitrogen magneto-ionics) by electrolyte-gating of a single CoN film (without an ion-reservoir layer). Nitrogen magneto-ionics in CoN is compared to oxygen magneto-ionics in Co3O4, both layers showing a nanocrystalline face-centered-cubic structure and reversible voltage-driven ON-OFF ferromagnetism. In con…
Magneto-ionic control of magnetic properties through ionic migration has shown promise in enabling new functionalities in energy-efficient spintronic devices. In this work, we demonstrate the effect of helium ion irradiation and oxygen implantation on magneto-ionically induced exchange bias effect in Gd/Ni$_{0.33}$Co$_{0.67}$O heterostructures. Irradiation using $He^+$ leads to an expansion of the Ni$_{0.33}$Co$_{0.67}$O lattice due to strain relaxation. At low He+ fluence ($\leq$ 2$\times$10$^{14}$ ions cm$^{-2}$), the redox-induced interfacial magnetic moment initially increases, owing to en…
Magnetic tunnel junctions (MTJs) with Hf0.5Zr0.5O2 barriers are reported to show both tunneling magnetoresistance effect (TMR) and tunneling electroresistance effect (TER), displaying four resistance states by magnetic and electric field switching. Here we show that, under electric field cycling of large enough magnitude, the TER can reach values as large as 10^6%. Moreover, concomitant with this TER enhancement, the devices develop electrical control of spin polarization, with sign reversal of the TMR effect. Currently, this intermediate state exists for a limited number of cycles and underst…
Voltage control of interfacial magnetism has been greatly highlighted in spintronics research for many years, as it might enable ultra-low power technologies. Among few suggested approaches, magneto-ionic control of magnetism has demonstrated large modulation of magnetic anisotropy. Moreover, the recent demonstration of magneto-ionic devices using hydrogen ions presented relatively fast magnetization toggle switching, tsw ~ 100 ms, at room temperature. However, the operation speed may need to be significantly improved to be used for modern electronic devices. Here, we demonstrate that the spee…
Magneto-ionics has emerged as a promising approach to manipulate magnetic properties, not only by drastically reducing power consumption associated with electric current based devices but also by enabling novel functionalities. To date, magneto-ionics have been mostly explored in oxygen-based systems, while there is a surge of interests in alternative ionic systems. Here we demonstrate highly effective hydroxide-based magneto-ionics in electrodeposited $α$-Co(OH)$_{2}$ films. The $α$-Co(OH)$_{2}$, which is a room temperature paramagnet, is switched to ferromagnetic after electrolyte gating wit…
Electrically induced ionic motion offers a new way to realize voltage-controlled magnetism, opening the door to a new generation of logic, sensor, and data storage technologies. Here, we demonstrate an effective approach to magneto-ionically and electrically tune exchange bias in Gd/Ni$_{1-x}$Co$_{x}$O thin films (x=0.50, 0.67), where neither of the layers alone is ferromagnetic at room temperature. The Gd capping layer deposited onto antiferromagnetic Ni$_{1-x}$Co$_{x}$O initiates a solid-state redox reaction that reduces an interfacial region of the oxide to ferromagnetic NiCo. Exchange bias…
AgCrSe$_2$ is an example of a super-ionic conductor that has recently attracted attention for its low thermal conductivity. Here we investigate the optical properties of AgCrSe$_2$ in the ordered phase between 14 K and 374 K using reflectivity experiments. The far infrared optical response is dominated by three phonon modes, while six interband transitions are observed in the visible range. From our analysis we find that the phonon parameters display an interesting temperature dependence around the Néel temperature, pointing to a small magneto-elastic coupling. In addition, the lifetimes of th…
In metal/oxide heterostructures, rich chemical, electronic, magnetic and mechanical properties can emerge from interfacial chemistry and structure. The possibility to dynamically control interface characteristics with an electric field paves the way towards voltage control of these properties in solid-state devices. Here we show that electrical switching of the interfacial oxidation state allows for voltage control of magnetic properties to an extent never before achieved through conventional magnetoelectric coupling mechanisms. We directly observe, for the first time, in situ voltage driven O…
In Ta/CoFeB/HfO2 stacks a gate voltage drives, in a nonvolatile way, the system from an underoxidized state exhibiting in-plane anisotropy (IPA) to an optimum oxidation level resulting in perpendicular anisotropy (PMA) and further into an overoxidized state with IPA. The IPA$\,\to\,$PMA regime is found to be significantly faster than the PMA$\,\to\,$IPA regime, while only the latter shows full reversibility under the same gate voltages. The effective damping parameter also shows a marked dependence with gate voltage in the IPA$\,\to\,$PMA regime, going from 0.029 to 0.012, and only a modest in…
Electric-field control of magnetism provides a promising route towards ultralow power information storage and sensor technologies. The effects of magneto-ionic motion have so far been prominently featured in the direct modification of interface chemical and physical characteristics. Here we demonstrate magnetoelectric coupling moderated by voltage-driven oxygen migration beyond the interface limit in relatively thick AlOx/GdOx/Co (15 nm) films. Oxygen migration and its ramifications on the Co magnetization are quantitatively mapped with polarized neutron reflectometry under thermal and electro…
The manipulation of magnetism with a gate voltage is expected to lead the way towards the realization of energy-efficient spintronics devices and high-performance magnetic memories. Exploiting magneto-ionic effects under micro-patterned electrodes in solid-state devices adds the possibility to modify magnetic properties locally, in a non-volatile and reversible way. Tuning magnetic anisotropy, magnetization and Dzyaloshinskii-Moriya interaction allows modifying at will the dynamics of non trivial magnetic textures such as skyrmions and chiral domain walls in magnetic race tracks. In this work,…
The recent realization of epitaxial SrCoO$_3$ thin films has triggered a renewed interest in their electronic, magnetic, and ionic properties. Here we uncover several unusual magneto-transport properties of this compound, suggesting that it hosts persistent spin fluctuation down to low temperatures. We achieve the metallic SrCoO$_3$ with record-low resistivity from insulating SrCoO$_{2.5}$ by the ionic liquid gating. We find a linear relationship between the anomalous Hall resistivity and the longitudinal resistivity, which cannot be accounted for by the conventional mechanisms. We theoretical…
Spin-resolved electron symmetry filtering is a key mechanism behind giant tunneling magnetoresistance (TMR) in Fe/MgO/Fe and similar magnetic tunnel junctions (MTJs), providing room temperature functionality in modern spin electronics. However, the core process of the electron symmetry filtering breaks down under applied bias, dramatically reducing the TMR above 0.5 V. This strongly hampers the application range of MTJs. To circumvent the problem, resonant tunneling between ferromagnetic electrodes through quantum well states in thin layers has been used so far. This mechanism, however, is mai…
Depth Profiling of Oxygen Migration in Ta/HfO2 Stacks During Ionic Liquid Gating
Institute of Physics, Johannes Gutenberg University Mainz（美因茨约翰内斯·古腾堡大学物理研究所）；Faculty of Physics, Bielefeld University（比勒费尔德大学物理学院）；Faculty of Physics, Osnabrück University（奥斯纳布吕克大学物理学院）
Topological insulators have been predicted to exhibit a variety of interesting phenomena including a quantized magnetoelectric response and novel spintronics effects due to spin textures on their surfaces. However, experimental observation of these phenomena has proved difficult due to the finite bulk carrier density which may overwhelm the intrinsic topological responses that are expressed at the surface. Here, we demonstrate a novel ionic gel gating technique to tune the chemical potential of Bi$_{2}$Se$_{3}$ thin films while simultaneously performing THz spectroscopy. We can tune the carrie…
Here we demonstrate that MnTe epitaxial films with zinc-blend structure and MnTe/ZnTe multilayers should show ferroelectric polarization in antiferromagnetically (AFM) ordered state and thus belong to multiferroics. Spontaneous ferroelectric polarization results from the bending of highly ionic Mn-Te-Mn bonds induced by magnetostrictive shear strain. Orientation of ferroelectric polarization is coupled with orientation of AFM vector and thus can be controlled by application of the external magnetic field. Due to the clamping of electric and magnetic order parameters, domain structure in MnTe i…
The valley-contrasting orbital magnetic moment of Bloch electrons allows the lifting of valley degeneracy by an out-of-plane magnetic field. We demonstrate that this leads to negative magnetoresistance, utilizing a gapped two-dimensional multi-valley model as an example. An intuitive physical picture in terms of the increased carrier density from a magnetic gating effect is proposed for this negative magnetoresistance. In particular, giant negative magnetoresistance is achieved after one of the two valleys is depleted by the magnetic field. This new mechanism of negative magnetoresistance is a…
The magnetoresistance is the magnetic field induced change of electrical resistivity of a material. Recent studies have revealed extremely large magnetoresistance in several non-magnetic semimetals, which has been explained on the basis of either electron-hole compensation or the Fermi surface topology, or the combination of both. Here, we present a single crystal study on MoSi$_2$, which exhibits extremely large magnetoresistance, approaching almost 10$^7$ % at 2 K and 14 T magnetic field. It is found that the electron-hole compensation level in MoSi$_2$ evolves with magnetic field, which is …
Magneto-electric multiferroics exemplified by TbMnO3 possess both magnetic and ferroelectric long-range order. The magnetic order is mostly understood, whereas the nature of the ferroelectricity has remained more elusive. Competing models proposed to explain the ferroelectricity are associated respectively with charge transfer and ionic displacements. Exploiting the magneto-electric coupling, we use an electric field to produce a single magnetic domain state, and a magnetic field to induce ionic displacements. Under these conditions, interference charge-magnetic X-ray scattering arises, encodi…
In recent years, the field of antiferromagnetic spintronics has been substantially advanced. Electric-field control is a promising approach to achieving ultra-low power spintronic devices via suppressing Joule heating. In this article, cutting-edge research, including electric-field modulation of antiferromagnetic spintronic devices using strain, ionic liquids, dielectric materials, and electrochemical ionic migration, are comprehensively reviewed. Various emergent topics such as the Neel spin-orbit torque, chiral spintronics, topological antiferromagnetic spintronics, anisotropic magnetoresis…
Neutron-Induced Enhancement of Ion Transport Through Lithium-Ion Battery Materials
Materials Sciences and Engineering Institute, University of Missouri（密苏里大学材料科学与工程研究所）；University of Missouri Research Reactor (MURR), University of Missouri（密苏里大学研究反应堆（MURR））；Department of Physics and Astronomy, University of Missouri（密苏里大学物理与天文学系）；Electron Microscopy Core, University of Missouri（密苏里大学电子显微镜核心设施）；Advanced Materials Characterization Core Facility, Missouri University of Science and Technology（密苏里科技大学先进材料表征核心设施）
We investigate the ultra-sharp jump in the isothermal magnetization and the resistivity in the polycrystalline $Sm_{0.5}(Ca_{0.5-y}Sr_{y})MnO_3$ $(y = 0, 0.1, 0.2, 0.25, 0.3, 0.5)$ compounds. The critical field $(H_{cr})$, required for the ultra-sharp jump, decreases with increase of `Sr' concentration, i.e. with increase of average A-site ionic radius $\langle r_A\rangle$. The magnetotransport data indicate that the phase separation increases with the increase of $\langle r_A\rangle$, i.e. with $y$. The dependency of $H_{cr}$ with magnetic field sweep rate reveals that the ultra-sharp jump fr…
We report on large modifications of current-induced spin-orbit torques in a gated Pt/Co/Gd-oxide microstrip due to voltage-driven O$^{2-}$ migration. The Slonczewski-like and field-like torques are quantified using a low-frequency harmonic technique based on the polar magneto-optical Kerr effect. Voltage-induced oxidation of Co enhances the Slonczewski-like torque by as much as an order of magnitude, and simultaneously reduces the anisotropy energy barrier by a factor of ~5. Such magneto-ionic tuning of interfacial spin-orbit effects may significantly enhance the efficiency of magnetization sw…
Collective behavior widely exists in nature, ranging from the macroscopic cloud of swallows to the microscopic cloud of colloidal particles. The behavior of an individual inside the collective is distinctive from its behavior alone, as it follows its neighbors. The introduction of such collective behavior in two-dimensional (2D) materials may offer new possibilities to achieve desired but unattained properties. Here, we report a highly sensitive magneto-optic effect and transmissive magneto-coloration via introducing collective behavior into magnetic 2D material dispersions. The increase of io…
Magneto-Structural Coupling Enables Cryogenic Cation Redistribution in a Spinel Oxide
Hainan University（海南大学）；Arizona State University（亚利桑那州立大学）；Institute of High Energy Physics, Chinese Academy of Sciences（中国科学院高能物理研究所）；Spallation Neutron Source Science Center（散裂中子源科学中心）；University of Science and Technology Beijing（北京科技大学）；Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所北京凝聚态物理国家实验室）
The magnetoelectric effect in the system $RAl_3(BO_3)_4$ ($R$ = Tb, Ho, Er, Tm) is investigated between 3 K and room temperature and at magnetic fields up to 70 kOe. We show a systematic increase of the magnetoelectric effect with decreasing magnetic anisotropy of the rare earth moment. A giant magnetoelectric polarization is found in the magnetically (nearly) isotropic $HoAl_3(BO_3)_4$. The polarization value in transverse field geometry at 70 kOe reaches 3600 $μC/m^2$ which is significantly higher than reported values for the field-induced polarization of linear magnetoelectric or even multi…
Co10Ge3O16 crystallizes in an intergrowth structure featuring alternating layers of spinel and rock salt. Variable-temperature powder synchrotron X-ray and neutron diffraction, magnetometry, and heat capacity experiments reveal a magnetostructural transition at T_N = 203 K. This rhombohedral-to-monoclinic transition involves a slight elongation of the CoO6 octahedra along the apical axis. Below T_N, the application of a large magnetic field causes a reorientation of the Co^2+ Ising spins. This metamagnetic transition is first-order as evidenced by a latent heat observed in temperature-dependen…
We have studied the [100]-[110] anisotropy of the Compton profile in the bilayer manganite. Quantitative agreement is found between theory and experiment with respect to the anisotropy in the two metallic phases (i.e. the low temperature ferromagnetic and the colossal magnetoresistant phase under a magnetic field of 7 T). Robust signatures of the metal-insulator transition are identified in the momentum density for the paramagnetic phase above the Curie temperature. We interpret our results as providing direct evidence for the transition from the metallic-like to the admixed ionic-covalent bon…
Material research has been a major driving force in the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices; identifying new magnetic materials is key to better device performance and new device paradigm. The advent of two-dimensional van der Waals crystals creates new possibilities. This family of materials retain their chemical stability and structural integrity down to monolayers and, being atomically thin, are readily tuned by various kinds of gate modulation. Recent experiments have demonstr…
Ab initio calculations of the electric polarization of correlation-driven insulating materials, namely Mott insulators, have not been possible so far. Using a combination of density functional theory and dynamical-mean-field theory we study the electric polarization of the Mott insulator Sr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. We predict a ferroelectric polarization of $\simeq 16.5 μC/cm^2$ in the high temperature paramagnetic phase and recover the measured value of $\simeq 13.3 μC/cm^2$ in the low temperature antiferromagnetic phase. Our calculations reveal that the driving force for the ferroelectric…
Multiferroic BiFeO3 ceramics have been doped with Ca. The smaller ionic size of Ca compared with Bi means that doping acts as a proxy for hydrostatic pressure, at a rate of 1%Ca=0.3GPa. It is also found that the magnetic Neel temperature (TNeel) increases as Ca concentration increases, at a rate of 0.66K per 1%Ca (molar). Based on the effect of chemical pressure on TNeel, we argue that applying hydrostatic pressure to pure BiFeO3 can be expected to increase its magnetic transition temperature at a rate around ~2.2K/GPa. The results also suggest that pressure (chemical or hydrostatic) could be …
Electrical control of magnetism in a two-dimensional (2D) semiconductor is of great interest for emerging nanoscale low-dissipation spintronic devices. Here, we propose a general approach of tuning magnetic coupling and anisotropy of a van der Waals (vdW) 2D magnetic semiconductor via a built-in electric field generated by the adsorption of superatomic ions. Using first-principles calculations, we predict a significant enhancement of ferromagnetic (FM) coupling and a great change of magnetic anisotropy in 2D semiconductors when they are sandwiched between superatomic cations and anions. The ma…
Within the ionic Hubbard model, electron correlations transmute the single-particle gap of a band insulator into a Mott gap in the strong correlation limit. However understanding the nature of possible phases in between these two extreme insulating phases remains an outstanding challenge. We find two strongly correlated insulating phases in between the above extremes: (i) The insulating phase just before the Mott phase can be viewed as gapping a non-Fermi liquid state of spinons through staggered ionic potential. The quasi-particles of underlying spinons are orthogonal to physical electrons an…
Dynamical multiferroicity features entangled dynamic orders: fluctuating electric dipoles induce magnetization. Hence, the material with paraelectric fluctuations can develop magnetic signatures if dynamically driven. We identify the paraelectric KTaO$_3$ (KTO) as a prime candidate for the observation of the dynamical multiferroicity. We show that when a KTO sample is exposed to a circularly polarized laser pulse, the dynamically induced ionic magnetic moments are of the order of 5\% of the nuclear magneton per unit cell. We determine the phonon spectrum using ab initio methods and identify T$…
Perpendicular exchange bias (EB), which combines the perpendicular magnetic anisotropy and the ferromagnetic (FM) - antiferromagnetic (AFM) exchange coupling, is extremely important in the high-density AFM spintronics. However, the effective modulation of EB remains challenging, since the alternant spins at the AFM/FM interface are strongly pinned by the AFM layer. Voltage tuning of EB through the magnetoelectric coupling provides a potential way to achieve a rapid magnetization switching in an energy-efficient manner. Nevertheless, the interfacial strain mediation of perpendicular EB induced …
We study the magnetic properties of single crystals of rutile TiO2 implanted with cobalt for various fluences. The temperature variation of zero field cooled(ZFC) and field cooled (FC) magnetization shows a much higher blocking temperature (TB) along [1-10]. Similarly the scaling of magnetization isotherms above TB is seen only when the field is parallel to [1-10] direction. With field along this direction, the magnetization shows near saturation at a much smaller field compared to that of[001] direction. The Co nanoclusters possess an "easy" and "hard axis" of magnetization coupled by the mag…
Oxygen vacancies play a crucial role in the control of the electronic, magnetic, ionic, and transport properties of functional oxide perovskites. Rare earth nickelates (RENiO$_{3-x}$) have emerged over the years as a rich platform to study the interplay between the lattice, the electronic structure, and ordered magnetism. In this study, we investigate the evolution of the electronic and magnetic structure in thin films of RENiO$_{3-x}$, using a combination of X-ray absorption spectroscopy and imaging, resonant X-ray scattering, and extended multiplet ligand field theory modeling. We find that …
